The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR inv...The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of catalysts.However,there is a contradiction in wettability requirements for the two half-reactions.Specifically,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)reactants.Conversely,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic catalyst.This was achieved through a selectively hydrophobic modification method and a charge-transfer-control strategy.Consequently,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark catalyst.This innovative approach holds great potential for application in universal overall reactions involving gas participation.展开更多
Precisely reducing the size of metal-organic frameworks(MOFs)derivatives is an effective strategy to manipulate their phase engineering owing to size-dependent oxidation;however,the underlying relationship between the...Precisely reducing the size of metal-organic frameworks(MOFs)derivatives is an effective strategy to manipulate their phase engineering owing to size-dependent oxidation;however,the underlying relationship between the size of derivatives and phase engineering has not been clarified so far.Herein,a spatial confined growth strategy is proposed to encapsulate small-size MOFs derivatives into hollow carbon nanocages.It realizes that the hollow cavity shows a significant spatial confinement effect on the size of confined MOFs crystals and subsequently affects the dielectric polarization due to the phase hybridization with tunable coherent interfaces and heterojunctions owing to size-dependent oxidation motion,yielding to satisfied microwave attenuation with an optimal reflection loss of-50.6 d B and effective bandwidth of 6.6 GHz.Meanwhile,the effect of phase hybridization on dielectric polarization is deeply visualized,and the simulated calculation and electron holograms demonstrate that dielectric polarization is shown to be dominant dissipation mechanism in determining microwave absorption.This spatial confined growth strategy provides a versatile methodology for manipulating the size of MOFs derivatives and the understanding of size-dependent oxidation-induced phase hybridization offers a precise inspiration in optimizing dielectric polarization and microwave attenuation in theory.展开更多
We calibrate the macroscopic vortex high-order harmonic generation(HHG)obtained by the quantitative rescattering(QRS)model to compute single-atom induced dipoles against that by solving the time-dependent Schr?dinger ...We calibrate the macroscopic vortex high-order harmonic generation(HHG)obtained by the quantitative rescattering(QRS)model to compute single-atom induced dipoles against that by solving the time-dependent Schr?dinger equation(TDSE).We show that the QRS perfectly agrees with the TDSE under the favorable phase-matching condition,and the QRS can accurately predict the main features in the spatial profiles of vortex HHG if the phase-matching condition is not good.We uncover that harmonic emissions from short and long trajectories are adjusted by the phase-matching condition through the time-frequency analysis and the QRS can simulate the vortex HHG accurately only when the interference between two trajectories is absent.This work confirms that it is an efficient way to employ the QRS model in the single-atom response for precisely simulating the macroscopic vortex HHG.展开更多
Synthesis of multi-color laser pulses has been developed as a promising way to improve low conversion efficiency of high-order harmonic generation(HHG). Here we systematically study the effect of laser focus in a two-...Synthesis of multi-color laser pulses has been developed as a promising way to improve low conversion efficiency of high-order harmonic generation(HHG). Here we systematically study the effect of laser focus in a two-color waveform on generation of macroscopic HHG in soft x-rays. We find that the dependence of HHG yields on laser focus at low or high gas pressure is sensitive to the characteristics of single-atom harmonic response, in which “short”-or “long”-trajectory emissions can be selectively controlled by changing the waveform of two-color synthesized laser pulse. We uncover the phase-matching mechanism of HHG in the gas medium by examining the propagation of the two-color waveform and the evolution of time-frequency emissions of high-harmonic field. We further reveal that the nonlinear effects, such as geometric phase, atomic dispersion, and plasma defocusing, are responsible for modification of two-color waveform upon propagation. This work can be used to find better macroscopic conditions for generating soft x-ray HHG by employing two-color optimized waveforms.展开更多
The development of high-efficiency and cost-effective bifunctional electrocatalysts for overall water splitting remains a formidable challenge.Herein,FeNi-Nd_(2)O_(3) nanoparticles anchored on N-doped carbon nanotubes...The development of high-efficiency and cost-effective bifunctional electrocatalysts for overall water splitting remains a formidable challenge.Herein,FeNi-Nd_(2)O_(3) nanoparticles anchored on N-doped carbon nanotubes(FeNi-Nd_(2)O_(3)/NCN) are designed for highly effective overall water splitting via a facile two-step hydrothermal approach.The synthetic FeNi-Nd_(2)O_(3) hetero-trimers(Fe 2p-Ni 2p-Nd 3d orbital coupling)on NCN achieve excellent oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) activities with overpotentials of 270 and 120 mV at 10 mA cm^(-2) in 1 M KOH solution.Moreover,a small voltage of 1.52 V at 10 mA cm^(-2) is achieved when FeNi-Nd_(2)O_(3)/NCN is assessed as bifunctional catalyst for overall water splitting,which is superior to the typically integrated Pt/C and RuO_(2) counterparts(1.54 V at 10 mA cm^(-2)).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy show that the remarkably improved activity is originated from Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction.Furthermore,density functional theory(DFT) calculations indicate that the lattice contraction reduces binding energies of intermediates by downshifting the position of FeNi bimetallic d-band center relative to the Fermi level to optimize catalytic performance.Therefore,the Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction may provide a new perspective for designing and synthesizing innovative catalytic systems.展开更多
The contradiction between classical and quantum physics can be identified through quantum contextuality, which does not need composite systems or spacelike separation. Contextuality is proven either by a logical contr...The contradiction between classical and quantum physics can be identified through quantum contextuality, which does not need composite systems or spacelike separation. Contextuality is proven either by a logical contradiction between the noncontextuality hidden variable predictions and those of quantum mechanics or by the violation of noncontextual inequality. We propose an experimental scheme of state-independent contextual inequality derived from the Mermin proof of the Kochen–Specker(KS) theorem in eight-dimensional Hilbert space, which could be observed either in an individual system or in a composite system. We also show how to resolve the compatibility problems. Our scheme can be implemented in optical systems with current experiment techniques.展开更多
