Crystallineγ-Ga_(2)O_(3)@rGO core-shell nanostructures are synthesized in gram scale,which are accomplished by a facile sonochemical strategy under ambient condition.They are composed of uniformγ-Ga_(2)O_(3)nanosphe...Crystallineγ-Ga_(2)O_(3)@rGO core-shell nanostructures are synthesized in gram scale,which are accomplished by a facile sonochemical strategy under ambient condition.They are composed of uniformγ-Ga_(2)O_(3)nanospheres encapsulated by reduced graphene oxide(rGO)nanolayers,and their formation is mainly attributed to the existed opposite zeta potential between the Ga_(2)O_(3)and rGO.The as-constructed lithium-ion batteries(LIBs)based on as-fabricatedγ-Ga_(2)O_(3)@rGO nanostructures deliver an initial discharge capacity of 1000 mAh g^(-1)at 100 mA g^(-1)and reversible capacity of 600 mAh g^(-1)under 500 mA g^(-1)after 1000 cycles,respectively,which are remarkably higher than those of pristineγ-Ga_(2)O_(3)with a much reduced lifetime of 100 cycles and much lower capacity.Ex situ XRD and XPS analyses demonstrate that the reversible LIBs storage is dominant by a conversion reaction and alloying mechanism,where the discharged product of liquid metal Ga exhibits self-healing ability,thus preventing the destroy of electrodes.Additionally,the rGO shell could act robustly as conductive network of the electrode for significantly improved conductivity,endowing the efficient Li storage behaviors.This work might provide some insight on mass production of advanced electrode materials under mild condition for energy storage and conversion applications.展开更多
Two-dimensional(2D)oxides have been the focus of substantial research interest recently,owing to their fascinating physico-chemical properties.However,fabrication of large-area 2D oxide materials in a controlled manne...Two-dimensional(2D)oxides have been the focus of substantial research interest recently,owing to their fascinating physico-chemical properties.However,fabrication of large-area 2D oxide materials in a controlled manner under mild conditions still remains a formidable challenge.Herein,we develop a facile and universal strategy based on the sonochemistry approach for controllable and large-area growth of quasi-aligned single-crystalline ZnO nanosheets on a Zn substrate(Zn@SC-ZnO)under ambient conditions.The obtained ZnO nanosheets possess the desired exclusively exposed(001)facets,which have been confirmed to play a critical role in significantly reducing the activation energy and facilitating the stripping/plating processes of Zn.Accordingly,the constructed Zn@SC-ZnO||Zn@SC-ZnO symmetric cell has very low polarization overpotential down to~20 mV,with limited dendrite growth and side reactions for Zn anodes.The developed Zn@SC-ZnO//MnO_(2)aqueous Zn-ion batteries(ZIBs)show a voltage efficiency of 88.2%under 500 mA g^(-1)at the stage of 50%depth of discharge,which is state of the art for ZIBs reported to date.Furthermore,the as-assembled large-size cell(5 cm×5 cm)delivers an open circuit potential of 1.648 V,and can be robustly operated under a high current of 20 mA,showing excellent potential for future scalable applications.展开更多
Conversion of solar energy into H_(2) by photoelectrochemical(PEC)water splitting is recognized as an ideal way to address the growing energy crisis and environmental issues.In a typical PEC cell,the construction of p...Conversion of solar energy into H_(2) by photoelectrochemical(PEC)water splitting is recognized as an ideal way to address the growing energy crisis and environmental issues.In a typical PEC cell,the construction of photoanodes is crucial to guarantee the high efficiency and stability of PEC reactions,which fundamentally rely on rationally designed semiconductors(as the active materials)and substrates(as the current collectors).In this review work,we start with a brief introduction of the roles of substrates in the PEC process.Then,we provide a systematic overview of representative strategies for the controlled fabrication of photoanodes on rationally designed substrates,including conductive glass,metal,sapphire,silicon,silicon carbide,and flexible substrates.Finally,some prospects concerning the challenges and research directions in this area are proposed.展开更多
Currently,the major challenge in terms of research on K-ion batteries is to ensure that they possess satisfactory cycle stability and specific capacity,especially in terms of the intrinsically sluggish kinetics induce...Currently,the major challenge in terms of research on K-ion batteries is to ensure that they possess satisfactory cycle stability and specific capacity,especially in terms of the intrinsically sluggish kinetics induced by the large radius of K+ions.Here,we explore high-performance K-ion half/full batteries with high rate capability,high specific capacity,and extremely durable cycle stability based on carbon nanosheets with tailored N dopants,which can alleviate the change of volume,increase electronic conductivity,and enhance the K+ion adsorption.The as-assembled K-ion half-batteries show an excellent rate capability of 468 mA h g^(−1) at 100 mA g^(−1),which is superior to those of most carbon materials reported to date.Moreover,the as-assembled half-cells have an outstanding life span,running 40,000 cycles over 8 months with a specific capacity retention of 100%at a high current density of 2000 mA g^(−1),and the target full cells deliver a high reversible specific capacity of 146 mA h g^(−1) after 2000 cycles over 2 months,with a specific capacity retention of 113%at a high current density of 500 mA g^(−1),both of which are state of the art in the field of K-ion batteries.This study might provide some insights into and potential avenues for exploration of advanced K-ion batteries with durable stability for practical applications.展开更多
