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Simultaneous hydrogen and peroxide production by photocatalytic water splitting 被引量:13
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作者 Lichao Wang Shuang Cao +3 位作者 Kai Guo Zhijiao Wu Zhi Ma Lingyu Piao 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第3期470-475,共6页
Photocatalytic oxidation of water is a promising method to realize large-scale H2O2 production without a hazardous and energy-intensive process. In this study, we introduce a Pt/TiO2(anatase) photocatalyst to construc... Photocatalytic oxidation of water is a promising method to realize large-scale H2O2 production without a hazardous and energy-intensive process. In this study, we introduce a Pt/TiO2(anatase) photocatalyst to construct a simple and environmentally friendly system to achieve simultaneous H2 and H2O2 production. Both H2 and H2O2 are high-value chemicals, and their separation is automatic. Even without the assistance of a sacrificial agent, the system can reach an efficiency of 7410 and 5096 μmol g^-1 h^–1 (first 1 h) for H2 and H2O2, respectively, which is much higher than that of a commercial Pt/TiO2(anatase) system that has a similar morphology. This exceptional activity is attributed to the more favorable two-electron oxidation of water to H2O2, compared with the four-electron oxidation of water to O2. 展开更多
关键词 photocatalytic water splitting HYDROGEN Hydrogen peroxide Anatase TiO2
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Machine learning aided design of perovskite oxide materials for photocatalytic water splitting 被引量:6
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作者 Qiuling Tao Tian Lu +3 位作者 Ye Sheng Long Li Wencong Lu Minjie Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第9期351-359,共9页
Suffering from the inefficient traditional trial-and-error methods and the huge searching space filled by millions of candidates, discovering new perovskite visible photocatalysts with higher hydrogen production rate(... Suffering from the inefficient traditional trial-and-error methods and the huge searching space filled by millions of candidates, discovering new perovskite visible photocatalysts with higher hydrogen production rate(RH_(2)) still remains a challenge in the field of photocatalytic water splitting(PWS). Herein, we established structural-property models targeted to RH_(2) and the proper bandgap(Eg) via machine learning(ML) technology to accelerate the discovery of efficient perovskite photocatalysts for PWS. The Pearson correlation coefficients(R) of leave-one-out cross validation(LOOCV) were adopted to compare the performances of different algorithms including gradient boosting regression(GBR), support vector regression(SVR), backpropagation artificial neural network(BPANN), and random forest(RF). It was found that the BPANN model showed the highest R values from LOOCV and testing data of 0.9897 and 0.9740 for RH_(2),while the GBR model had the best values of 0.9290 and 0.9207 for Eg. Furtherly, 14 potential PWS perovskite candidates were screened out from 30,000 ABO3-type perovskite structures under the criteria of structural stability, Eg, conduction band energy, valence band energy and RH_(2). The average RH_(2) of these14 perovskites is 6.4% higher than the highest value in the training data set. Moreover, the online web servers were developed to share our prediction models, which could be accessible in http://materialsdata-mining.com/ocpmdm/material_api/ahfga3d9puqlknig(E_g prediction) and http://materials-datamining.com/ocpmdm/material_api/i0 ucuyn3 wsd14940(RH_(2) prediction). 展开更多
关键词 PEROVSKITE Machine learning Online web service photocatalytic water splitting Bandgap Hydrogen production rate
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Engineering the Local Coordination Environment of Single-Atom Catalysts and Their Applications in Photocatalytic Water Splitting:A Review
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作者 Hongli Sun Yunfei Ma +1 位作者 Qitao Zhang Chenliang Su 《Transactions of Tianjin University》 EI CAS 2021年第4期313-330,共18页
Single-atom catalysts(SACs),with atomically dispersed metal atoms anchored on a typical support,representing the utmost utilization effi ciency of the atoms,have recently emerged as promising catalysts for a variety o... Single-atom catalysts(SACs),with atomically dispersed metal atoms anchored on a typical support,representing the utmost utilization effi ciency of the atoms,have recently emerged as promising catalysts for a variety of catalytic applications.The electronic properties of the active center of SACs are highly dependent on the local environment constituted by the single metal atom and its surrounding coordination elements.Therefore,engineering the coordination environment near single metal sites,from the fi rst coordination shell to the second shell or higher,would be a rational way to design effi cient SACs with optimized electronic structure for catalytic applications.The wide range of coordination confi gurations,guaranteed by the multiple choices of the type and heterogeneity of the coordination element(N,O,P,S,etc.),further off er a large opportunity to rationally design SACs for satisfactory activities and investigate the structure-performance relationship.In this review,the coordination engineering of SACs by varying the type of coordination element was elaborated and the photocatalytic water splitting of SACs was highlighted.Finally,challenging issues related to the coordination engineering of SACs and their photocatalytic applications were discussed to call for more eff orts devoted to the further development of single-atom catalysis. 展开更多
