The Haber-Bosch process for industrial NH_(3) production is energy-intensive with heavy CO_(2) emissions.Electrochemical N_(2) reduction reaction(NRR)is an attractive carbon-neutral alternative for NH_(3) synthesis,wh...The Haber-Bosch process for industrial NH_(3) production is energy-intensive with heavy CO_(2) emissions.Electrochemical N_(2) reduction reaction(NRR)is an attractive carbon-neutral alternative for NH_(3) synthesis,while the challenge associated with N_(2) activation highlights the demand for efficient electrocatalysts.Herein,we demonstrate that PdCu nanoparticles with different Pd/Cu ratios anchored on boron nanosheet(PdCu/B)behave as efficient NRR electrocatalysts toward NH_(3) synthesis.Theoretical and experimental results confirm that the highly efficient NH_(3) synthesis can be achieved by regulating the charge transfer between interfaces and forming a symmetry-breaking site,which not only alleviates the hydrogen evolution but also changes the adsorption configuration of N_(2) and thus optimizes the reaction pathway of NRR over the separated Pd sites.Compared with monometallic Pd/B and Cu/B,the PdCu/B with the optimized Pd/Cu ratio of 1 exhibits superior activity and selectivity for NH_(3) synthesis.This study provides new insight into developing efficient catalysts for small energy molecule catalytic conversion via regulating the charge transfer between interfaces and constructing symmetry-breaking sites.展开更多
Triboelectricity,when rubbing or contacting materials causes electric charge transfer,is ubiquitous across many fields,and has been studied in detail for centuries.Despite this,a complete description of triboelectrici...Triboelectricity,when rubbing or contacting materials causes electric charge transfer,is ubiquitous across many fields,and has been studied in detail for centuries.Despite this,a complete description of triboelectricity remains elusive.Here,we analyze the contact between a metal asperity and a semiconductor,including contributions from the depletion zone of the semiconductor and from flexoelectric polarization that arises due to the strain gradients at asperity contacts.The free charges involved in charge transfer are then discussed and calculated.As a result,we develop a quantitative model for triboelectric charge transfer that details how charge transfer scales with contact parameters,the relative influence of depletion and flexoelectricity,and which agrees with various trends in multiple classes of triboelectric experiments.展开更多
The dark oxidation reactions of ethers including aether, isopropyl ether, phenyl isopropyl ether, and benzyl isopropyl ether have been studied by using density functional theory calculations. The structures of initial...The dark oxidation reactions of ethers including aether, isopropyl ether, phenyl isopropyl ether, and benzyl isopropyl ether have been studied by using density functional theory calculations. The structures of initial Contact charge transfer complexes （CCTCs）, transition states and caged radical intermediates have been located at the B3LYP/6-31G （d） level, The bonding nature of ethers with triplet 02 in CCTCs has been analyzed, and the detailed mechanism of dark oxidation reactions of ether is presented clearly.展开更多
We theoretically investigate the excited state intramolecular proton transfer(ESIPT) behavior of the novel fluorophore bis-imine derivative molecule HNP which was designed based on the intersection of 1-(hydrazonometh...We theoretically investigate the excited state intramolecular proton transfer(ESIPT) behavior of the novel fluorophore bis-imine derivative molecule HNP which was designed based on the intersection of 1-(hydrazonomethyl)-naphthalene-2-ol and 1-pyrenecarboxaldehyde. Especially, the density functional theory(DFT) and time-dependent density functional theory(TDDFT) methods for HNP monomer are introduced. Moreover, the "our own n-layered integrated molecular orbital and molecular mechanics"(ONIOM) method(TDDFT:universal force field(UFF)) is used to reveal the aggregation-induced emission(AIE) effect on the ESIPT process for HNP in crystal. Our results confirm that the ESIPT process happens upon the photoexcitation for the HNP monomer and HNP in crystal, which is distinctly monitored by the optimized geometric structures and the potential energy curves. In addition, the results of potential energy curves reveal that the ESIPT process in HNP will be promoted by the AIE effect. Furthermore, the highest occupied molecular orbital(HOMO) and lowest unoccupied molecular orbital(LUMO) for the HNP monomer and HNP in crystal have been calculated. The calculation demonstrates that the electron density decrease of proton donor caused by excitation promotes the ESIPT process. In addition, we find that the variation of atomic dipole moment corrected Hirshfeld population(ADCH) charge for proton acceptor induced by the AIE effect facilitates the ESIPT process. The results will be expected to deepen the understanding of ESIPT dynamics for luminophore under the AIE effect and provide insight into future design of high-efficient AIE compounds.展开更多