Manganese-based oxide electrode materials suffer from severe Jahn-Teller(J-T)distortion,leading to severe cycle instability in sodium ion storage.However,it is difficult to adjust the electron at d orbitals exactly to...Manganese-based oxide electrode materials suffer from severe Jahn-Teller(J-T)distortion,leading to severe cycle instability in sodium ion storage.However,it is difficult to adjust the electron at d orbitals exactly to a low spin state to eliminate orbital degeneracy and suppress J-T distortion fundamentally.This article constructed concentration-controllable Mn/O coupled vacancy and amorphous network in Mn_(3)O_(4) and coated it with nitrogen-doped carbon aerogel(Mn_(3-x)O_(4-y)@NCA).The existence of Mn/O vacancies has been confirmed by scanning transmission electron microscopy(STEM)and positron annihilation lifetime spectroscopy(PALS).Atomic absorption spectroscopy(AAS)and X-ray photoelectron spectroscopy(XPS)determine the most optimal ratio of Mn/O vacancies for sodium ion storage is 1:2.Density functional theory(DFT)calculations prove that Mn/O coupled vacancies with the ratio of 1:2could exactly induce a low spin states and a d~4 electron configuration of Mn,suppressing the J-T distortion successfully.The abundant amorphous regions can shorten the transport distance of sodium ions,increase the electrochemically active sites and improve the pseudocapacitance response.From the synergetic effect of Mn/O coupled vacancies and amorphous regions,Mn_(3-x)O_(4-y)@NCA exhibits an energy density of 37.5 W h kg^(-1)and an ultra-high power density of 563 W kg^(-1)in an asymmetric supercapacitor.In sodium-ion batteries,it demonstrates high reversible capacity and exceptional cycling stability.This research presents a new method to improve the Na^(+)storage performance in manganese-based oxide,which is expected to be generalized to other structural distortion.展开更多
Anion exchange membrane fuel cell(AEMFC)technology is attracting intensive attention,due to its great potential by using non-precious-metal catalysts(NPMCs)in the cathode and cheap bipolar plate materials in alkaline ...Anion exchange membrane fuel cell(AEMFC)technology is attracting intensive attention,due to its great potential by using non-precious-metal catalysts(NPMCs)in the cathode and cheap bipolar plate materials in alkaline media.However,in such case,the kinetics of hydrogen oxidation reaction(HOR)in the anode is two orders of magnitude sluggish than that of acidic electrolytes,which is recognized as the grand challenge in this field.Herein,we report the rationally designed Ni nanoparticles encapsulated by N-doped graphene layers(Ni@NG)using a facile pyrolysis strategy.Based on the density functional theory calculations and electrochemical performance analysis,it is witnessed that the rich Pyridinic-N within the graphene shell optimizes the binding energy of the intermediates,thus enabling the fundamentally enhanced activity for HOR with robust stability.As a proof of concept,the resultant Ni@NG sample as the anode with a low loading(1.8 mg cm^(-2))in AEMFCs delivers a high peak power density of 500 mW cm^(-2),outperforming all of those of NPMC-based analogs ever reported.展开更多
The sluggish kinetics for water oxidation is recognized as one of the major problems for the unsatisfied photoelectrochemical(PEC) performance. Herein, we developed a feasible strategy based on in-situ selective surfa...The sluggish kinetics for water oxidation is recognized as one of the major problems for the unsatisfied photoelectrochemical(PEC) performance. Herein, we developed a feasible strategy based on in-situ selective surface cation exchange, for activating surface water oxidation reactivity toward boosted PEC water oxidation of BiVO_(4) photoanodes with fundamentally improved surface charge transfer. The asconstructed Co/BiVO_(4) photoanodes exhibit 2.6 times increase in photocurrent density with superior stability, in comparison to those of pristine counterpart. Moreover, the faradaic efficiency of as-fabricated photoanode can be up to ~ 95% at 1.23 V(vs. RHE). The unique selective replacement of Bi by Co on the surface could modify the electronic structure of BiVO_(4) with reduced energy barrier of the deprotonation of OH^(+) to O, thus favoring the overall excellent PEC performance of Co/BiVO_(4) photoanode.展开更多
We report the scalable fabrication of CdS/ZnS 1D/2D heterojunctions under ambient air conditions(i.e.,room temperature and atmospheric pressure)in which ZnS nanoparticles are anchored on the surface of CdS nanosheets....We report the scalable fabrication of CdS/ZnS 1D/2D heterojunctions under ambient air conditions(i.e.,room temperature and atmospheric pressure)in which ZnS nanoparticles are anchored on the surface of CdS nanosheets.The as-formed heterojunctions exhibit a significantly enhanced photocatalytic H_(2) evolution rate of 14.02 mmol h^(-1) g^(-1) when irradiated with visible light,which is~10 and 85 times higher than those of pristine CdS nanosheets and CdS nanoparticles,respectively,and superior to most of the CdS-based photocatalysts reported to date.Furthermore,they provide robust photocatalytic performance with demonstratable stability over 58 h,indicating their potential for practical applications.The formation of 1D/2D heterojunctions not only provides improved exposed active sites that respond to illumination but also provides a rapid pathway to generate photogenerated carriers for efficient separation and transfer through the matrix of single-crystalline CdS nanosheets.In addition,first-principles simulations demonstrate that the existence of rich Zn vacancies increases the energy level of the ZnS valence band maximum to construct type-II and Z-scheme mixed heterojunctions,which plays a critical role in suppressing the recombination of carriers with limited photocorrosion of CdS to enhance photocatalytic behavior.展开更多
Currently,the synthesis of nanostructures still encounters two grand challenges:one is the often-required high temperatures and/or high pressures,and the other is the scalable fabrication.Here,to break through such bo...Currently,the synthesis of nanostructures still encounters two grand challenges:one is the often-required high temperatures and/or high pressures,and the other is the scalable fabrication.Here,to break through such bottlenecks,we demonstrate an ambient-condition strategy for rapid mass production of fourthgeneration semiconductor Ga_(2)O_(3)nanoarchitectures assembled by single-crystalline nanosheets in a controlled manner based on sonochemistry.Their growth is fundamentally determined by the introduced ethanediamine in rationally designed source materials,which could not only protect the metal Ga against reacting with H_(2)O into GaOOH,but facilitate the reaction of Ga with OH·radicals for target crystalline Ga_(2)O_(3)nanostructures.As a proof of concept for applications,the as-fabricated Ga_(2)O_(3)nanoarchitectures exhibit superb performances for electromagnetic wave absorption with a reflection loss value of 52.2 dB at 8.1 GHz,and ammonia sensing with high sensitivity and selectivity at room temperature,representing their bright future to be commercially applied in modern devices.展开更多