关键词 Single-atom catalysts Coordination engineering Coordination environment photocatalytic water splitting
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Mg-doped SrTaO_(2)N as a visible-light-driven H_(2)-evolution photocatalyst for accelerated Z-scheme overall water splitting
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作者 Jun Xu Ying Luo +4 位作者 Qiaoqi Guo Wenzheng Sun Shanshan Chen Zheng Wang Hong He 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第10期70-78,共9页
Perovskite SrTaO_(2)N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting.However,the formation of defect states during thermal nitridation severely hinders the separation o... Perovskite SrTaO_(2)N is one of the most promising narrow-bandgap photocatalysts for Z-scheme overall water splitting.However,the formation of defect states during thermal nitridation severely hinders the separation of charges,resulting in poor photocatalytic activity.In the present study,we successfully synthesize SrTaO_(2)N photocatalyst with low density of defect states,uniform morphology and particle size by flux-assisted one-pot nitridation combined with Mg doping.Some important parameters,such as the size of unit cell,the content of nitrogen,and microstructure,prove the successful doping of Mg.The defect-related carrier recombination has been significantly reduced by Mg doping,which effectively promotes the charge separation.Moreover,Mg doping induces a change of the band edge,which makes proton reduction have a stronger driving force.After modifying with the core/shell-structured Pt/Cr_(2)O_(3)cocatalyst,the H_(2)evolution activity of the optimized SrTaO_(2)N:Mg is 10 times that of the undoped SrTaO_(2)N,with an impressive apparent quantum yield of 1.51%at 420 nm.By coupling with Au-FeCoO_(x)modified BiVO_(4)as an O_(2)-evolution photocatalyst and[Fe(CN)_(6)]_(3)−/[Fe(CN)_(6)]_(4)−as the redox couple,a redox-based Z-scheme overall water splitting system is successfully constructed with an apparent quantum yield of 1.36%at 420 nm.This work provides an alternative way to prepare oxynitride semiconductors with reduced defects to promote the conversion of solar energy. 展开更多
关键词 photocatalytic overall water splitting SrTaO_(2)N photocatalyst Mg doping Defect density COCATALYST
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Enhanced photocatalytic water splitting with surface defective SrTiO_(3)nanocrystals 被引量:1
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作者 Junying LIU Zhidong WEI Wenfeng SHANGGUAN 《Frontiers in Energy》 SCIE CSCD 2021年第3期700-709,共10页
Surface reconstructed SrTiO_(3)nanocrystals were synthesized by a thermal treatment process in presence of NaBH_(4)and SrTiO_(3)nanocrystals.The surface reconstruction of SrTiO_(3)nanocrystals is attributed to the int... Surface reconstructed SrTiO_(3)nanocrystals were synthesized by a thermal treatment process in presence of NaBH_(4)and SrTiO_(3)nanocrystals.The surface reconstruction of SrTiO_(3)nanocrystals is attributed to the introduction of surface oxygen vacancies or Ti sites(such as Ti^(3+)and Ti^(2+))during the hydrogenation treatment process.The light absorption and the charge transfer ability of SrTiO_(3)nanocrystals are simultaneously enhanced due to surface oxygen vacancies or Ti sites(such as Ti^(3+)and Ti^(2+)),which are beneficial to photocatalytic water splitting.Meanwhile,these defects also change the redox potential of the photocatalysts.Since there existed a synergistic effect between the three,the ratio of hydrogen to oxygen production was also regulated. 展开更多
关键词 SrTiO_(3) surface reconstruction oxygen vacancies photocatalytic water splitting
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Water oxidation sites located at the interface of Pt/SrTiO_(3) for photocatalytic overall water splitting 被引量:1
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作者 Xianwen Zhang Zheng Li +4 位作者 Taifeng Liu Mingrun Li Chaobin Zeng Hiroaki Matsumoto Hongxian Han 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第8期2223-2230,共8页