Recently, the synthesis of new elements above Z = 118 has been a hot topic in nuclear physics. Meanwhile, the α-decay chain is expected to be the unique tool to identify these heaviest nuclei. We have systematically ...Recently, the synthesis of new elements above Z = 118 has been a hot topic in nuclear physics. Meanwhile, the α-decay chain is expected to be the unique tool to identify these heaviest nuclei. We have systematically calculated the α-decay energies and half-lives on the same footing for superheavy nuclei (SHN) within the cluster model along with a slightly modified Woods-Saxon (W.S.) potential as the nuclear potential. Based on the available experimental data, the key radius parameter (R) in the α-core potential is determined via the systematic trend from the α-decay and isotopic chains. The α-decay energy (Qα) values and half-lives are then obtained simultaneously for those unknown SHN in the range of 117 ≤ Z ≤ 120, during which the decay width is obtained using a new treatment for the asymptotic behavior of the α-core wave function. The theoretical values and experimental data are found to be in excellent agreement for the nuclei ^(293,294)117 and ^(294)118 regardless of the method used to determine the R parameter. Predicting the α-decay chains for new elements Z = 119 and Z = 120 can be useful in ongoing or forthcoming experiments.展开更多
X-ray photoelectron spectroscopy(XPS)is an important characterization tool in the pursuit of controllable fluorination of two-dimensional hexagonal boron nitride(h-BN).However,there is a lack of clear spectral interpr...X-ray photoelectron spectroscopy(XPS)is an important characterization tool in the pursuit of controllable fluorination of two-dimensional hexagonal boron nitride(h-BN).However,there is a lack of clear spectral interpretation,and seemingly conflicting measurements exist.To discern the structure−spectroscopy relation,we performed a comprehensive first-principles study on the boron 1s edge XPS of fluorinated h-BN(F-BN)nanosheets.By gradually introducing 1−6 fluorine atoms into different boron or nitrogen sites,we created various F-BN structures with doping ratios ranging from 1 to 6%.Our calculations reveal that fluorines landed at boron or nitrogen sites exert competitive effects on the B 1s binding energies(BEs),leading to red or blue shifts in different measurements.Our calculations affirmed the hypothesis that fluorination affects 1s BEs of all borons in theπ-conjugated system,opposing the transferability from h-BN to F-BN.Additionally,we observe that BE generally increases with higher fluorine concentration when both borons and nitrogens are nonexclusively fluorinated.These findings provide critical insights into how fluorination affects boron’s 1s BEs,contributing to a better understanding of fluorination functionalization processes in h-BN and its potential applications in materials science.展开更多
Black phosphorus(BP)has been regarded as a promising two-dimensional semiconductor due to its excellent properties including high carrier mobility and widely tunable direct bandgap.Despite extensive interest as well a...Black phosphorus(BP)has been regarded as a promising two-dimensional semiconductor due to its excellent properties including high carrier mobility and widely tunable direct bandgap.Despite extensive interest as well as research progress,the preparation of large-size and high-quality BP single crystal in high throughput still remains challenging.Here,a facile growth of centimeter-sized BP single crystal flakes with dozens of throughput per batch is achieved by using bidirectional vapor transport(BVT)method.High crystal quality is confirmed by structural and spectrum characterizations,with an X-ray diffraction rocking curve peak half-height width of only 0.02°.The as-grown BP single crystal flake with smooth cleavage plane can be easily exfoliated into large scale nanosheets.Field-effect transistors fabricated based on the BP by such approach show excellent performance including reliable carrier mobility up to 1150 cm^(2) V^(−1) s^(−1) and on/off current ratio of~10^(6)at 15 K.This approach is also applicable to various doped-BP,such as As-BP,Se-BP,Te-BP,etc.The ability to grow centimeter-sized BP single crystal flakes in high yield will accelerate the research and applications of BP-based electronics and optoelectronics.展开更多
Ohmic contacts are fundamental components in semiconductor technology,facilitating efficient electrical connection and excellent device performance.We employ first-principles calculations to show that semimetallic gra...Ohmic contacts are fundamental components in semiconductor technology,facilitating efficient electrical connection and excellent device performance.We employ first-principles calculations to show that semimetallic graphene is a natural Ohmic contact partner of monolayer semiconducting black arsenic(BAs),for which the top of the valence band is below the Fermi energy of the order of 10~2 meV.The Ohmic contact arises from the giant Stark effect induced by van der Waals electron transfer from BAs to graphene,which does not destroy their respective band features.Remarkably,we show that this intrinsic Ohmic contact remains robust across a wide range of interlayer distances(adjustable by strain)or vertical electric fields,whereas the weak spin splitting of the order of 1 meV induced by symmetry breaking plays little part in Ohmic contact.These findings reveal the potential applications of graphene–BAs in ultralow dissipation transistors.展开更多
As a fundamental thermodynamic variable, pressure can alter the bonding patterns and drive phase transitions leading to the creation of new high-pressure phases with exotic properties that are inaccessible at ambient ...As a fundamental thermodynamic variable, pressure can alter the bonding patterns and drive phase transitions leading to the creation of new high-pressure phases with exotic properties that are inaccessible at ambient pressure. Using the swarm intelligence structural prediction method, the phase transition of TiF_(3), from R-3c to the Pnma phase, was predicted at high pressure, accompanied by the destruction of TiF_6 octahedra and formation of TiF_8 square antiprismatic units. The Pnma phase of TiF_(3), formed using the laser-heated diamond-anvil-cell technique was confirmed via high-pressure x-ray diffraction experiments. Furthermore, the in situ electrical measurements indicate that the newly found Pnma phase has a semiconducting character, which is also consistent with the electronic band structure calculations. Finally, it was shown that this pressure-induced phase transition is a general phenomenon in ScF_(3), VF_(3), CrF_(3), and MnF_(3), offering valuable insights into the high-pressure phases of transition metal trifluorides.展开更多