To date,the synthesis of crystalline ZnO nanostructures was often performed under high temperatures and/or high pressures with tiny output,which limits their commercial applications.Herein,we report the progress on sy...To date,the synthesis of crystalline ZnO nanostructures was often performed under high temperatures and/or high pressures with tiny output,which limits their commercial applications.Herein,we report the progress on synthesizing single-crystalline ZnO nanosheets under ambient conditions(i.e.,room temperature(RT)and atmospheric pressure)based on a sonochemistry strategy.Furthermore,their controllable growth is accomplished by adjusting the pH values of solutions,enabling the tailored crystal growth habits on the polar-charged faces of ZnO along c-axis.As a proof of concept for their potential applications,the ZnO nanosheets exhibit highly efficient performance for sensing ammonia at RT,with ultrahigh sensitivity(S=610 at 100 ppm),excellent selectivity,rapid detection(response time/recover time=70 s/4 s),and outstanding detection limit down to 0.5 ppm,superior to those of all pure ZnO nanostructures and most ZnO-based composite counterparts ever reported.The present work might open a door for controllable production of ZnO nanostructures under mild conditions,and facilitate the exploration of modern gas sensors for detecting gaseous molecules at RT,which underscores their potential toward practical applications in opto-electronic nanodevices.展开更多
Single-crystalline Ni-rich cathodes can provide high energy density and capacity retention rates for lithium-ion batteries(LIBs).However,single-crystalline Ni-rich cathodes experience severe transition metal dissoluti...Single-crystalline Ni-rich cathodes can provide high energy density and capacity retention rates for lithium-ion batteries(LIBs).However,single-crystalline Ni-rich cathodes experience severe transition metal dissolution,irreversible phase transitions,and reduced structural stability during prolonged cycling at high voltage,which will significantly hinder their practical application.Herein,a Li4TeO5surface coating along with bulk Te-gradient doping strategy is proposed and developed to solve these issues for single-crystalline Ni-rich LiNi_(0.90)Co_(0.05)Mn_(0.05)O_(2)cathode(LTeO-1.0).It has been found that the bulk Te^(6+)gradient doping can lead to the formation of robust Te-O bonds that effectively inhibit H_(2)-H3 phase transformations and reinforce the lattice framework,and the in-situ Li4TeO5coating layer can act as a protective layer that suppresses the parasitic reactions and grain fragmentation.Besides,the modified material exhibits a higher Young's modulus,which will be conducive to maintaining significant structural and electrochemical stability under high-voltage conditions,Especially,the LTeO-1.0 electrode shows the improved Li^(+)diffusion kinetics and thermodynamic stability as well as high capacity retention of 95.83%and 82.12%after 200 cycles at the cut-off voltage of 4.3 and 4,5 V.Therefore,the efficacious dualmodification strategy will definitely contribute to enhancing the structural and electrochemical stability of single-crystalline Ni-rich cathodes and developing their application in LIBs.展开更多
Engineering the morphology of the support is effective in tuning the redox properties of active metals for efficient catalytic methane combustion via tailoring the metal-support interaction.Herein,uniform Ir nanoparti...Engineering the morphology of the support is effective in tuning the redox properties of active metals for efficient catalytic methane combustion via tailoring the metal-support interaction.Herein,uniform Ir nanoparticles supported on anatase TiO_(2)with different morphologies predominantly exposing{100},{101},and{001}planes were synthesized and tested for methane combustion.The CH_(4) catalytic activity shows a remarkable TiO_(2)-facet-dependent effect and follows the order of Ir/TiO_(2)-{100}>Ir/TiO_(2)-{101}>>Ir/TiO_(2)-{001}.Detailed characterizations and DFT calculations reveal that compared with Ir-TiO_(2)-{101}and Ir-TiO_(2)-{001}interfaces,the superior Ir-TiO_(2)-{100}interface facilitates the generation of electron-rich Ir species through more profound charge transfer from TiO_(2)-{100}to Ir atoms.The electron-rich Ir structure,featuring abundant defect oxygen vacancies,significantly enhances the redox properties of active Ir species and reduces the activation energy for breaking the initial C-H bond in CH_(4),resulting in the superior catalytic activity for methane combustion.These findings deepen fundamental insights into the TiO_(2)-facet-dependent reactivity of different Ir/TiO_(2)nanomaterials in methane oxidation and pave the way for designing efficient Ir-based methane oxidation catalysts.展开更多
One key step for advancing the widespread practical application of rechargeable metal-air batteries and water electrolysis fundamentally relies on the development of cost-effective multifunctional electrocata-lysts to...One key step for advancing the widespread practical application of rechargeable metal-air batteries and water electrolysis fundamentally relies on the development of cost-effective multifunctional electrocata-lysts toward oxygen and hydrogen-involving reactions.The present work initiates a tofu-derived one-pot strategy for green,facile,and mass production of highly active and stable catalyst toward oxygen reduc-tion/evolution and hydrogen evolution reactions,through the preparation of Fe/Co cross-linked tofu gel and the subsequent pyrolysis.Despite the free use of additional N/P precursors or pore-forming agents,the as-prepared materials comprise highly dispersive FeCo-rich phosphides nanoparticles and porous N,P co-doped carbon network inherited from the tofu skeleton.The resultant catalysts exhibit remarkably enhanced trifunctional activities as compared to the Fe_(2)P and Co_(2)P counterparts,along with better long-term stabilities than the benchmark RuO_(2)and Pt/C catalysts.Accordingly,the as-assembled Zn-air battery delivers a large power density(174 mW cm^(-2))with excellent cycle stability(the gap of charge/discharge voltage@10 mA cm^(-2)increases by 0.01 V after 720 h of operation,vs.0.16 V of Pt/C-RuO_(2)based battery after 378 h).Furthermore,the as-constructed alkaline electrolyzer just requires a small voltage of 1.55 V@10 mA cm^(-2),which outperforms nearly all of those of biomass-derived electrocatalysts ever reported,and that of noble metal catalysts-based electrolyzers(1.72 V@10 mA cm^(-2)for Pt/C-RuO_(2)),underscoring their bright future toward commercial applications in green energy conversion devices.展开更多