When a proton reduction cocatalyst is loaded on an n-type semiconductor for photocatalytic overall water splitting(POWS),the location of water oxidation sites is generally considered at the surface of the semiconducto... When a proton reduction cocatalyst is loaded on an n-type semiconductor for photocatalytic overall water splitting(POWS),the location of water oxidation sites is generally considered at the surface of the semiconductor due to upward band-bending of n-type semiconductor which may ease the transfer of the photogenerated holes to the surface.However,this is not the case for Pt/SrTiO_(3),a model semiconductor based photocatalyst for POWS.It was found that the photogenerated holes are more readily accumulated at the interface between Pt cocatalyst and SrTiO_(3) photocatalyst as probed by photo-oxidative deposition of PbO_(2),indicating that the water oxidation sites are located at the interface between Pt and SrTiO_(3).Electron paramagnetic resonance and scanning transmission electron microscope studies suggest that the interfacial oxygen atoms between Pt and SrTiO_(3) in Pt/SrTiO_(3) after POWS are more readily lost to form oxygen vacancies upon vacuum heat treatment,regardless of Pt loading by photodeposition or impregnation methods,which may serve as additional support for the location of the active sites for water oxidation at the interface.Density functional theory calculations also suggest that the oxygen evolution reaction more readily occurs at the interfacial sites with the lowest overpotential.These experimental and theoretical studies reveal that the more active sites for water oxidation are located at the interface between Pt and SrTiO_(3),rather than on the surface of SrTiO_(3).Hence,the tailor design and control of the interfacial properties are extremely important for the achievement or improvement of the POWS on cocatalyst loaded semiconductor photocatalyst. 展开更多
关键词 photocatalytic overall water splitting Active site Oxygen vacancy INTERFACE COCATALYST
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Electron transfer kinetics in CdS/Pt heterojunction photocatalyst during water splitting 被引量:2
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作者 Jianjun Zhang Gaoyuan Yang +4 位作者 Bowen He Bei Cheng Youji Li Guijie Liang Linxi Wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第10期2530-2538,共9页
Noble metal cocatalysts have shown great potential in boosting the performance of CdS in photocatalytic water splitting.However,the mechanism and kinetics of electron transfer in noble-metal-decorated CdS during pract... Noble metal cocatalysts have shown great potential in boosting the performance of CdS in photocatalytic water splitting.However,the mechanism and kinetics of electron transfer in noble-metal-decorated CdS during practical hydrogen evolution is not clearly elucidated.Herein,Pt-nanoparticle-decorated CdS nanorods(CdS/Pt)are utilized as the model system to analyze the electron transfer kinetics in CdS/Pt heterojunction.Through femtosecond transient absorption spectroscopy,three dominating exciton quenching pathways are observed and assigned to the trapping of photogenerated electrons at shallow states,recombination of free electrons and trapped holes,and radiative recombination of locally photogenerated electron-hole pairs.The introduction of Pt cocatalyst can release the electrons trapped at the shallow states and construct an ultrafast electron transfer tunnel at the CdS/Pt interface.When CdS/Pt is dispersed in acetonitrile,the lifetime and rate for interfacial electron transfer are respectively calculated to be~5.5 ps and~3.5×10^(10) s^(−1).The CdS/Pt is again dispersed in water to simulate photocatalytic water splitting.The lifetime of the interfacial electron transfer decreases to~5.1 ps and the electron transfer rate increases to~4.9×10^(10) s^(−1),confirming that Pt nanoparticles serve as the main active sites of hydrogen evolution.This work reveals the role of Pt cocatalysts in enhancing the photocatalytic performance of CdS from the perspective of electron transfer kinetics. 展开更多
关键词 Femtosecond transient absorption SPECTROSCOPY photocatalytic water splitting CDS Electron transfer kinetics Trap state
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Blue phosphorene/MoSi2N4 van der Waals type-Ⅱ heterostructure:Highly efficient bifunctional materials for photocatalytics and photovoltaics
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作者 李晓华 王宝基 柯三黄 《Chinese Physics B》 SCIE EI CAS CSCD 2023年第2期429-435,共7页
Converting solar energy into electric power or hydrogen fuel is a promising means to obtain renewable green energy.Here, we design a two-dimensional blue phosphorene(BlueP)/MoSi2N4van der Waals heterostructure(vdWH) a... Converting solar energy into electric power or hydrogen fuel is a promising means to obtain renewable green energy.Here, we design a two-dimensional blue phosphorene(BlueP)/MoSi2N4van der Waals heterostructure(vdWH) and investigate its potential application in photocatalysis and photovoltaics using first-principles calculations. We find that the BlueP/MoSi2N4vdWH possesses type-Ⅱ band structure with a large build-in electric field, thus endowing it with a potential ability to separate photogenerated electron–hole pairs. The