Quantum error correction is essential for achieving reliable quantum information processing tasks,as it can mitigate the detrimental effects of noise by encoding single-qubit information into a larger quantum system.H...Quantum error correction is essential for achieving reliable quantum information processing tasks,as it can mitigate the detrimental effects of noise by encoding single-qubit information into a larger quantum system.However,the generation of distributed entanglement between logical qubits located within two spatially separated nodes presents a significant resource-intensive challenge that has yet to be overcome.Here we present a heralded protocol for generating distributed entanglement between two nonlocal error-protected logical qubits.A high-dimensional single photon can evolve physical qubits into a logical qubit that entangles with the photon and then converts logical qubit-photon entanglement into entanglement between two logical qubits,when the photon state is properly tuned and an effective photon-spin interface between single photons and individual spins is exploited.Furthermore,the success of the entanglement generation is heralded by the detection of the photon,and the corresponding efficiency can,in principle,approach unity.These distinguished features make our protocol highly appealing for future large-scale quantum technologies.展开更多
This review describes recent advances in wettability adjustment to improve the main green energy conversion and storage systems,i.e.,photocatalysis and electrocatalysis.Because both are redox reactions involving elect...This review describes recent advances in wettability adjustment to improve the main green energy conversion and storage systems,i.e.,photocatalysis and electrocatalysis.Because both are redox reactions involving electron behavior,they follow a similar pattern in the surface reaction step,which is related to wettability adjustment.Thus,we consider photocatalysis and electrocatalysis together in terms of mass transfer adjustment based on commonalities,aiming to understand the fundamentals more deeply and bring greater mutual inspiration to photocatalysis and electrocatalysis.The theoretical basis is first laid out,and then various strategies are introduced.Subsequently,according to the different requirements of mass transfer,we classify the photocatalytic and electrocatalytic reactions into gas consumption reactions preferring hydrophobic surfaces,and gas evolution reactions preferring hydrophilic surfaces.Pollutant degradation reactions involving different water-soluble substrates are also mentioned.Further,we introduce the specific optimization effect of wettability regulation on the reaction,and the mechanism behind the effect.This comprehensive and insightful review will provide a strategic guide to the reasonable design and development of wettability-optimized photocatalytic and electrocatalytic systems.展开更多
Attosecond transient absorption(ATA)has been developed as an all-optical technique for probing electron dynamics in matter.Here we present a scheme that can modify the laserinduced state and the corresponding ATA spec...Attosecond transient absorption(ATA)has been developed as an all-optical technique for probing electron dynamics in matter.Here we present a scheme that can modify the laserinduced state and the corresponding ATA spectrum via excitation by a pair of XUV attosecond pulses and by a time-delayed mid-infrared(MIR)laser probe.Different from the scheme of the electronic excitation by a single XUV attosecond pulse,the application of a pair of XUV pulses provides extra degrees of freedom,such as the time delay and the intensity ratio between two XUV pulses,which make it possible to adjust the pump process,resulting in the modification of the ATA spectrum.We show that by varying the time delay between the two XUV pulses,the population of the dark state and the ATA spectrum of the laser-induced state have periodic modulations.We also demonstrate that the peak of the ATA spectrum of the laser-induced state appears at a fixed time delay between the XUV pair and the MIR laser when the intensity ratio is large,and it changes with the time delay when the intensity ratio is small,which can be related to either one of two peaks in the population of the dark state.展开更多
In addition to the Coulomb displacement energy,the residual differences between the binding energies of mirror nuclei(a pair of nuclei with the same mass number plus interchanged proton and neutron numbers)contribute ...In addition to the Coulomb displacement energy,the residual differences between the binding energies of mirror nuclei(a pair of nuclei with the same mass number plus interchanged proton and neutron numbers)contribute to the shell effect via the valence scheme in this study.To this end,one linear combining type of valence nucleon number,namely,αNp+βNn,is chosen to tackle this shell correction,in which Npand Nnare the valence proton and neutron numbers with respect to the nearest shell closure,respectively.The mass differences of mirror nuclei,as the sum of the empirical Coulomb displacement energy and shell effect correction,are then used to obtain the binding energies of proton-rich nuclei through the available data of their mirror partners to explore the proton dripline of the nuclear chart.展开更多
The propagating of laser-generated ultrasonic waves in K9 glass was investigated. Many methods have been developed to detect the laser ultrasound since laser ultrasonic waves can be used to measure material parameters...The propagating of laser-generated ultrasonic waves in K9 glass was investigated. Many methods have been developed to detect the laser ultrasound since laser ultrasonic waves can be used to measure material parameters or characterize materials properties. In order to reduce the measuring time, a Mach–Zehnder interferometer, a full field measuring tool,was preferred in this paper. The ultrasonic wave was produced on the K9 glass surface by a Q-switched Nd:YAG laser absorbed in a liquid layer. The interferograms were then taken at various delay times by a CCD camera after single pulse induced laser ultrasonic waves. Ultrasonic waves in the K9 glass can be observed from interferogram images. The results provide an understanding of laser ultrasound propagation in K9 glass in the lifetime.展开更多