Rationally constructed new catalyst can promote carbon dioxide reduction reaction(CO_(2)RR)to valuable carbo-naceous fuels such as formate and CO,providing a promising strategy for low CO_(2)emissions.Herein,the syn-t...Rationally constructed new catalyst can promote carbon dioxide reduction reaction(CO_(2)RR)to valuable carbo-naceous fuels such as formate and CO,providing a promising strategy for low CO_(2)emissions.Herein,the syn-thesized Ni_(3)S_(2)@C as a highly efficient electro-catalyst exhibits remarkable selectivity for formate with 73.9%faradaic efficiency(FE)at-0.7 V vs.RHE.At high applied potential,it shows a high syngas evolution with CO/H_(2)ratios(0.54-3.15)that are suitable for typical downstream thermochemical reactions.The experimental and theoretical analyses demonstrate that the electron-rich Ni^(2+)in Ni_(3)S_(2)enhances the adsorption behavior of*OCHO intermediate,reduces the energy barrier of the formation of intermediates,and improves the selectivity of the formate product.Attenuated total reflection surface-enhanced infrared absorption spectra conducted in situ show that*OCHO intermediate is more likely to be generated and adsorbed on Ni_(3)S_(2),enhancing the selectivity and activity of the formate product.展开更多
High areal capacity is one of the critically important points for potassium-ion batteries(PIBs)for practical applications,which relies on high areal-massloading electrodes operating at high reversible capacity.However...High areal capacity is one of the critically important points for potassium-ion batteries(PIBs)for practical applications,which relies on high areal-massloading electrodes operating at high reversible capacity.However,it is remarkably restricted by the mechanical instability and sluggish charge transfer induced by the increased mass loading.To overcome such challenge,we report the rationally designed bimetallic selenides CoSe2/SnSe2 heterostructures confined in hierarchical carbon nanofibers(CSSe@CNFs),which enables the electrodes robust mechanical stability,enhanced electron transport,and reduced ion-diffusion energy barrier for facilitating reaction kinetics.Accordingly,an impressive areal mass loading up to 25.3 mg cm^(−2)was achieved,which endowed a high areal capacity of 7.58 mAh cm^(−2)for such a free-standing electrode.This is stateof-the-art among the PIBs,exceeding that of today’s industry standard(∼3 mAh cm^(−2)for LIBs).Furthermore,it delivered long-term stability over 3700 cycles at high current density(∼2 mA cm^(−2),vs 1 mA cm^(−2)in LIBs).Moreover,the as-constructed full battery achieved a high energy density of 172.8 Wh kg-1 at 0.05 A g^(−1)with a satisfied cycle stability over 2000 cycles at 2 A g^(−1)and high reversibility with Coulombic efficiency of 100%;thus,signifying its bright future toward commercial application for advanced PIBs.展开更多
Moore’s Law has been the driving force behind the semiconductor in-dustry for several decades,but as silicon-based transistors approach their physical limits,researchers are searching for new materials to sustain thi...Moore’s Law has been the driving force behind the semiconductor in-dustry for several decades,but as silicon-based transistors approach their physical limits,researchers are searching for new materials to sustain this exponential growth.Two-dimensional transition metal dichalcogenides(TMDs),with their atomically thin structure and en-ticing physical properties,have emerged as the most promising can-didates for downsizing and improving device integration.Embold-ened by the direction of achieving large-area and high-quality TMDs growth,wafer-scale TMDs growth strategies have been continuously developed,suggesting that TMDs are poised to become a new plat-form for next-generation electronic devices.In this review,advanced synthesis routes and inherent properties of wafer-scale TMDs were critically assessed.In addition,the performance in electronic devices was also discussed,providing an outlook on the opportunities and challenges that lie ahead in their development.展开更多
The controllable synthesis of complicated nanostructures in advanced two-dimensional(2D)semiconductors,such as periodic regular hole arrays,is essential and remains immature.Here,we report a green,facile,highly contro...The controllable synthesis of complicated nanostructures in advanced two-dimensional(2D)semiconductors,such as periodic regular hole arrays,is essential and remains immature.Here,we report a green,facile,highly controlled synthetic method to efficiently pattern 2D semiconductors,such as periodic regular hexagonal-shaped hole arrays(HHA),in 2D-TMDs.Combining the production of artificial defect arrays through laser irradiation with anisotropic annealing etching,we created HHA with different arrangements,controlled hole sizes,and densities in bilayer WS_(2).Atomic force microscopy(AFM),Raman,photoluminescence(PL),and scanning transmission electron microscopy(STEM)characterization show that the 2D semiconductors have high quality with atomical clean and sharp edges as well as undamaged crystals in the unetched region.Furthermore,other nanostructures,such as nanoribbons and periodic regular triangular-shaped 2D-TMD arrays,can be fabricated.This kind of 2D semiconductors fabrication strategy is general and can be extended to a series of 2D materials.Density functional theory(DFT)calculations show that one WS_(2)molecule from the edges of the laser-irradiated holed region exhibits a robust etching activation,making selective etching at the artificial defects and the fabrication of regular 2D semiconductors possible.展开更多
基金supported by National Natural Science Foundation of China(NSFC,Grant No.51972178)Natural Science Foundation of Ningbo(2022J139)Ningbo Yongjiang Talent Introduction Programme(2022A-227-G)
文摘Crystallineγ-Ga_(2)O_(3)@rGO core-shell nanostructures are synthesized in gram scale,which are accomplished by a facile sonochemical strategy under ambient condition.They are composed of uniformγ-Ga_(2)O_(3)nanospheres encapsulated by reduced graphene oxide(rGO)nanolayers,and their formation is mainly attributed to the existed opposite zeta potential between the Ga_(2)O_(3)and rGO.The as-constructed lithium-ion batteries(LIBs)based on as-fabricatedγ-Ga_(2)O_(3)@rGO nanostructures deliver an initial discharge capacity of 1000 mAh g^(-1)at 100 mA g^(-1)and reversible capacity of 600 mAh g^(-1)under 500 mA g^(-1)after 1000 cycles,respectively,which are remarkably higher than those of pristineγ-Ga_(2)O_(3)with a much reduced lifetime of 100 cycles and much lower capacity.Ex situ XRD and XPS analyses demonstrate that the reversible LIBs storage is dominant by a conversion reaction and alloying mechanism,where the discharged product of liquid metal Ga exhibits self-healing ability,thus preventing the destroy of electrodes.Additionally,the rGO shell could act robustly as conductive network of the electrode for significantly improved conductivity,endowing the efficient Li storage behaviors.This work might provide some insight on mass production of advanced electrode materials under mild condition for energy storage and conversion applications.