calculated band-edge positions show that the heterostructure is a very promising water-splitting photocatalyst. Its solar-to-hydrogen efficiency(ηSTH) can reach up to 15.8%, which is quite promising for commercial applications. Furthermore, the BlueP/MoSi2N4vdWH shows remarkably light absorption capacity and distinguished maximum power conversion efficiency(ηPCE) up to 10.61%. Remarkably, its ηPCEcan be further enhanced by the external strain: the ηPCEof 21.20% can be obtained under a 4% tensile strain. Finally, we determine that adjusting the number of the BlueP sublayer is another effective method to modulate the band gaps and band alignments of the heterostructures. These theoretical findings indicate that BlueP/MoSi2N4vd WH is a promising candidate for photocatalyst and photovoltaic device. 展开更多
关键词 ab initio study HETEROSTRUCTURE photovoltaic cell photocatalytic water splitting
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Reducing the vacancies associated with ferroelectric polarization to promote photocatalytic overall water splitting
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作者 Haozhi Qi Yuyang Kang +8 位作者 Jian-An Liu Lichang Yin Wenyu Zhang Shangyi Ma Jianhang Qiu Lingli Li Weijin Hu Lianzhou Wang Gang Liu 《Science China Chemistry》 SCIE EI CAS CSCD 2024年第10期3258-3264,共7页
Ferroelectric materials hold great promise in photocatalytic water splitting because their built-in electric field induced by the depolarization field can fulfill the separation of photogenerated carriers.However,a nu... Ferroelectric materials hold great promise in photocatalytic water splitting because their built-in electric field induced by the depolarization field can fulfill the separation of photogenerated carriers.However,a number of intrinsic charged vacancy defects are simultaneously generated to screen the depolarized field for stabilizing the crystal structure,always resulting in severe recombination of photogenerated carriers and thus poor overall water splitting activity.Herein,we proposed a strategy to promote the separation and transport of photogenerated carriers of ferroelectric photocatalysts by adjusting the ferroelectric polarization and altering the coordination environment of elements to reduce the defect concentration.Specifically,we prepared a series of Ta-doped PbTiO_(3)with low Pb(V_(Pb))and O(V_(O))vacancy concentrations by reducing the polarization intensity and strengthening the Pb–O interaction.The Ta-doped PbTiO_(3)shows efficient charge separation and greatly enhanced photocatalytic overall water splitting activity with the assistance of cocatalyst.This work highlights the importance of regulating ferroelectric polarization and vacancy defect concentration by the doping strategy in charge separation for photocatalytic water splitting. 展开更多
关键词 PbTiO_(3) ferroelectric polarization vacancy defect element doping photocatalytic overall water splitting
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Regulating photocatalytic overall water splitting of ferroelectric heterostructures by size effect
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作者 Zixing Ye Daifu Yu +8 位作者 Ruian Zhang Fei Qin Yiran Sun Jie Huang Zhanqi Zhou He Tian Gaorong Han Zhaohui Ren Gang Liu 《Nano Research》 SCIE EI CSCD 2024年第9期8000-8006,共7页
In the past decade,ferroelectric materials have been intensively explored as promising photocatalysts.An intriguing ability of ferroelectrics is to directly sperate the photogenerated electrons and holes,which is beli... In the past decade,ferroelectric materials have been intensively explored as promising photocatalysts.An intriguing ability of ferroelectrics is to directly sperate the photogenerated electrons and holes,which is believed to arise from a spontaneous polarization.Understanding how polarization affects the photocatalytic performance is vital to design high-efficiency photocatalysts.In this work,we report a size effect of ferroelectric polarization on regulating the photocatalytic overall water splitting of SrTiO_(3)/PbTiO_(3)nanoplate heterostructures for the first time.This was realized hydrothermally by controlling the thickness and thus spontaneous polarization strength of single-crystal and single-domain PbTiO_(3)nanoplates,which served as the substrate for selective heteroepitaxial growth of SrTiO_(3).An enhancement of 22 times in the photocatalytic overall water splitting performance of the heterostructures has been achieved when the average thickness of the nanoplate increases from 30 to 107 nm.A combined experimental investigation revealed that the incompletely compensated depolarization filed is the dominated driving force for the photogenerated carrier separation within heterostructures,and its increase with the thickness of the nanoplates accounts for the enhancement of photocatalytic activity.Moreover,the concentration of oxygen vacancies for negative polarization compensation has been found to grow as the thickness of the nanoplates increases,which promotes oxygen evolution reaction and reduces the stoichiometric ratio of H_(2)/O_(2).These findings may provide the opportunity to design and develop high-efficiency ferroelectric photocatalysts. 展开更多