Constructing a S-scheme heterojunction with tight interface contact and fast charge transfer is beneficial to improving the photocatalytic hydrogen evolution performance.Herein,a unique one-dimensional(1D)/two-dimensi...Constructing a S-scheme heterojunction with tight interface contact and fast charge transfer is beneficial to improving the photocatalytic hydrogen evolution performance.Herein,a unique one-dimensional(1D)/two-dimensional(2D)S-scheme heterojunction containing 1D Sb_(2)S_(3) nanorods and 2D ZnIn_(2)S_(4) with affluent sulfur vacancies(denoted as Sv-ZnIn_(2)S_(4)@Sb_(2)S_(3)) was designed.The introduced sulfur vacancy can promote the effective adsorption of H+for the following interfacial hydrogen-evolution reaction.Furthermore,the larger contact area and stronger electron interaction between Sb_(2)S_(3) and ZnIn_(2)S_(4) effectively inhibits the recombination of photo-generated electron–hole pairs and abridges the migration distance of charges.As a result,the optimal Sv-ZnIn_(2)S_(4)@Sb_(2)S_(3) sample achieves H_(2) evolution activity of 2741.3 mol·h^(−1)·g^(−1),which is 8.6 times that of pristine ZnIn_(2)S_(4) and 3.0 times that of the Sv-ZnIn_(2)S_(4) samples.Based on the experimental result,the photo-reactivity S-scheme mechanism of hydrogen evolution from water splitting with Sv-ZnIn_(2)S_(4)@Sb_(2)S_(3) is proposed.This work provides an effective method for developing S-scheme heterojunction composites of transition metal sulfide with high hydrogen evolution performance.展开更多
Photoelectrocatalytic seawater splitting is a promising low-cost method to produce green hydrogen in a large scale.The effects of Cl^(-)ions in seawater on the performance of a photoanode have been reported in previou...Photoelectrocatalytic seawater splitting is a promising low-cost method to produce green hydrogen in a large scale.The effects of Cl^(-)ions in seawater on the performance of a photoanode have been reported in previous studies.However,few researches have been done on the roles of Cl^(-)ions in a photocathode.Herein,for the first time,we find that Cl^(-)ions in the electrolyte improve the photocurrent of a Si/In_(2)S_(3) photocathode by 50% at-0.6 V_(RHE).An in-situ X-ray photoelectron spectroscopy(XPS)characterization combined with the time-of-flight secondary-ion mass spectrometry by simulating photoelectrochemical conditions was used to investigate the interface charge transfer mechanism.The results suggest that there is an In_(2)^(+3)S_(3-x)(OH)_(2x)layer on the surface of In_(2)S_(3) in the phosphate buffer solution(PBS)electrolyte,which plays a role as an interface charge transfer mediator in the Si/In_(2)S_(3) photocathode.The In_(2)^(+3)S_(3-x)(OH)_(2x)surface layer becomes In_(2)^(+3)S_(3-x)(Cl)_(2x)in the PBS electrolyte with NaCl and accelerates the charge transfer rate at the In_(2)S_(3)/electrolyte interface.These results offer a new concept of regulating interface charge transfer mediator to enhance the performance of photoelectrocatalytic seawater splitting for hydrogen production.展开更多
A novel benzene-ring engineered 1D/2D WO_(3)/g-C_(3)N_(4)S-scheme photocatalyst(BCNW)was rationally de-signed and successfully synthesized by the electrostatic self-assembly method.Experimental and Density Functional ...A novel benzene-ring engineered 1D/2D WO_(3)/g-C_(3)N_(4)S-scheme photocatalyst(BCNW)was rationally de-signed and successfully synthesized by the electrostatic self-assembly method.Experimental and Density Functional Theory results reveal that the integration of molecular benzene-ring in the framework of g-C_(3)N_(4)can not only narrow its bandgap and accelerate charge separation by forming a mid-state at the top of its valence band but more importantly open up a new additional bridge for speeding up the interfacial S-scheme charge transfer in BCNW.Benefitting from those multiple positive effects of benzene-ring inte-gration,as expected,BCNW S-scheme photocatalysts show superior photocatalytic H_(2)-production activity and reach 2971μmol h^(-1)g^(-1)under visible-light illumination,which is 3.35 times WO_(3)/g-C_(3)N_(4)S-scheme photocatalyst without benzene-ring integration.This work supplies an innovative strategy for the design of a high-efficiency S-scheme photocatalytic system by constructing a facile and additional molecular charge transfer channel at the interface.展开更多
Galvanic replacement, one of the popular strategies for producing hollow metallic nanostructures, has enjoyed great success in the past. However, it is rarely used with Au nanopartides as the self-sacrificed templates...Galvanic replacement, one of the popular strategies for producing hollow metallic nanostructures, has enjoyed great success in the past. However, it is rarely used with Au nanopartides as the self-sacrificed templates, even though these nanoparticles can be produced with well-controlled size, shape, and structure. Here, both Ag and Au from the core-sheU Au@Ag nanorods are demonstrated to be involved in the galvanic replacement for producing hollow nanostructures. The enhanced oxidation of metallic Au could be attributed to the close contact between Au and Ag and the unique charge compensation from Au to Ag, both of which are indispensable for the etching of Au via galvanic replacement. As a result of this reaction, these bimetallic nanorods experience a structural evolution from nanorattles, to tip-empty nanorods, and eventually to porous nanotubes. The nanotubes exhibit high catalytic activities in the electrooxidation of formic acid. These results not only disclose the underlying mechanism by which metallic Au could be replaced under mild conditions, but also expand the selection of self-sacrificed templates for galvanic replacement, which is an important reaction in many applications.展开更多