The efficiency of photocatalytic CO_(2) reduction reaction(PCRR)is restricted by the low solubility and mobility of CO_(2) in water,poor CO_(2) adsorption capacity of catalyst,and competition with hydrogen evolution r...The efficiency of photocatalytic CO_(2) reduction reaction(PCRR)is restricted by the low solubility and mobility of CO_(2) in water,poor CO_(2) adsorption capacity of catalyst,and competition with hydrogen evolution reaction(HER).Recently,hydrophobic modification of the catalyst surface has been proposed as a potential solution to induce the formation of triple-phase contact points(TPCPs)of CO_(2)(gas phase),H_(2) O(liquid phase),and catalysts(solid phase)near the surface of the catalyst,enabling direct delivery of highly concentrated CO_(2) molecules to the active reaction sites,resulting in higher CO_(2) and lower H+surface concentrations.The TPCPs thus act as the ideal reaction points with enhanced PCRR and suppressed HER.However,the initial synthesis of triple-phase photocatalysts tends to possess a lower bulk density of TPCPs due to the simple structure leading to limited active points and CO_(2) adsorption sites.Here,based on constructing a hydrophobic hierarchical porous TiO_(2)(o-HPT)with interconnected macropores and mesopores structure,we have significantly increased the density of TPCPs in a unit volume of the photocatalyst.Compared with hydrophobic macroporous TiO_(2)(o-MacPT)or mesoporous TiO_(2)(o-MesPT),the o-HPT with increased TPCP density leads to enhanced photoactivity,enabling a high methanol production rate with 1111.5μmol g^(−1) h^(−1) from PCRR.These results emphasize the significance of high-density TPCPs design and propose a potential path for developing efficient PCRR systems.展开更多
The facile reconfiguration of phases plays a pivotal role in enhancing the electrocatalytic production of H2 through heterostructure formation.While chemical methods have been explored extensively for this purpose,pla...The facile reconfiguration of phases plays a pivotal role in enhancing the electrocatalytic production of H2 through heterostructure formation.While chemical methods have been explored extensively for this purpose,plasma-based techniques offer a promising avenue for achieving heterostructured nano-frameworks.However,the conventional plasma approach introduces complexities,leading to a multi-step fabrication process and challenges in precisely controlling partial surface structure modulation due to the intricate interaction environment.In our pursuit of heterostructures with optimized oxygen evolution reaction(OER)behavior,we have designed a facile auxiliary insulator-confined plasma system to directly attain a Ni_(3)N-NiO heterostructure(hNiNO).By meticulously controlling the surface heating process during plasma processing,such approach allows for the streamlined fabrication of hNiNO nano-frameworks.The resulting nano-framework exhibits outstanding catalytic performance,as evidenced by its overpotential of 320 mV at a current density of 10 mA·cm^(-2),in an alkaline environment.This stands in stark contrast to the performance of NiO-covered Ni_(3)N fabricated using the conventional plasma method(sNiNO).Operando plasma diagnostics,coupled with numerical simulations,further substantiates the influence of surface heating due to auxiliary insulator confinement of the substrate on typical plasma parameters and the formation of the Ni_(3)N-NiO nanostructure,highlighting the pivotal role of controlled surface temperature in creating a high-performance heterostructured electrocatalyst.展开更多
Magnetic metal absorbers exhibit remarkable microwave absorption capacity.However,their practical application is severely limited due to their susceptibility to corrosion,particularly in marine environ-ments.To addres...Magnetic metal absorbers exhibit remarkable microwave absorption capacity.However,their practical application is severely limited due to their susceptibility to corrosion,particularly in marine environ-ments.To address this challenge,we propose a novel approach involving the modification and control of FeCo/rGO microwave absorbers using rare earth lanthanum(La).This strategy aims to achieve both high-performance microwave absorption and enhanced resistance to marine corrosion.In this study,we employ a La_(2)O_(3) modifying control strategy to refine the FeCo magnetic particles and coat them with CoFe_(2)O_(4) on the surface,leveraging the pinning effect of in situ generated La_(2)O_(3) .This process enhances the interface polarization of the absorbers,thereby improving their electromagnetic performance and ma-rine corrosion resistance.Consequently,the La_(2)O_(3) modified FeCo@rGO composites exhibit broadband ab-sorption,covering a wide frequency range of 6.11 GHz at 1.55 mm.Notably,the electromagnetic proper-ties of the La_(2)O_(3) modified FeCo@rGO absorbers remain stable even after prolonged exposure to a 3.5 wt% NaCI solution,simulating marine conditions,for at least 15 days.Furthermore,we perform first-principle calculations on FeCo and FeCo-O to validate the corrosion resistance of the La_(2)O_(3) modified FeCo@rGO composites at the atomic level.This comprehensive investigation explores the control of rare earth lan-thanum modification on the size of magnetic metal particles,enabling efficient electromagnetic wave absorption and marine corrosion resistance.The results of this study provide a novel and facile strategy for the control of microwave absorbers,offering promising prospects for future research and development in this field.展开更多
Photocatalytic hydrogen generation represents a promising strategy for the establishment of a sustainable and environmentally friendly energy reservoir.However,the current solar-to-hydrogen conversion efficiency is no...Photocatalytic hydrogen generation represents a promising strategy for the establishment of a sustainable and environmentally friendly energy reservoir.However,the current solar-to-hydrogen conversion efficiency is not yet sufficient for practical hydrogen production,highlighting the need for further research and development.Here,we report the synthesis of a Sn-doped TiO_(2)continuous homojunction hollow sphere,achieved through controlled calcination time.The incorporation of a gradient doping profile has been demonstrated to generate a gradient in the band edge energy,facilitating carrier orientation migration.Furthermore,the hollow sphere’s outer and inner sides provide spatially separated reaction sites allowing for the separate acceptance of holes and electrons,which enables the rapid utilization of carriers after separation.As a result,the hollow sphere TiO_(2)with gradient Sn doping exhibits a significantly increased hydrogen production rate of 20.1 mmol·g^(−1)·h^(−1).This study offers a compelling and effective approach to the designing and fabricating highly efficient nanostructured photocatalysts for solar energy conversion applications.展开更多
基金financially supported by the National Natural Science Foundation of China(22378204,22008121,51790492)the National Outstanding Youth Science Fund Project of National Natural Science Foundation of China(T2125004)+1 种基金the Funding of NJUST(No.TSXK2022D002)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX23_0454)。
文摘The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of catalysts.However,there is a contradiction in wettability requirements for the two half-reactions.Specifically,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)reactants.Conversely,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic catalyst.This was achieved through a selectively hydrophobic modification method and a charge-transfer-control strategy.Consequently,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark catalyst.This innovative approach holds great potential for application in universal overall reactions involving gas participation.