关键词 single-domain nanoplates size effect ferroelectric polarization screening photocatalytic overall water splitting
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Activating d^(10)electronic configuration to regulate p-band centers as efficient active sites for solar energy conversion into H_(2)by surface atomic arrangement
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作者 Shanshan Lai Jiakun Su +2 位作者 Shujuan Jiang Jianjun Zhang Shaoqing Song 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第10期185-194,共10页
Relationship between the activity for photocatalytic H_(2)O overall splitting(HOS)and the electron occupancy on d orbits of the active component in photocatalysts shows volcanic diagram,and specially the d^(10)electro... Relationship between the activity for photocatalytic H_(2)O overall splitting(HOS)and the electron occupancy on d orbits of the active component in photocatalysts shows volcanic diagram,and specially the d^(10)electronic configuration in valley bottom exhibits inert activity,which seriously fetters the development of catalytic materials with great potentials.Herein,In d^(10)electronic configuration of In_(2)O_(3)was activated by phosphorus atoms replacing its lattice oxygen to regulate the collocation of the ascended In 5p-band(Inɛ5p)and descended O 2p-band(Oɛ2p)centers as efficient active sites for chemisorption to*OH and*H during forward HOS,respectively,along with a declined In 4d-band center(Inɛ4d)to inhibit its backward reaction.A stable STH efficiency of 2.23%under AM 1.5 G irradiation at 65°C has been obtained over the activated d^(10)electronic configuration with a lowered activation energy for H_(2)evolution,verified by femtosecond transient absorption spectroscopy,in situ diffuse reflectance infrared Fourier transform spectroscopy and theoretical calculations of dynamics.These findings devote to activating d^(10)electronic configuration for resolving the reaction energy barrier and dynamical bottleneck of forward HOS,which expands the exploration of high-efficiency catalytic materials. 展开更多
关键词 d-Band center p-Band center Localized field photocatalytic water splitting Dynamic process
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Self-assembled synthesis of oxygen-doped g-C3N4 nanotubes in enhancement of visible-light photocatalytic hydrogen 被引量:7
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作者 Yizeng Zhang Zhiwu Chen +2 位作者 Jinliang Li Zhenya Lu Xin Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第3期36-44,共9页
Currently,photocatalytic water splitting is regarded as promising technology in renewable energy generation.However,the conversion efficiency suffers great restriction due to the rapid recombination of charge carriers... Currently,photocatalytic water splitting is regarded as promising technology in renewable energy generation.However,the conversion efficiency suffers great restriction due to the rapid recombination of charge carriers.Rational designed the structure and doping elements become important alternative routes to improve the performance of photocatalyst.In this work,we rational designed oxygen-doped graphitic carbon nitride(OCN)nanotubes derived from supermolecular intermediates for photocata lytic water splitting.The as prepared OCN nanotubes exhibit an outstanding hydrogen evolution rate of 73.84μmol h^(-1),outperforming the most of reported one dimensional(1D)g-C_(3)N_(4) previously.Due to the rational oxygen doping,the band structure of g-C_(3)N_(4) is meliorated,which can narrow the band gap and reduce the recombination rate of photogene rated carriers.Furthermore,the hollow nanotube structure of OCN also provide multiple diffuse reflection during photocata lytic reaction,which can significantly promote the utilization capacity of visible light and enhance the photocatalytic water splitting performance.It is believed that our work not only rationally controls the nanostructure,but also introduces useful heteroatom into the matrix of photocatalyst,which provides an effective way to design high-efficiency g-C_(3)N_(4) photocatalyst. 展开更多
关键词 Graphitic carbon nitride Oxygen-doped NANOTUBE photocatalytic water splitting Reaction process
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Fluorination over Cr doped layered perovskite Sr_(2)TiO_(4) for efficient photocatalytic hydrogen production under visible light illumination
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作者 Jinxing Yu Xiaoxiang Xu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第12期30-38,共9页