Surface enhanced Raman scattering(SERS)is a fingerprint spectral technique whose performance is highly dependent on the physicochemical properties of the substrate materials.In addition to the traditional plasmonic me...Surface enhanced Raman scattering(SERS)is a fingerprint spectral technique whose performance is highly dependent on the physicochemical properties of the substrate materials.In addition to the traditional plasmonic metal substrates that feature prominent electromagnetic enhancements,boosted SERS activities have been reported recently for various categories of non-metal materials,including graphene,MXenes,transition-metal chalcogens/oxides,and conjugated organic molecules.Although the structural compositions of these semiconducting substrates vary,chemical enhancements induced by interfacial charge transfer are often the major contributors to the overall SERS behavior,which is distinct from that of the traditional SERS based on plasmonic metals.Regarding charge-transfer-induced SERS enhancements,this short review introduces the basic concepts underlying the SERS enhancements,the most recent semiconducting substrates that use novel manipulation strategies,and the extended applications of these versatile substrates.展开更多
The NO gas is easily oxidized to form toxic by-products(NO_(2))during the oxidation process,which are adsorbed on the catalyst surface and inhibit the subsequent reaction.For photocatalytic NO removal,a significant ch...The NO gas is easily oxidized to form toxic by-products(NO_(2))during the oxidation process,which are adsorbed on the catalyst surface and inhibit the subsequent reaction.For photocatalytic NO removal,a significant challenge is to achieve catalytic stability while maintaining high conversion efficiency.Here,we fabricated a(BiO)_(2)CO_(3)/β-Bi_(2)O_(3)heterostructure that enables efficient charge transfer and promotes the NO removal.We propose that the catalytic stability depends on the heterojunction structure,which is able to generate interfacial charge transfer channels.In addition,we further introduce graphene quantum dots on the heterojunction structure,which further strengthens the interfacial charge transfer dynamics and finally realizes that the NO_(2)byproduct could gain electrons and convert to the final product(nitrite or nitrate).This composite structure not only exhibits high activity for NO removal but also maintains long-term stability under visible light.展开更多
We investigate nanorod assemblies of two 64-substituted pentacenes, namely （2,3-X2-9,10-Y2）-substituted pentacenes with X -- Y = OCH3 （MOP） and with X = F, Y-- OCH3 （MOPF）, grown on Au（111） single crystals. By...We investigate nanorod assemblies of two 64-substituted pentacenes, namely （2,3-X2-9,10-Y2）-substituted pentacenes with X -- Y = OCH3 （MOP） and with X = F, Y-- OCH3 （MOPF）, grown on Au（111） single crystals. By using a multi-technique approach based on ultraviolet photoelectron spectroscopy X-ray photoelectron spectroscopy; and X-ray absorption, we find evidence for charge transfer screening at the interface with gold. Furthermore, the MOP and MOPF nanorods show a rough surface morphology, which was investigated with atomic force microscopy. We use molecular simulation techniques to investigate the energetic barriers to diffusion and to traverse step-edges to estimate their influence on the nanorod roughness. We find that barriers to surface diffusion on a terrace are anisotropic and that their direction favors the formation of nanorods in these materials.展开更多
基金National Key R&D Program of China,Grant/Award Number:2020YFA0710000National Natural Science Foundation of China,Grant/Award Numbers:22008170,21978200,22161142002,22121004。
文摘The Haber-Bosch process for industrial NH_(3) production is energy-intensive with heavy CO_(2) emissions.Electrochemical N_(2) reduction reaction(NRR)is an attractive carbon-neutral alternative for NH_(3) synthesis,while the challenge associated with N_(2) activation highlights the demand for efficient electrocatalysts.Herein,we demonstrate that PdCu nanoparticles with different Pd/Cu ratios anchored on boron nanosheet(PdCu/B)behave as efficient NRR electrocatalysts toward NH_(3) synthesis.Theoretical and experimental results confirm that the highly efficient NH_(3) synthesis can be achieved by regulating the charge transfer between interfaces and forming a symmetry-breaking site,which not only alleviates the hydrogen evolution but also changes the adsorption configuration of N_(2) and thus optimizes the reaction pathway of NRR over the separated Pd sites.Compared with monometallic Pd/B and Cu/B,the PdCu/B with the optimized Pd/Cu ratio of 1 exhibits superior activity and selectivity for NH_(3) synthesis.This study provides new insight into developing efficient catalysts for small energy molecule catalytic conversion via regulating the charge transfer between interfaces and constructing symmetry-breaking sites.