基金This work was financially supported by the National Natural Science Foundation of China(U21A2093 and 52102370)the Natural Science Foundation of Shaanxi Province(2022JM-260)+2 种基金the Shanghai Key Laboratory of R&D for Metallic Functional Materials(2021-01)and Open Fund of Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province(JBGS014)Open access funding provided by Shanghai Jiao Tong University
文摘Precisely reducing the size of metal-organic frameworks(MOFs)derivatives is an effective strategy to manipulate their phase engineering owing to size-dependent oxidation;however,the underlying relationship between the size of derivatives and phase engineering has not been clarified so far.Herein,a spatial confined growth strategy is proposed to encapsulate small-size MOFs derivatives into hollow carbon nanocages.It realizes that the hollow cavity shows a significant spatial confinement effect on the size of confined MOFs crystals and subsequently affects the dielectric polarization due to the phase hybridization with tunable coherent interfaces and heterojunctions owing to size-dependent oxidation motion,yielding to satisfied microwave attenuation with an optimal reflection loss of-50.6 d B and effective bandwidth of 6.6 GHz.Meanwhile,the effect of phase hybridization on dielectric polarization is deeply visualized,and the simulated calculation and electron holograms demonstrate that dielectric polarization is shown to be dominant dissipation mechanism in determining microwave absorption.This spatial confined growth strategy provides a versatile methodology for manipulating the size of MOFs derivatives and the understanding of size-dependent oxidation-induced phase hybridization offers a precise inspiration in optimizing dielectric polarization and microwave attenuation in theory.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.12274230,91950102,and 11834004)the Funding of Nanjing University of Science and Technology (Grant No.TSXK2022D005)the Postgraduate Research&Practice Innovation Program of Jiangsu Province of China (Grant No.KYCX230443)。
文摘We calibrate the macroscopic vortex high-order harmonic generation(HHG)obtained by the quantitative rescattering(QRS)model to compute single-atom induced dipoles against that by solving the time-dependent Schr?dinger equation(TDSE).We show that the QRS perfectly agrees with the TDSE under the favorable phase-matching condition,and the QRS can accurately predict the main features in the spatial profiles of vortex HHG if the phase-matching condition is not good.We uncover that harmonic emissions from short and long trajectories are adjusted by the phase-matching condition through the time-frequency analysis and the QRS can simulate the vortex HHG accurately only when the interference between two trajectories is absent.This work confirms that it is an efficient way to employ the QRS model in the single-atom response for precisely simulating the macroscopic vortex HHG.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.91950102,12274230,and 11834004)the Funding of Nanjing University of Science and Technology (Grant No.TSXK2022D005)。
文摘Synthesis of multi-color laser pulses has been developed as a promising way to improve low conversion efficiency of high-order harmonic generation(HHG). Here we systematically study the effect of laser focus in a two-color waveform on generation of macroscopic HHG in soft x-rays. We find that the dependence of HHG yields on laser focus at low or high gas pressure is sensitive to the characteristics of single-atom harmonic response, in which “short”-or “long”-trajectory emissions can be selectively controlled by changing the waveform of two-color synthesized laser pulse. We uncover the phase-matching mechanism of HHG in the gas medium by examining the propagation of the two-color waveform and the evolution of time-frequency emissions of high-harmonic field. We further reveal that the nonlinear effects, such as geometric phase, atomic dispersion, and plasma defocusing, are responsible for modification of two-color waveform upon propagation. This work can be used to find better macroscopic conditions for generating soft x-ray HHG by employing two-color optimized waveforms.
基金supported by the National Natural Science Foundation of China (NSFC) (52171206, 51762013)the Key Project of Hebei Natural Science Foundation (E20202201030)+5 种基金the BeijingTianjin-Hebei Collaborative Innovation Community Construction Project (21344301D)The Second Batch of Young Talent of Hebei Province (70280016160250, 70280011808)the Key Fund in Hebei Province Department of Education China (ZD2021014)The Central Government Guide Local Funding Projects for Scientific and Technological Development (216Z4404G, 206Z4402G)the Interdisciplinary Research Program of Natural Science of Hebei University (DXK202107)the China Postdoctoral Science Foundation (No. 2021M701718)。
文摘The development of high-efficiency and cost-effective bifunctional electrocatalysts for overall water splitting remains a formidable challenge.Herein,FeNi-Nd_(2)O_(3) nanoparticles anchored on N-doped carbon nanotubes(FeNi-Nd_(2)O_(3)/NCN) are designed for highly effective overall water splitting via a facile two-step hydrothermal approach.The synthetic FeNi-Nd_(2)O_(3) hetero-trimers(Fe 2p-Ni 2p-Nd 3d orbital coupling)on NCN achieve excellent oxygen evolution reaction(OER) and hydrogen evolution reaction(HER) activities with overpotentials of 270 and 120 mV at 10 mA cm^(-2) in 1 M KOH solution.Moreover,a small voltage of 1.52 V at 10 mA cm^(-2) is achieved when FeNi-Nd_(2)O_(3)/NCN is assessed as bifunctional catalyst for overall water splitting,which is superior to the typically integrated Pt/C and RuO_(2) counterparts(1.54 V at 10 mA cm^(-2)).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy show that the remarkably improved activity is originated from Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction.Furthermore,density functional theory(DFT) calculations indicate that the lattice contraction reduces binding energies of intermediates by downshifting the position of FeNi bimetallic d-band center relative to the Fermi level to optimize catalytic performance.Therefore,the Nd_(2)O_(3)-induced FeNi bimetallic lattice contraction may provide a new perspective for designing and synthesizing innovative catalytic systems.
基金Project supported by the National Natural Science Foundation of China (Grant No. U1930402)support from the Project Funded by China Postdoctoral Science Foundation (Grant Nos. 2020M680006 and 2021T140045)+1 种基金support from the National Natural Science Foundation of China (Grant No. 12004184)the Natural Science Foundation of Jiangsu Province, China (Grants No. BK20190428)。
文摘The contradiction between classical and quantum physics can be identified through quantum contextuality, which does not need composite systems or spacelike separation. Contextuality is proven either by a logical contradiction between the noncontextuality hidden variable predictions and those of quantum mechanics or by the violation of noncontextual inequality. We propose an experimental scheme of state-independent contextual inequality derived from the Mermin proof of the Kochen–Specker(KS) theorem in eight-dimensional Hilbert space, which could be observed either in an individual system or in a composite system. We also show how to resolve the compatibility problems. Our scheme can be implemented in optical systems with current experiment techniques.