基金the National Natural Science Foundation of China(NSFC,Grant No.51972178)the Natural Science Foundation of Ningbo(2022J139)the Ningbo Yongjiang Talent Introduction Programme(2022A-227-G).
文摘Two-dimensional(2D)oxides have been the focus of substantial research interest recently,owing to their fascinating physico-chemical properties.However,fabrication of large-area 2D oxide materials in a controlled manner under mild conditions still remains a formidable challenge.Herein,we develop a facile and universal strategy based on the sonochemistry approach for controllable and large-area growth of quasi-aligned single-crystalline ZnO nanosheets on a Zn substrate(Zn@SC-ZnO)under ambient conditions.The obtained ZnO nanosheets possess the desired exclusively exposed(001)facets,which have been confirmed to play a critical role in significantly reducing the activation energy and facilitating the stripping/plating processes of Zn.Accordingly,the constructed Zn@SC-ZnO||Zn@SC-ZnO symmetric cell has very low polarization overpotential down to~20 mV,with limited dendrite growth and side reactions for Zn anodes.The developed Zn@SC-ZnO//MnO_(2)aqueous Zn-ion batteries(ZIBs)show a voltage efficiency of 88.2%under 500 mA g^(-1)at the stage of 50%depth of discharge,which is state of the art for ZIBs reported to date.Furthermore,the as-assembled large-size cell(5 cm×5 cm)delivers an open circuit potential of 1.648 V,and can be robustly operated under a high current of 20 mA,showing excellent potential for future scalable applications.
基金Natural Science Foundation of Zhejiang Province,Grant/Award Number:LY23E020002National Natural Science Foundation of China,Grant/Award Number:52272085 and 51972178+1 种基金Natural Science Foundation of Ningbo,Grant/Award Number:2021J145China Postdoctoral Science Foundation,Grant/Award Number:2020M681966。
文摘Conversion of solar energy into H_(2) by photoelectrochemical(PEC)water splitting is recognized as an ideal way to address the growing energy crisis and environmental issues.In a typical PEC cell,the construction of photoanodes is crucial to guarantee the high efficiency and stability of PEC reactions,which fundamentally rely on rationally designed semiconductors(as the active materials)and substrates(as the current collectors).In this review work,we start with a brief introduction of the roles of substrates in the PEC process.Then,we provide a systematic overview of representative strategies for the controlled fabrication of photoanodes on rationally designed substrates,including conductive glass,metal,sapphire,silicon,silicon carbide,and flexible substrates.Finally,some prospects concerning the challenges and research directions in this area are proposed.
基金National Natural Science Foundation of China,Grant/Award Numbers:51972178,52202061Hunan Provincial Nature Science Foundation,Grant/Award Number:2022JJ40068。
文摘Currently,the major challenge in terms of research on K-ion batteries is to ensure that they possess satisfactory cycle stability and specific capacity,especially in terms of the intrinsically sluggish kinetics induced by the large radius of K+ions.Here,we explore high-performance K-ion half/full batteries with high rate capability,high specific capacity,and extremely durable cycle stability based on carbon nanosheets with tailored N dopants,which can alleviate the change of volume,increase electronic conductivity,and enhance the K+ion adsorption.The as-assembled K-ion half-batteries show an excellent rate capability of 468 mA h g^(−1) at 100 mA g^(−1),which is superior to those of most carbon materials reported to date.Moreover,the as-assembled half-cells have an outstanding life span,running 40,000 cycles over 8 months with a specific capacity retention of 100%at a high current density of 2000 mA g^(−1),and the target full cells deliver a high reversible specific capacity of 146 mA h g^(−1) after 2000 cycles over 2 months,with a specific capacity retention of 113%at a high current density of 500 mA g^(−1),both of which are state of the art in the field of K-ion batteries.This study might provide some insights into and potential avenues for exploration of advanced K-ion batteries with durable stability for practical applications.
基金supported by the National Natural Science Foundation of China (22278231,22005165 and 22376110)the Natural Science Foundation Project of Shandong Province (ZR2022MB092 and ZR2023ME098)the Taishan Scholar Program (ts201712030)。
文摘Manganese-based oxide electrode materials suffer from severe Jahn-Teller(J-T)distortion,leading to severe cycle instability in sodium ion storage.However,it is difficult to adjust the electron at d orbitals exactly to a low spin state to eliminate orbital degeneracy and suppress J-T distortion fundamentally.This article constructed concentration-controllable Mn/O coupled vacancy and amorphous network in Mn_(3)O_(4) and coated it with nitrogen-doped carbon aerogel(Mn_(3-x)O_(4-y)@NCA).The existence of Mn/O vacancies has been confirmed by scanning transmission electron microscopy(STEM)and positron annihilation lifetime spectroscopy(PALS).Atomic absorption spectroscopy(AAS)and X-ray photoelectron spectroscopy(XPS)determine the most optimal ratio of Mn/O vacancies for sodium ion storage is 1:2.Density functional theory(DFT)calculations prove that Mn/O coupled vacancies with the ratio of 1:2could exactly induce a low spin states and a d~4 electron configuration of Mn,suppressing the J-T distortion successfully.The abundant amorphous regions can shorten the transport distance of sodium ions,increase the electrochemically active sites and improve the pseudocapacitance response.From the synergetic effect of Mn/O coupled vacancies and amorphous regions,Mn_(3-x)O_(4-y)@NCA exhibits an energy density of 37.5 W h kg^(-1)and an ultra-high power density of 563 W kg^(-1)in an asymmetric supercapacitor.In sodium-ion batteries,it demonstrates high reversible capacity and exceptional cycling stability.This research presents a new method to improve the Na^(+)storage performance in manganese-based oxide,which is expected to be generalized to other structural distortion.