基金supported by the Northwestern University McCormick School of Engineering,USA.
文摘Triboelectricity,when rubbing or contacting materials causes electric charge transfer,is ubiquitous across many fields,and has been studied in detail for centuries.Despite this,a complete description of triboelectricity remains elusive.Here,we analyze the contact between a metal asperity and a semiconductor,including contributions from the depletion zone of the semiconductor and from flexoelectric polarization that arises due to the strain gradients at asperity contacts.The free charges involved in charge transfer are then discussed and calculated.As a result,we develop a quantitative model for triboelectric charge transfer that details how charge transfer scales with contact parameters,the relative influence of depletion and flexoelectricity,and which agrees with various trends in multiple classes of triboelectric experiments.
基金Project supported by the National Natural Science Foundation of China (No. 20473047) and the Major State Basic Research Development Program of China (973 Program, No. 2004CB719902)
文摘The dark oxidation reactions of ethers including aether, isopropyl ether, phenyl isopropyl ether, and benzyl isopropyl ether have been studied by using density functional theory calculations. The structures of initial Contact charge transfer complexes （CCTCs）, transition states and caged radical intermediates have been located at the B3LYP/6-31G （d） level, The bonding nature of ethers with triplet 02 in CCTCs has been analyzed, and the detailed mechanism of dark oxidation reactions of ether is presented clearly.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11574115 and 11704146)
文摘We theoretically investigate the excited state intramolecular proton transfer(ESIPT) behavior of the novel fluorophore bis-imine derivative molecule HNP which was designed based on the intersection of 1-(hydrazonomethyl)-naphthalene-2-ol and 1-pyrenecarboxaldehyde. Especially, the density functional theory(DFT) and time-dependent density functional theory(TDDFT) methods for HNP monomer are introduced. Moreover, the "our own n-layered integrated molecular orbital and molecular mechanics"(ONIOM) method(TDDFT:universal force field(UFF)) is used to reveal the aggregation-induced emission(AIE) effect on the ESIPT process for HNP in crystal. Our results confirm that the ESIPT process happens upon the photoexcitation for the HNP monomer and HNP in crystal, which is distinctly monitored by the optimized geometric structures and the potential energy curves. In addition, the results of potential energy curves reveal that the ESIPT process in HNP will be promoted by the AIE effect. Furthermore, the highest occupied molecular orbital(HOMO) and lowest unoccupied molecular orbital(LUMO) for the HNP monomer and HNP in crystal have been calculated. The calculation demonstrates that the electron density decrease of proton donor caused by excitation promotes the ESIPT process. In addition, we find that the variation of atomic dipole moment corrected Hirshfeld population(ADCH) charge for proton acceptor induced by the AIE effect facilitates the ESIPT process. The results will be expected to deepen the understanding of ESIPT dynamics for luminophore under the AIE effect and provide insight into future design of high-efficient AIE compounds.
基金This study was financially supported by the National Natural Science Foundation of China(Nos.12075174 and 91963207)the National Key Research and Development Program of China(No.2022YFA1602701).