基金Supported by the National Natural Science Foundation of China (12075121),the Natural Science Foundation of Jiangsu Province (BK20190067),and the Fundamental Research Funds for the Central Universities (30922010312)。
文摘Recently, the synthesis of new elements above Z = 118 has been a hot topic in nuclear physics. Meanwhile, the α-decay chain is expected to be the unique tool to identify these heaviest nuclei. We have systematically calculated the α-decay energies and half-lives on the same footing for superheavy nuclei (SHN) within the cluster model along with a slightly modified Woods-Saxon (W.S.) potential as the nuclear potential. Based on the available experimental data, the key radius parameter (R) in the α-core potential is determined via the systematic trend from the α-decay and isotopic chains. The α-decay energy (Qα) values and half-lives are then obtained simultaneously for those unknown SHN in the range of 117 ≤ Z ≤ 120, during which the decay width is obtained using a new treatment for the asymptotic behavior of the α-core wave function. The theoretical values and experimental data are found to be in excellent agreement for the nuclei ^(293,294)117 and ^(294)118 regardless of the method used to determine the R parameter. Predicting the α-decay chains for new elements Z = 119 and Z = 120 can be useful in ongoing or forthcoming experiments.
基金support from the National Natural Science Foundation of China(Grant No.12274229)is greatly acknowledged.
文摘X-ray photoelectron spectroscopy(XPS)is an important characterization tool in the pursuit of controllable fluorination of two-dimensional hexagonal boron nitride(h-BN).However,there is a lack of clear spectral interpretation,and seemingly conflicting measurements exist.To discern the structure−spectroscopy relation,we performed a comprehensive first-principles study on the boron 1s edge XPS of fluorinated h-BN(F-BN)nanosheets.By gradually introducing 1−6 fluorine atoms into different boron or nitrogen sites,we created various F-BN structures with doping ratios ranging from 1 to 6%.Our calculations reveal that fluorines landed at boron or nitrogen sites exert competitive effects on the B 1s binding energies(BEs),leading to red or blue shifts in different measurements.Our calculations affirmed the hypothesis that fluorination affects 1s BEs of all borons in theπ-conjugated system,opposing the transferability from h-BN to F-BN.Additionally,we observe that BE generally increases with higher fluorine concentration when both borons and nitrogens are nonexclusively fluorinated.These findings provide critical insights into how fluorination affects boron’s 1s BEs,contributing to a better understanding of fluorination functionalization processes in h-BN and its potential applications in materials science.
基金National Key R&D Program of China (2021YFA1200804)National Natural Science Foundation of China (62274175 and 61927813)+2 种基金Jiangsu Province Key R&D Program (BE2023009-5 and BK20232044)Suzhou Basic Research Program (SJC2023004)The support from the Vacuum Interconnected Nanotech Workstation (Nano-X) of Suzhou Institute of Nanotech and Nanobionics (SINANO),Chinese Academy of Sciences is also acknowledged。
文摘Black phosphorus(BP)has been regarded as a promising two-dimensional semiconductor due to its excellent properties including high carrier mobility and widely tunable direct bandgap.Despite extensive interest as well as research progress,the preparation of large-size and high-quality BP single crystal in high throughput still remains challenging.Here,a facile growth of centimeter-sized BP single crystal flakes with dozens of throughput per batch is achieved by using bidirectional vapor transport(BVT)method.High crystal quality is confirmed by structural and spectrum characterizations,with an X-ray diffraction rocking curve peak half-height width of only 0.02°.The as-grown BP single crystal flake with smooth cleavage plane can be easily exfoliated into large scale nanosheets.Field-effect transistors fabricated based on the BP by such approach show excellent performance including reliable carrier mobility up to 1150 cm^(2) V^(−1) s^(−1) and on/off current ratio of~10^(6)at 15 K.This approach is also applicable to various doped-BP,such as As-BP,Se-BP,Te-BP,etc.The ability to grow centimeter-sized BP single crystal flakes in high yield will accelerate the research and applications of BP-based electronics and optoelectronics.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.62374088 and 12074193)。
文摘Ohmic contacts are fundamental components in semiconductor technology,facilitating efficient electrical connection and excellent device performance.We employ first-principles calculations to show that semimetallic graphene is a natural Ohmic contact partner of monolayer semiconducting black arsenic(BAs),for which the top of the valence band is below the Fermi energy of the order of 10~2 meV.The Ohmic contact arises from the giant Stark effect induced by van der Waals electron transfer from BAs to graphene,which does not destroy their respective band features.Remarkably,we show that this intrinsic Ohmic contact remains robust across a wide range of interlayer distances(adjustable by strain)or vertical electric fields,whereas the weak spin splitting of the order of 1 meV induced by symmetry breaking plays little part in Ohmic contact.These findings reveal the potential applications of graphene–BAs in ultralow dissipation transistors.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 12034009, 91961204, and 11974134)。
文摘As a fundamental thermodynamic variable, pressure can alter the bonding patterns and drive phase transitions leading to the creation of new high-pressure phases with exotic properties that are inaccessible at ambient pressure. Using the swarm intelligence structural prediction method, the phase transition of TiF_(3), from R-3c to the Pnma phase, was predicted at high pressure, accompanied by the destruction of TiF_6 octahedra and formation of TiF_8 square antiprismatic units. The Pnma phase of TiF_(3), formed using the laser-heated diamond-anvil-cell technique was confirmed via high-pressure x-ray diffraction experiments. Furthermore, the in situ electrical measurements indicate that the newly found Pnma phase has a semiconducting character, which is also consistent with the electronic band structure calculations. Finally, it was shown that this pressure-induced phase transition is a general phenomenon in ScF_(3), VF_(3), CrF_(3), and MnF_(3), offering valuable insights into the high-pressure phases of transition metal trifluorides.