基金financially funded by the Natural Science Foundation of Ningbo(No.2022J139)the Ningbo Yongjiang Talent Introduction Programme(No.2022A-227-G)+5 种基金the National Natural Science Foundation of China(No.51972178)the financial support from Scientific and Technological Bases and Talents of Guangxi(Guike AD21075051)the National Natural Science Foundation of China(12174075)the special fund for“Guangxi Bagui Scholars”support by ERC-CZ program(project LL2101)from the Ministry of Education Youth and Sports(MEYS)by the project Advanced Functional Nanorobots(reg.No.CZ.02.1.01/0.0/0.0/15_003/0000444 financed by the EFRR)
文摘Anion exchange membrane fuel cell(AEMFC)technology is attracting intensive attention,due to its great potential by using non-precious-metal catalysts(NPMCs)in the cathode and cheap bipolar plate materials in alkaline media.However,in such case,the kinetics of hydrogen oxidation reaction(HOR)in the anode is two orders of magnitude sluggish than that of acidic electrolytes,which is recognized as the grand challenge in this field.Herein,we report the rationally designed Ni nanoparticles encapsulated by N-doped graphene layers(Ni@NG)using a facile pyrolysis strategy.Based on the density functional theory calculations and electrochemical performance analysis,it is witnessed that the rich Pyridinic-N within the graphene shell optimizes the binding energy of the intermediates,thus enabling the fundamentally enhanced activity for HOR with robust stability.As a proof of concept,the resultant Ni@NG sample as the anode with a low loading(1.8 mg cm^(-2))in AEMFCs delivers a high peak power density of 500 mW cm^(-2),outperforming all of those of NPMC-based analogs ever reported.
基金supported by the project funded by the National Natural Science Foundation of China (52172222, 5197226 and 51972178)the China Postdoctoral Science Foundation(2020 M681966)+1 种基金the exchange project of the sixth ChinaNorthern Macedonia Science and Technology Meeting (6-11)the Natural Science Foundation of Ningbo Municipal Government(202003 N4164 and 2021J145)。
文摘The sluggish kinetics for water oxidation is recognized as one of the major problems for the unsatisfied photoelectrochemical(PEC) performance. Herein, we developed a feasible strategy based on in-situ selective surface cation exchange, for activating surface water oxidation reactivity toward boosted PEC water oxidation of BiVO_(4) photoanodes with fundamentally improved surface charge transfer. The asconstructed Co/BiVO_(4) photoanodes exhibit 2.6 times increase in photocurrent density with superior stability, in comparison to those of pristine counterpart. Moreover, the faradaic efficiency of as-fabricated photoanode can be up to ~ 95% at 1.23 V(vs. RHE). The unique selective replacement of Bi by Co on the surface could modify the electronic structure of BiVO_(4) with reduced energy barrier of the deprotonation of OH^(+) to O, thus favoring the overall excellent PEC performance of Co/BiVO_(4) photoanode.
基金Hunan Provincial Innovation Foundation for Postgraduate,Grant/Award Number:CX20200454National Natural Science Foundation of China,Grant/Award Number:51972178。
文摘We report the scalable fabrication of CdS/ZnS 1D/2D heterojunctions under ambient air conditions(i.e.,room temperature and atmospheric pressure)in which ZnS nanoparticles are anchored on the surface of CdS nanosheets.The as-formed heterojunctions exhibit a significantly enhanced photocatalytic H_(2) evolution rate of 14.02 mmol h^(-1) g^(-1) when irradiated with visible light,which is~10 and 85 times higher than those of pristine CdS nanosheets and CdS nanoparticles,respectively,and superior to most of the CdS-based photocatalysts reported to date.Furthermore,they provide robust photocatalytic performance with demonstratable stability over 58 h,indicating their potential for practical applications.The formation of 1D/2D heterojunctions not only provides improved exposed active sites that respond to illumination but also provides a rapid pathway to generate photogenerated carriers for efficient separation and transfer through the matrix of single-crystalline CdS nanosheets.In addition,first-principles simulations demonstrate that the existence of rich Zn vacancies increases the energy level of the ZnS valence band maximum to construct type-II and Z-scheme mixed heterojunctions,which plays a critical role in suppressing the recombination of carriers with limited photocorrosion of CdS to enhance photocatalytic behavior.
基金Top Talent Project of Ningbo Municipal Government,National Natural Science Foundation of China(No.51972178)。
文摘Currently,the synthesis of nanostructures still encounters two grand challenges:one is the often-required high temperatures and/or high pressures,and the other is the scalable fabrication.Here,to break through such bottlenecks,we demonstrate an ambient-condition strategy for rapid mass production of fourthgeneration semiconductor Ga_(2)O_(3)nanoarchitectures assembled by single-crystalline nanosheets in a controlled manner based on sonochemistry.Their growth is fundamentally determined by the introduced ethanediamine in rationally designed source materials,which could not only protect the metal Ga against reacting with H_(2)O into GaOOH,but facilitate the reaction of Ga with OH·radicals for target crystalline Ga_(2)O_(3)nanostructures.As a proof of concept for applications,the as-fabricated Ga_(2)O_(3)nanoarchitectures exhibit superb performances for electromagnetic wave absorption with a reflection loss value of 52.2 dB at 8.1 GHz,and ammonia sensing with high sensitivity and selectivity at room temperature,representing their bright future to be commercially applied in modern devices.