文摘Constructing a S-scheme heterojunction with tight interface contact and fast charge transfer is beneficial to improving the photocatalytic hydrogen evolution performance.Herein,a unique one-dimensional(1D)/two-dimensional(2D)S-scheme heterojunction containing 1D Sb_(2)S_(3) nanorods and 2D ZnIn_(2)S_(4) with affluent sulfur vacancies(denoted as Sv-ZnIn_(2)S_(4)@Sb_(2)S_(3)) was designed.The introduced sulfur vacancy can promote the effective adsorption of H+for the following interfacial hydrogen-evolution reaction.Furthermore,the larger contact area and stronger electron interaction between Sb_(2)S_(3) and ZnIn_(2)S_(4) effectively inhibits the recombination of photo-generated electron–hole pairs and abridges the migration distance of charges.As a result,the optimal Sv-ZnIn_(2)S_(4)@Sb_(2)S_(3) sample achieves H_(2) evolution activity of 2741.3 mol·h^(−1)·g^(−1),which is 8.6 times that of pristine ZnIn_(2)S_(4) and 3.0 times that of the Sv-ZnIn_(2)S_(4) samples.Based on the experimental result,the photo-reactivity S-scheme mechanism of hydrogen evolution from water splitting with Sv-ZnIn_(2)S_(4)@Sb_(2)S_(3) is proposed.This work provides an effective method for developing S-scheme heterojunction composites of transition metal sulfide with high hydrogen evolution performance.
基金supported by the National Natural Science Foundation of China(22279052)the China Postdoctoral Science Foundation(2023M741613)。
文摘Photoelectrocatalytic seawater splitting is a promising low-cost method to produce green hydrogen in a large scale.The effects of Cl^(-)ions in seawater on the performance of a photoanode have been reported in previous studies.However,few researches have been done on the roles of Cl^(-)ions in a photocathode.Herein,for the first time,we find that Cl^(-)ions in the electrolyte improve the photocurrent of a Si/In_(2)S_(3) photocathode by 50% at-0.6 V_(RHE).An in-situ X-ray photoelectron spectroscopy(XPS)characterization combined with the time-of-flight secondary-ion mass spectrometry by simulating photoelectrochemical conditions was used to investigate the interface charge transfer mechanism.The results suggest that there is an In_(2)^(+3)S_(3-x)(OH)_(2x)layer on the surface of In_(2)S_(3) in the phosphate buffer solution(PBS)electrolyte,which plays a role as an interface charge transfer mediator in the Si/In_(2)S_(3) photocathode.The In_(2)^(+3)S_(3-x)(OH)_(2x)surface layer becomes In_(2)^(+3)S_(3-x)(Cl)_(2x)in the PBS electrolyte with NaCl and accelerates the charge transfer rate at the In_(2)S_(3)/electrolyte interface.These results offer a new concept of regulating interface charge transfer mediator to enhance the performance of photoelectrocatalytic seawater splitting for hydrogen production.
基金This work was financially supported by National Natural Sci-ence Foundation(No.52000044)the Outstanding Youth Project of Guangdong Natural Science Foundation(No.2021B1515020051)+3 种基金the Natural Science Foundation of Guangdong Province(Nos.2021A1515012610,2019050001)Special Fund Project of Science and Technology Application in Guangdong(No.2017B020240002)National 111 project,Department of Science and Technology of Guangdong(Nos.2019JC01L203,2020B0909030004)Science and Technology Program of Guangzhou(No.202102010418).
文摘A novel benzene-ring engineered 1D/2D WO_(3)/g-C_(3)N_(4)S-scheme photocatalyst(BCNW)was rationally de-signed and successfully synthesized by the electrostatic self-assembly method.Experimental and Density Functional Theory results reveal that the integration of molecular benzene-ring in the framework of g-C_(3)N_(4)can not only narrow its bandgap and accelerate charge separation by forming a mid-state at the top of its valence band but more importantly open up a new additional bridge for speeding up the interfacial S-scheme charge transfer in BCNW.Benefitting from those multiple positive effects of benzene-ring inte-gration,as expected,BCNW S-scheme photocatalysts show superior photocatalytic H_(2)-production activity and reach 2971μmol h^(-1)g^(-1)under visible-light illumination,which is 3.35 times WO_(3)/g-C_(3)N_(4)S-scheme photocatalyst without benzene-ring integration.This work supplies an innovative strategy for the design of a high-efficiency S-scheme photocatalytic system by constructing a facile and additional molecular charge transfer channel at the interface.
基金We would like to acknowledge the financial support from the National Natural Science Foundation of China （Nos. 21071055 and 21172076）, Shandong Provincial Natural Science Foundation for Distinguished Young Scholar （No. JQ201205）, Taishan Scholar Program of Shandong Province （No. ts201511004）, and Independent Innovation Foundation of Shandong University.