Cr doped Ruddlesden-Popper compound Sr2 TiO4 has been successfully modified by fluorine to form a new compound Sr2 Ti(0.95) Cr(0.05) O3 F2. Structure analysis suggests two types of fluorine in the structure of this ne... Cr doped Ruddlesden-Popper compound Sr2 TiO4 has been successfully modified by fluorine to form a new compound Sr2 Ti(0.95) Cr(0.05) O3 F2. Structure analysis suggests two types of fluorine in the structure of this new compound, i.e. intralayer and interlayer F, which induce strong built-in electric field within this layered compound. The electric field stems from uneven distribution of F atoms on the two sides of perovskite layers therefore leads to charge disproportionation. DFT calculations suggest that this unique structural feature is highly beneficial for charge dissociations as it breaks the coplanar settlement of conduction band minimum and valence band maximum whilst maintains the 2 D charge transportation properties. This is clearly demonstrated by the superior photocatalytic activities of Sr2 Ti(0.95) Cr(0.05) O3 F2 for hydrogen production from water. Apparent quantum efficiency(AQE) as high as 1.16% at 420 ± 20 nm has been achieved which stands as the highest AQE reported on Sr2 TiO4 to date. Photoelectrochemical(PEC)analysis confirms improved charge separation conditions and prolonged charge lifetime. 展开更多
关键词 DFT FLUORINATION Sr_(2)TiO_(4) photocatalytic water splitting 2D charge transportation
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Simultaneously Effi cient Solar Light Harvesting and Charge Transfer of Hollow Octahedral Cu_(2)S/CdS p-n Heterostructures for Remarkable Photocatalytic Hydrogen Generation
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作者 Yanting Zhang Lei Ran +7 位作者 Zhuwei Li Panlong Zhai Bo Zhang Zhaozhong Fan Chen Wang Xiaomeng Zhang Jungang Hou Licheng Sun 《Transactions of Tianjin University》 EI CAS 2021年第4期348-357,共10页
Solar-driven water splitting is a promising alternative to industrial hydrogen production.This study reports an elaborate design and synthesis of the integration of cadmium sulfi de(CdS)quantum dots and cuprous sulfi ... Solar-driven water splitting is a promising alternative to industrial hydrogen production.This study reports an elaborate design and synthesis of the integration of cadmium sulfi de(CdS)quantum dots and cuprous sulfi de(Cu_(2)S)nanosheets as three-dimensional(3D)hollow octahedral Cu_(2)S/CdS p-n heterostructured architectures by a versatile template and one-pot sulfi dation strategy.3D hierarchical hollow nanostructures can strengthen multiple refl ections of solar light and provide a large specifi c surface area and abundant reaction sites for photocatalytic water splitting.Owing to the construction of the p-n heterostructure as an ideal catalytic model with highly matched band alignment at Cu_(2)S/CdS interfaces,the emerging internal electric fi eld can facilitate the space separation and transfer of photoexcited charges between CdS and Cu_(2)S and also enhance charge dynamics and prolong charge lifetimes.Notably,the unique hollow Cu_(2)S/CdS architectures deliver a largely enhanced visible-light-driven hydrogen generation rate of 4.76 mmol/(g·h),which is nearly 8.5 and 476 times larger than that of pristine CdS and Cu_(2)S catalysts,respectively.This work not only paves the way for the rational design and fabrication of hollow photocatalysts but also clarifi es the crucial role of unique heterostructure in photocatalysis for solar energy conversion. 展开更多
关键词 Hollow octahedrons P-n heterostructure Charge separation photocatalytic water splitting
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Intrinsic Mechanisms of Morphological Engineering and Carbon Doping for Improved Photocatalysis of 2D/2D Carbon Nitride Van Der Waals Heterojunction
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作者 Jinqiang Zhang Xiaoli Zhao +10 位作者 Lin Chen Shuli Li Haijun Chen Yuezhao Zhu Shuaijun Wang Yang Liu Huayang Zhang Xiaoguang Duan Mingbo Wu Shaobin Wang Hongqi Sun 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第3期96-106,共11页
Van der Waals(VDW)heterojunctions in a 2D/2D contact provide the highest area for the separation and transfer of charge carriers.In this work,a top-down strategy with a gas erosion process was employed to fabricate a ... Van der Waals(VDW)heterojunctions in a 2D/2D contact provide the highest area for the separation and transfer of charge carriers.In this work,a top-down strategy with a gas erosion process was employed to fabricate a 2D/2D carbon nitride VDW heterojunction in carbon nitride(g-C_(3)N_(4))with carbon-rich carbon nitride.The created 2D semiconducting channel in the VDW structure exhibits enhanced electric field exposure and radiation absorption,which facilitates the separation of the charge carriers and their mobility.Consequently,compared with bulk g-C_(3)N_(4)and its nanosheets,the photocatalytic performance of the fabricated carbon nitride VDW heterojunction in the water splitting reaction to hydrogen is improved by 8.6 and 3.3 times,respectively,while maintaining satisfactory photo-stability.Mechanistically,the finite element method(FEM)was employed to evaluate and clarify the contributions of the formation of VDW heterojunction to enhanced photocatalysis,in agreement quantitatively with experimental ones.This study provides a new and effective strategy for the modification and more insights to performance improvement on polymeric semiconductors in photocatalysis and energy conversion. 展开更多