基金supported by the National Natural Science Foundation of China(Grant Nos.11904171,and 62221004)the Fundamental Research Funds for the Central Universities(Grant No.30922010807)。
文摘Quantum error correction is essential for achieving reliable quantum information processing tasks,as it can mitigate the detrimental effects of noise by encoding single-qubit information into a larger quantum system.However,the generation of distributed entanglement between logical qubits located within two spatially separated nodes presents a significant resource-intensive challenge that has yet to be overcome.Here we present a heralded protocol for generating distributed entanglement between two nonlocal error-protected logical qubits.A high-dimensional single photon can evolve physical qubits into a logical qubit that entangles with the photon and then converts logical qubit-photon entanglement into entanglement between two logical qubits,when the photon state is properly tuned and an effective photon-spin interface between single photons and individual spins is exploited.Furthermore,the success of the entanglement generation is heralded by the detection of the photon,and the corresponding efficiency can,in principle,approach unity.These distinguished features make our protocol highly appealing for future large-scale quantum technologies.
基金supported by the National Key R&D Program of China(2021YFA1501503)the National Natural Science Foundation of China(T2125004,22008121,22121004)+1 种基金the Haihe Laboratory of Sustainable Chemical Transformations(CYZC202107)the Program of Introducing Talents of Discipline to Universities(No.BP0618007)and the Xplorer Prize for financial support.
文摘This review describes recent advances in wettability adjustment to improve the main green energy conversion and storage systems,i.e.,photocatalysis and electrocatalysis.Because both are redox reactions involving electron behavior,they follow a similar pattern in the surface reaction step,which is related to wettability adjustment.Thus,we consider photocatalysis and electrocatalysis together in terms of mass transfer adjustment based on commonalities,aiming to understand the fundamentals more deeply and bring greater mutual inspiration to photocatalysis and electrocatalysis.The theoretical basis is first laid out,and then various strategies are introduced.Subsequently,according to the different requirements of mass transfer,we classify the photocatalytic and electrocatalytic reactions into gas consumption reactions preferring hydrophobic surfaces,and gas evolution reactions preferring hydrophilic surfaces.Pollutant degradation reactions involving different water-soluble substrates are also mentioned.Further,we introduce the specific optimization effect of wettability regulation on the reaction,and the mechanism behind the effect.This comprehensive and insightful review will provide a strategic guide to the reasonable design and development of wettability-optimized photocatalytic and electrocatalytic systems.
基金supported by the National Natural Science Foundation of China(Grant Nos.91950102 and 11834004)the Natural Science Foundation of Jiangsu Province(Grant No.BK20220925)the Funding of Nanjing University of Science and Technology(NJUST)(Grant No.TSXK2022D005)
文摘Attosecond transient absorption(ATA)has been developed as an all-optical technique for probing electron dynamics in matter.Here we present a scheme that can modify the laserinduced state and the corresponding ATA spectrum via excitation by a pair of XUV attosecond pulses and by a time-delayed mid-infrared(MIR)laser probe.Different from the scheme of the electronic excitation by a single XUV attosecond pulse,the application of a pair of XUV pulses provides extra degrees of freedom,such as the time delay and the intensity ratio between two XUV pulses,which make it possible to adjust the pump process,resulting in the modification of the ATA spectrum.We show that by varying the time delay between the two XUV pulses,the population of the dark state and the ATA spectrum of the laser-induced state have periodic modulations.We also demonstrate that the peak of the ATA spectrum of the laser-induced state appears at a fixed time delay between the XUV pair and the MIR laser when the intensity ratio is large,and it changes with the time delay when the intensity ratio is small,which can be related to either one of two peaks in the population of the dark state.
基金Supported by the National Natural Science Foundation of China(12075121 and 11605089)by the Natural Science Foundation of Jiangsu Province(BK20190067 and BK20150762)。
文摘In addition to the Coulomb displacement energy,the residual differences between the binding energies of mirror nuclei(a pair of nuclei with the same mass number plus interchanged proton and neutron numbers)contribute to the shell effect via the valence scheme in this study.To this end,one linear combining type of valence nucleon number,namely,αNp+βNn,is chosen to tackle this shell correction,in which Npand Nnare the valence proton and neutron numbers with respect to the nearest shell closure,respectively.The mass differences of mirror nuclei,as the sum of the empirical Coulomb displacement energy and shell effect correction,are then used to obtain the binding energies of proton-rich nuclei through the available data of their mirror partners to explore the proton dripline of the nuclear chart.
基金This work was supported by the National Natural Science Foundation of China(NNSFC)(Nos.61975080 and 11774176).
文摘The propagating of laser-generated ultrasonic waves in K9 glass was investigated. Many methods have been developed to detect the laser ultrasound since laser ultrasonic waves can be used to measure material parameters or characterize materials properties. In order to reduce the measuring time, a Mach–Zehnder interferometer, a full field measuring tool,was preferred in this paper. The ultrasonic wave was produced on the K9 glass surface by a Q-switched Nd:YAG laser absorbed in a liquid layer. The interferograms were then taken at various delay times by a CCD camera after single pulse induced laser ultrasonic waves. Ultrasonic waves in the K9 glass can be observed from interferogram images. The results provide an understanding of laser ultrasound propagation in K9 glass in the lifetime.
基金National Natural Science Foundation of China(Nos.22008121,11774173,51790492)the National Outstanding Youth Science Fund Project of National Natural Science Foundation of China(No.T2125004)+2 种基金the Fundamental Research Funds for the Central Universities(Nos.30920032204,30920041115)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(No.2022-K12)Funding of NJUST(No.TSXK2022D002)for financial support.