文摘Galvanic replacement, one of the popular strategies for producing hollow metallic nanostructures, has enjoyed great success in the past. However, it is rarely used with Au nanopartides as the self-sacrificed templates, even though these nanoparticles can be produced with well-controlled size, shape, and structure. Here, both Ag and Au from the core-sheU Au@Ag nanorods are demonstrated to be involved in the galvanic replacement for producing hollow nanostructures. The enhanced oxidation of metallic Au could be attributed to the close contact between Au and Ag and the unique charge compensation from Au to Ag, both of which are indispensable for the etching of Au via galvanic replacement. As a result of this reaction, these bimetallic nanorods experience a structural evolution from nanorattles, to tip-empty nanorods, and eventually to porous nanotubes. The nanotubes exhibit high catalytic activities in the electrooxidation of formic acid. These results not only disclose the underlying mechanism by which metallic Au could be replaced under mild conditions, but also expand the selection of self-sacrificed templates for galvanic replacement, which is an important reaction in many applications.
基金supported by the National Natural Science Foundation of China(51772319,51772320,51972331,and 61575196)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(2018356)+7 种基金the External Cooperation Program of the Chinese Academy of Sciences(121E32KYSB20190008)the Outstanding Youth Fund of Jiangxi Province(20192BCBL23027)the Natural Science Foundation of Jiangxi Province(20181ACB20011)the Six Talent Peaks Project of Jiangsu Province(XCL-170)the Science and Technology Project of Nanchang(2017-SJSYS-008)the Chongqing Talents Program(grant no.CQYC201905041)the Chongqing Scientific and Technological Program Project of China(cstc2019jcyj-msxmX0663)the Science and Technology Research Program of Chongqing Municipal Education Commission(grant no.KJQN201904102).
文摘Surface enhanced Raman scattering(SERS)is a fingerprint spectral technique whose performance is highly dependent on the physicochemical properties of the substrate materials.In addition to the traditional plasmonic metal substrates that feature prominent electromagnetic enhancements,boosted SERS activities have been reported recently for various categories of non-metal materials,including graphene,MXenes,transition-metal chalcogens/oxides,and conjugated organic molecules.Although the structural compositions of these semiconducting substrates vary,chemical enhancements induced by interfacial charge transfer are often the major contributors to the overall SERS behavior,which is distinct from that of the traditional SERS based on plasmonic metals.Regarding charge-transfer-induced SERS enhancements,this short review introduces the basic concepts underlying the SERS enhancements,the most recent semiconducting substrates that use novel manipulation strategies,and the extended applications of these versatile substrates.
基金supported by the National Natural Science Foundation of China(Nos.22172019,52002054)the Sichuan Science and Technology Program(No.2022JDRC0084)。
文摘The NO gas is easily oxidized to form toxic by-products(NO_(2))during the oxidation process,which are adsorbed on the catalyst surface and inhibit the subsequent reaction.For photocatalytic NO removal,a significant challenge is to achieve catalytic stability while maintaining high conversion efficiency.Here,we fabricated a(BiO)_(2)CO_(3)/β-Bi_(2)O_(3)heterostructure that enables efficient charge transfer and promotes the NO removal.We propose that the catalytic stability depends on the heterojunction structure,which is able to generate interfacial charge transfer channels.In addition,we further introduce graphene quantum dots on the heterojunction structure,which further strengthens the interfacial charge transfer dynamics and finally realizes that the NO_(2)byproduct could gain electrons and convert to the final product(nitrite or nitrate).This composite structure not only exhibits high activity for NO removal but also maintains long-term stability under visible light.
文摘We investigate nanorod assemblies of two 64-substituted pentacenes, namely （2,3-X2-9,10-Y2）-substituted pentacenes with X -- Y = OCH3 （MOP） and with X = F, Y-- OCH3 （MOPF）, grown on Au（111） single crystals. By using a multi-technique approach based on ultraviolet photoelectron spectroscopy X-ray photoelectron spectroscopy; and X-ray absorption, we find evidence for charge transfer screening at the interface with gold. Furthermore, the MOP and MOPF nanorods show a rough surface morphology, which was investigated with atomic force microscopy. We use molecular simulation techniques to investigate the energetic barriers to diffusion and to traverse step-edges to estimate their influence on the nanorod roughness. We find that barriers to surface diffusion on a terrace are anisotropic and that their direction favors the formation of nanorods in these materials.