关键词 carbon nitride Van der Waals heterojunctions enhanced electric field exposure improved radiation absorption photocatalytic water splitting promoted dynamics of charge carriers
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Sulfone-functionalized stable molecular single crystals for photocatalytic hydrogen evolution
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作者 Xunliang Hu Xiaoju Yang +9 位作者 Bingyi Song Zhen Zhan Ruixue Sun Yantong Guo Li-Ming Yang Xuan Yang Chun Zhang Irshad Hussain Xiaoyan Wang Bien Tan 《SusMat》 SCIE EI 2024年第3期240-250,共11页
Highly crystalline organic semiconductors are ideal materials for photocatalytic hydrogen evolution in water splitting.However,the instability and complex synthesis processes of most reported organic molecule-based ph... Highly crystalline organic semiconductors are ideal materials for photocatalytic hydrogen evolution in water splitting.However,the instability and complex synthesis processes of most reported organic molecule-based photocatalysts restrict their applications.In this study,we introduce benzo[1,2-b:4,5-bʹ]bis[1]benzothiophene-3,9-dicarboxylic acid,5,5,11,11-tetraoxide(FSOCA),a highly crystalline,stable molecular crystal that is easy to synthesize and serves as an efficient photocatalyst for the hydrogen evolution reaction.FSOCA exhibits high efficiency in sacrificial hydrogen evolution reaction(760μmol h^(−1),76 mmol g^(−1)h^(−1)at 330 mW cm^(−2);570μmol h^(−1),57 mmol g^(−1)h^(−1)at 250 mW cm^(−2)),and FSOCA remains stable during photocatalysis for up to 400 h.Experiments and theoretical studies confirmed the presence of hydrogen bonds between the sulfone group and the sacrificial agent(ascorbic acid).This interaction significantly improved the oxidation reaction kinetics and boosted the photocatalytic performance.This study presents a scalable and convenient approach to synthesize highly crystalline,active,and stable organic photocatalysts with potential applications in large-scale photocatalysis. 展开更多
关键词 exceptional durability molecular single crystals photocatalytic water splitting
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Synthesis and application of transition metal phosphides as electrocatalyst for water splitting 被引量:16
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作者 Jinzhan Su Jinglan Zhou +2 位作者 Lu Wang Cong Liu Yubin Chen 《Science Bulletin》 SCIE EI CAS CSCD 2017年第9期633-644,共12页
With continuous research on photocatalytic water splitting, searching for efficient catalyst for hydrogen evolution reaction(HER) becomes popular topic in addition to main catalyst research. Transition metal phosphide... With continuous research on photocatalytic water splitting, searching for efficient catalyst for hydrogen evolution reaction(HER) becomes popular topic in addition to main catalyst research. Transition metal phosphides are receiving intense attention due to its abundance in the Earth's crust and comparable catalytic properties to noble metals. In this review, the synthesis approaches, HER reaction mechanism,photocatalytic activity, approaches to improve the activity of transition metal phosphides were reviewed and discussed. It was showed that the transition metal phosphides have great potential to reduce the cost of photocatalyst and promising application on water splitting. The stability problem and participation of poisonous reactant and product in its synthesis reaction limit its application and developing in a certain extent, but with the continuous efforts on the development and improvement of the synthesis methods,transition metal phosphides will find wide application in water splitting. 展开更多
关键词 Transition metal phosphide ELECTROCATALYST HER photocatalytic water splitting
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Facile one-pot hydrothermal method to prepare Sn(Ⅱ) and N co-doped TiO_(2) photocatalyst for water splitting under visible light irradiation 被引量:8
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作者 Xiao-Huan Jiang Ying-Nan Duan +5 位作者 Yu Tian Meng Chen Mao-Kun Li Huan-Huan Liu Wan-Liang Yang Meng-Kui Tian 《Rare Metals》 SCIE EI CAS CSCD 2022年第2期406-414,共9页