基金This work was supported by the National Natural Science Foundation of China(Grant No.51972178)Hunan Provincial Innovation Foundation for Postgraduate(Grant No.CX20200454).
文摘To date,the synthesis of crystalline ZnO nanostructures was often performed under high temperatures and/or high pressures with tiny output,which limits their commercial applications.Herein,we report the progress on synthesizing single-crystalline ZnO nanosheets under ambient conditions(i.e.,room temperature(RT)and atmospheric pressure)based on a sonochemistry strategy.Furthermore,their controllable growth is accomplished by adjusting the pH values of solutions,enabling the tailored crystal growth habits on the polar-charged faces of ZnO along c-axis.As a proof of concept for their potential applications,the ZnO nanosheets exhibit highly efficient performance for sensing ammonia at RT,with ultrahigh sensitivity(S=610 at 100 ppm),excellent selectivity,rapid detection(response time/recover time=70 s/4 s),and outstanding detection limit down to 0.5 ppm,superior to those of all pure ZnO nanostructures and most ZnO-based composite counterparts ever reported.The present work might open a door for controllable production of ZnO nanostructures under mild conditions,and facilitate the exploration of modern gas sensors for detecting gaseous molecules at RT,which underscores their potential toward practical applications in opto-electronic nanodevices.
基金supported by the National Natural Science Foundation of China(U19A2018)the Natural Science Foundation of Hunan Province(2021JJ30651)the Postgraduate Scientific Research Innovation Project of Hunan Province(CX20230643).
文摘Single-crystalline Ni-rich cathodes can provide high energy density and capacity retention rates for lithium-ion batteries(LIBs).However,single-crystalline Ni-rich cathodes experience severe transition metal dissolution,irreversible phase transitions,and reduced structural stability during prolonged cycling at high voltage,which will significantly hinder their practical application.Herein,a Li4TeO5surface coating along with bulk Te-gradient doping strategy is proposed and developed to solve these issues for single-crystalline Ni-rich LiNi_(0.90)Co_(0.05)Mn_(0.05)O_(2)cathode(LTeO-1.0).It has been found that the bulk Te^(6+)gradient doping can lead to the formation of robust Te-O bonds that effectively inhibit H_(2)-H3 phase transformations and reinforce the lattice framework,and the in-situ Li4TeO5coating layer can act as a protective layer that suppresses the parasitic reactions and grain fragmentation.Besides,the modified material exhibits a higher Young's modulus,which will be conducive to maintaining significant structural and electrochemical stability under high-voltage conditions,Especially,the LTeO-1.0 electrode shows the improved Li^(+)diffusion kinetics and thermodynamic stability as well as high capacity retention of 95.83%and 82.12%after 200 cycles at the cut-off voltage of 4.3 and 4,5 V.Therefore,the efficacious dualmodification strategy will definitely contribute to enhancing the structural and electrochemical stability of single-crystalline Ni-rich cathodes and developing their application in LIBs.
文摘Engineering the morphology of the support is effective in tuning the redox properties of active metals for efficient catalytic methane combustion via tailoring the metal-support interaction.Herein,uniform Ir nanoparticles supported on anatase TiO_(2)with different morphologies predominantly exposing{100},{101},and{001}planes were synthesized and tested for methane combustion.The CH_(4) catalytic activity shows a remarkable TiO_(2)-facet-dependent effect and follows the order of Ir/TiO_(2)-{100}>Ir/TiO_(2)-{101}>>Ir/TiO_(2)-{001}.Detailed characterizations and DFT calculations reveal that compared with Ir-TiO_(2)-{101}and Ir-TiO_(2)-{001}interfaces,the superior Ir-TiO_(2)-{100}interface facilitates the generation of electron-rich Ir species through more profound charge transfer from TiO_(2)-{100}to Ir atoms.The electron-rich Ir structure,featuring abundant defect oxygen vacancies,significantly enhances the redox properties of active Ir species and reduces the activation energy for breaking the initial C-H bond in CH_(4),resulting in the superior catalytic activity for methane combustion.These findings deepen fundamental insights into the TiO_(2)-facet-dependent reactivity of different Ir/TiO_(2)nanomaterials in methane oxidation and pave the way for designing efficient Ir-based methane oxidation catalysts.
基金supported by the National Natural Science Fund for Distinguished Young Scholars(No.52025041)supported by the National Natural Sci-ence Foundation of China(Nos.51702176 and 51974021)+1 种基金Zhejiang Provincial Nature Science Foundation(No.LY20E020009)the Interdisciplinary Research Project for Young Teachers of USTB(Fun-damental Research Funds for the Central Universities,No.FRF-IDRY-21-028).
文摘One key step for advancing the widespread practical application of rechargeable metal-air batteries and water electrolysis fundamentally relies on the development of cost-effective multifunctional electrocata-lysts toward oxygen and hydrogen-involving reactions.The present work initiates a tofu-derived one-pot strategy for green,facile,and mass production of highly active and stable catalyst toward oxygen reduc-tion/evolution and hydrogen evolution reactions,through the preparation of Fe/Co cross-linked tofu gel and the subsequent pyrolysis.Despite the free use of additional N/P precursors or pore-forming agents,the as-prepared materials comprise highly dispersive FeCo-rich phosphides nanoparticles and porous N,P co-doped carbon network inherited from the tofu skeleton.The resultant catalysts exhibit remarkably enhanced trifunctional activities as compared to the Fe_(2)P and Co_(2)P counterparts,along with better long-term stabilities than the benchmark RuO_(2)and Pt/C catalysts.Accordingly,the as-assembled Zn-air battery delivers a large power density(174 mW cm^(-2))with excellent cycle stability(the gap of charge/discharge voltage@10 mA cm^(-2)increases by 0.01 V after 720 h of operation,vs.0.16 V of Pt/C-RuO_(2)based battery after 378 h).Furthermore,the as-constructed alkaline electrolyzer just requires a small voltage of 1.55 V@10 mA cm^(-2),which outperforms nearly all of those of biomass-derived electrocatalysts ever reported,and that of noble metal catalysts-based electrolyzers(1.72 V@10 mA cm^(-2)for Pt/C-RuO_(2)),underscoring their bright future toward commercial applications in green energy conversion devices.