文摘The efficiency of photocatalytic CO_(2) reduction reaction(PCRR)is restricted by the low solubility and mobility of CO_(2) in water,poor CO_(2) adsorption capacity of catalyst,and competition with hydrogen evolution reaction(HER).Recently,hydrophobic modification of the catalyst surface has been proposed as a potential solution to induce the formation of triple-phase contact points(TPCPs)of CO_(2)(gas phase),H_(2) O(liquid phase),and catalysts(solid phase)near the surface of the catalyst,enabling direct delivery of highly concentrated CO_(2) molecules to the active reaction sites,resulting in higher CO_(2) and lower H+surface concentrations.The TPCPs thus act as the ideal reaction points with enhanced PCRR and suppressed HER.However,the initial synthesis of triple-phase photocatalysts tends to possess a lower bulk density of TPCPs due to the simple structure leading to limited active points and CO_(2) adsorption sites.Here,based on constructing a hydrophobic hierarchical porous TiO_(2)(o-HPT)with interconnected macropores and mesopores structure,we have significantly increased the density of TPCPs in a unit volume of the photocatalyst.Compared with hydrophobic macroporous TiO_(2)(o-MacPT)or mesoporous TiO_(2)(o-MesPT),the o-HPT with increased TPCP density leads to enhanced photoactivity,enabling a high methanol production rate with 1111.5μmol g^(−1) h^(−1) from PCRR.These results emphasize the significance of high-density TPCPs design and propose a potential path for developing efficient PCRR systems.
基金supported by the National Natural Science Foundation of China(Nos.12304020,21905118,and 22378204)National Science Fund for Distinguished Young Scholars(No.T2125004)+1 种基金the Natural Science Foundation of Jiangsu Province(No.BK20230909)Fundamental Research Funds for the Central Universities(No.30923011013)。
文摘The facile reconfiguration of phases plays a pivotal role in enhancing the electrocatalytic production of H2 through heterostructure formation.While chemical methods have been explored extensively for this purpose,plasma-based techniques offer a promising avenue for achieving heterostructured nano-frameworks.However,the conventional plasma approach introduces complexities,leading to a multi-step fabrication process and challenges in precisely controlling partial surface structure modulation due to the intricate interaction environment.In our pursuit of heterostructures with optimized oxygen evolution reaction(OER)behavior,we have designed a facile auxiliary insulator-confined plasma system to directly attain a Ni_(3)N-NiO heterostructure(hNiNO).By meticulously controlling the surface heating process during plasma processing,such approach allows for the streamlined fabrication of hNiNO nano-frameworks.The resulting nano-framework exhibits outstanding catalytic performance,as evidenced by its overpotential of 320 mV at a current density of 10 mA·cm^(-2),in an alkaline environment.This stands in stark contrast to the performance of NiO-covered Ni_(3)N fabricated using the conventional plasma method(sNiNO).Operando plasma diagnostics,coupled with numerical simulations,further substantiates the influence of surface heating due to auxiliary insulator confinement of the substrate on typical plasma parameters and the formation of the Ni_(3)N-NiO nanostructure,highlighting the pivotal role of controlled surface temperature in creating a high-performance heterostructured electrocatalyst.
基金National Key R&D Program of China(No.2021YFB3502500)National Natural Science Foundation of China(Nos.52172091 and 52172295)+3 种基金Natural Science Foundation of Jiangsu Province(No.BK20211199)Scientific Research Fund of AnHui Provincial Education Department(No.KJ2021A0034)Open Fund of Key Laboratory of Materials Preparation and Protection for Harsh Environment(Nanjing University of Aeronautics and Astronautics)Ministry of Industry and Information Technology(No.56XCA22042).
文摘Magnetic metal absorbers exhibit remarkable microwave absorption capacity.However,their practical application is severely limited due to their susceptibility to corrosion,particularly in marine environ-ments.To address this challenge,we propose a novel approach involving the modification and control of FeCo/rGO microwave absorbers using rare earth lanthanum(La).This strategy aims to achieve both high-performance microwave absorption and enhanced resistance to marine corrosion.In this study,we employ a La_(2)O_(3) modifying control strategy to refine the FeCo magnetic particles and coat them with CoFe_(2)O_(4) on the surface,leveraging the pinning effect of in situ generated La_(2)O_(3) .This process enhances the interface polarization of the absorbers,thereby improving their electromagnetic performance and ma-rine corrosion resistance.Consequently,the La_(2)O_(3) modified FeCo@rGO composites exhibit broadband ab-sorption,covering a wide frequency range of 6.11 GHz at 1.55 mm.Notably,the electromagnetic proper-ties of the La_(2)O_(3) modified FeCo@rGO absorbers remain stable even after prolonged exposure to a 3.5 wt% NaCI solution,simulating marine conditions,for at least 15 days.Furthermore,we perform first-principle calculations on FeCo and FeCo-O to validate the corrosion resistance of the La_(2)O_(3) modified FeCo@rGO composites at the atomic level.This comprehensive investigation explores the control of rare earth lan-thanum modification on the size of magnetic metal particles,enabling efficient electromagnetic wave absorption and marine corrosion resistance.The results of this study provide a novel and facile strategy for the control of microwave absorbers,offering promising prospects for future research and development in this field.
基金the National Natural Science Foundation of China(Nos.22008121,11774173,and 51790492)the National Outstanding Youth Science Fund Project of National Natural Science Foundation of China(No.T2125004)+2 种基金the Fundamental Research Funds for the Central Universities(Nos.30920032204,30920021307,and 30920041115)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(No.2022-K12)the Funding of NJUST(No.TSXK2022D002)for financial support.
文摘Photocatalytic hydrogen generation represents a promising strategy for the establishment of a sustainable and environmentally friendly energy reservoir.However,the current solar-to-hydrogen conversion efficiency is not yet sufficient for practical hydrogen production,highlighting the need for further research and development.Here,we report the synthesis of a Sn-doped TiO_(2)continuous homojunction hollow sphere,achieved through controlled calcination time.The incorporation of a gradient doping profile has been demonstrated to generate a gradient in the band edge energy,facilitating carrier orientation migration.Furthermore,the hollow sphere’s outer and inner sides provide spatially separated reaction sites allowing for the separate acceptance of holes and electrons,which enables the rapid utilization of carriers after separation.As a result,the hollow sphere TiO_(2)with gradient Sn doping exhibits a significantly increased hydrogen production rate of 20.1 mmol·g^(−1)·h^(−1).This study offers a compelling and effective approach to the designing and fabricating highly efficient nanostructured photocatalysts for solar energy conversion applications.