In this paper,a visible light-responsive Sn^(2+)and N co-doped TiO_(2)photocatalyst was prepared by facile one-pot hydrothermal method.All as-prepared samples were characterized in detail by a series of characterizati... In this paper,a visible light-responsive Sn^(2+)and N co-doped TiO_(2)photocatalyst was prepared by facile one-pot hydrothermal method.All as-prepared samples were characterized in detail by a series of characterization approaches.The results showed that the Sn^(2+)and N elements were co-doped into TiO_(2),while the catalyst still maintains anatase crystal structure and gets irregular little nanocluster in diameter of 9–10 nm with higher specific surface area.The absorption edge of Sn^(2+)and N co-doped TiO_(2)extends to the visible light region.Compared with Sn^(2+)-doped TiO_(2)and N-TiO_(2),the absorption edges have obvious red-shift of about 50 and 70 nm,respectively.The synergistic effect of O 2p-N 2p and O 2p-Sn 5s hybridization to form impurity levels is the main reason for the red-shift.The hydrogen production performance of the Sn^(2+)and N co-doping TiO_(2)(n(N)/n(Ti)=1)catalyst reached the maximum value of 0.37 mmol·h^(-1)·g^(-1)under visible light,which is higher than that of N-doped TiO_(2)and SnTiO_(2)-doped TiO_(2)singly.This result is due to the wider visible light region-responsive ability of Sn^(2+)and N codoped into TiO_(2).Furthermore,mild hydrothermal methods will not make the Sn^(2+)oxidized to Sn^(4+),which make the catalysts still maintain high photocatalytic performance.This work provides a simple and mild method for the preparation of dual-element co-doped TiO_(2)with high crystallinity,excellent performance and broad application prospects. 展开更多
关键词 PHOTOCATALYST photocatalytic water splitting Visible light driven Sn^(2+)and N co-doped TiO_(2)
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Highly-efficient overall water splitting in 2D Janus group-Ⅲ chalcogenide multilayers: the roles of intrinsic electric filed and vacancy defects 被引量:3
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作者 Yingcai Fan Xikui Ma +4 位作者 Junru Wang Xiaohan Song Aizhu Wang Hong Liu Mingwen Zhao 《Science Bulletin》 SCIE EI CSCD 2020年第1期27-34,M0003,共9页
Two-dimensional(2 D)van der Waals materials have been widely adopted as photocatalysts for water splitting,but the energy conversion efficiency remains low.On the basis of first-principles calculations,we demonstrate ... Two-dimensional(2 D)van der Waals materials have been widely adopted as photocatalysts for water splitting,but the energy conversion efficiency remains low.On the basis of first-principles calculations,we demonstrate that the 2 D Janus group-Ⅲchalcogenide multilayers:In Ga XY,M2XY and In GaX2(M=In/Ga;X,Y=S/Se/Te),are promising photocatalysts for highly-efficient overall water splitting.The intrinsic electric field enhances the spatial separations of photogenerated carriers and alters the band alignment,which is more pronounced compared with the Janus monolayers.High solar-to-hydrogen(STH)efficiency with the upper limit of 38.5%was predicted in the Janus multilayers.More excitingly,the Ga vacancy of In Ga SSe bilayer effectively lowers the overpotentials of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)to the levels provided solely by the photogenerated carriers.Our theoretical results suggest that the 2 D Janus group-III chalcogenide multilayers could be utilized as highly efficient photocatalysts for overall water splitting without the needs of sacrificial reagents. 展开更多
关键词 Janus group-Ⅲchalcogenides Solar-to-hydrogen efficiency photocatalytic water splitting Intrinsic electric fields First-principle calculation
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Controllable synthesis of Au-TiO2 nanodumbbell photocatalysts with spatial redox region 被引量:1
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作者 Ye Liu Zhaozhong Xiao +2 位作者 Shuang Cao Jinhui Li Lingyu Piao 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第1期219-226,共8页
Photocatalytic water splitting has increasingly attracted attention as one of the most useful methods of converting solar energy into chemical fuel.However,the undesirable reverse reaction significantly limits the enh... Photocatalytic water splitting has increasingly attracted attention as one of the most useful methods of converting solar energy into chemical fuel.However,the undesirable reverse reaction significantly limits the enhancement of efficiency.Herein,we fabricated an Au nanorods/TiO2 nanodumbbells structure photocatalyst(Au NRs/TiO2 NDs)via a facile synthetic strategy,which has spatially separated oxidation and reduction reaction zones.Owing to the unique structure,the charge separation of these photocatalysts can be significantly improved and the reverse reaction can be efficiently inhibited.The photogenerated electrons were injected from the TiO2 to the Au NRs,and a positively charged TiO2 region and negatively charged Au region were formed under UV irradiation.An enhanced hydrogen production performance was obtained compared with that seen in normal Au-TiO2 heterostructure.Under optimized conditions,the H2-production rate can reach up to 60,264μmol/g/h,about six times higher than previously reported Au/TiO2 photocatalysts.Besides this,our work also demonstrates the key factors of precise synthesis of the Au NRs/TiO2 NDs structure,which provides a new perspective and experience for the design of similar catalysts. 展开更多
关键词 Au nanorods Dumbbell structure photocatalytic water splitting Controllable synthesis
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