基金the National Natural Science Foundation of China(Nos.52302272 and 22376110)the Taishan Scholars Program(No.tsqn202211124)+2 种基金the Natural Science Foundation of Shandong Province(No.ZR2022QB023)the Qingchuang Talents Induction Program of Shandong Higher Education Institution(Research and Innovation Team of Marine Polysaccharides Fibers-based Energy Materials)the State Key Laboratory of Bio-Fibers and Eco-Textiles,Qingdao University(Nos.ZKT10,GZRC202006,ZFZ201809,and ZDKT202105).
文摘Rationally constructed new catalyst can promote carbon dioxide reduction reaction(CO_(2)RR)to valuable carbo-naceous fuels such as formate and CO,providing a promising strategy for low CO_(2)emissions.Herein,the syn-thesized Ni_(3)S_(2)@C as a highly efficient electro-catalyst exhibits remarkable selectivity for formate with 73.9%faradaic efficiency(FE)at-0.7 V vs.RHE.At high applied potential,it shows a high syngas evolution with CO/H_(2)ratios(0.54-3.15)that are suitable for typical downstream thermochemical reactions.The experimental and theoretical analyses demonstrate that the electron-rich Ni^(2+)in Ni_(3)S_(2)enhances the adsorption behavior of*OCHO intermediate,reduces the energy barrier of the formation of intermediates,and improves the selectivity of the formate product.Attenuated total reflection surface-enhanced infrared absorption spectra conducted in situ show that*OCHO intermediate is more likely to be generated and adsorbed on Ni_(3)S_(2),enhancing the selectivity and activity of the formate product.
基金supported by the National Natural Science Foundation of China(grant nos.52074113,22005091,and 22005092)the Hunan University Outstanding Youth Science Foundation(grant no.531118040319).
文摘High areal capacity is one of the critically important points for potassium-ion batteries(PIBs)for practical applications,which relies on high areal-massloading electrodes operating at high reversible capacity.However,it is remarkably restricted by the mechanical instability and sluggish charge transfer induced by the increased mass loading.To overcome such challenge,we report the rationally designed bimetallic selenides CoSe2/SnSe2 heterostructures confined in hierarchical carbon nanofibers(CSSe@CNFs),which enables the electrodes robust mechanical stability,enhanced electron transport,and reduced ion-diffusion energy barrier for facilitating reaction kinetics.Accordingly,an impressive areal mass loading up to 25.3 mg cm^(−2)was achieved,which endowed a high areal capacity of 7.58 mAh cm^(−2)for such a free-standing electrode.This is stateof-the-art among the PIBs,exceeding that of today’s industry standard(∼3 mAh cm^(−2)for LIBs).Furthermore,it delivered long-term stability over 3700 cycles at high current density(∼2 mA cm^(−2),vs 1 mA cm^(−2)in LIBs).Moreover,the as-constructed full battery achieved a high energy density of 172.8 Wh kg-1 at 0.05 A g^(−1)with a satisfied cycle stability over 2000 cycles at 2 A g^(−1)and high reversibility with Coulombic efficiency of 100%;thus,signifying its bright future toward commercial application for advanced PIBs.
基金supported by Hunan Provincial Natural Science Foundation of China (grant No.2022JJ20085)Changsha Natural Science Foundation (grant No.kq2202092).
文摘Moore’s Law has been the driving force behind the semiconductor in-dustry for several decades,but as silicon-based transistors approach their physical limits,researchers are searching for new materials to sustain this exponential growth.Two-dimensional transition metal dichalcogenides(TMDs),with their atomically thin structure and en-ticing physical properties,have emerged as the most promising can-didates for downsizing and improving device integration.Embold-ened by the direction of achieving large-area and high-quality TMDs growth,wafer-scale TMDs growth strategies have been continuously developed,suggesting that TMDs are poised to become a new plat-form for next-generation electronic devices.In this review,advanced synthesis routes and inherent properties of wafer-scale TMDs were critically assessed.In addition,the performance in electronic devices was also discussed,providing an outlook on the opportunities and challenges that lie ahead in their development.
基金National Key R&D Program of the Ministry of Science and Technology of China,Grant/Award Number:2022YFA1203801The National Natural Science Foundation of China,Grant/Award Numbers:51991340,51991343,52221001,62174051+1 种基金The Hunan Key R&D Program Project,Grant/Award Number:2022GK2005Ningbo Natural Science Foundation,Grant/Award Number:2023J023。
文摘The controllable synthesis of complicated nanostructures in advanced two-dimensional(2D)semiconductors,such as periodic regular hole arrays,is essential and remains immature.Here,we report a green,facile,highly controlled synthetic method to efficiently pattern 2D semiconductors,such as periodic regular hexagonal-shaped hole arrays(HHA),in 2D-TMDs.Combining the production of artificial defect arrays through laser irradiation with anisotropic annealing etching,we created HHA with different arrangements,controlled hole sizes,and densities in bilayer WS_(2).Atomic force microscopy(AFM),Raman,photoluminescence(PL),and scanning transmission electron microscopy(STEM)characterization show that the 2D semiconductors have high quality with atomical clean and sharp edges as well as undamaged crystals in the unetched region.Furthermore,other nanostructures,such as nanoribbons and periodic regular triangular-shaped 2D-TMD arrays,can be fabricated.This kind of 2D semiconductors fabrication strategy is general and can be extended to a series of 2D materials.Density functional theory(DFT)calculations show that one WS_(2)molecule from the edges of the laser-irradiated holed region exhibits a robust etching activation,making selective etching at the artificial defects and the fabrication of regular 2D semiconductors possible.
