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Enhancing multifunctional photocatalysis with acetate-assisted cesium doping and unlocking the potential of z-scheme solar water splitting

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Carbon Energy 2024年第3期6卷 178-195页

作者： Mengmeng Ma Jingzhen Li Xiaogang zhu Kong Liu Kaige Huang Guodong Yuan Shizhong Yue zhijie Wang Shengchun Qu Key Laboratory of Semiconductor Materials Science Beijing Key Laboratory of Low Dimensional Semiconductor Materials and DevicesInstitute of SemiconductorsChinese Academy of SciencesBeijingChina Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijingChina Department of Physics College of Physical Science and TechnologyXiamen UniversityXiamenChina State Key Laboratory for Superlattices and Microstructures Institute of SemiconductorsChinese Academy of SciencesBeijingChina

Graphitic carbon nitride(g-C_(3)N_(4))has been extensively doped with alkali metals to enlarge photocatalytic output,in which cesium(Cs)doping is predicted to be the most efficient.Nevertheless,the sluggish diffusion and doping kinetics of precursors with high melting points,along with imprecise regulation,have raised the debate on whether Cs doping could make sense.For this matter,we attempt to confirm the positive effects of Cs doping on multifunctional photocatalysis by first using cesium acetate with the character of easy manipulation.The optimized Csdoped g-C_(3)N_(4)(CCN)shows a 41.6-fold increase in visible-light-driven hydrogen evolution reaction(HER)compared to pure g-C_(3)N_(4) and impressive degradation capability,especially with 77%refractory tetracycline and almost 100%rhodamine B degradedwithin an hour.The penetration ofCs+is demonstrated to be a mode of interlayer doping,and Cs–N bonds(especially with sp^(2) pyridine N in C═N–C),along with robust chemical interaction and electron exchange,are fabricated.This atomic configuration triggers the broadened spectral response,the improved charge migration,and the activated photocatalytic capacity.Furthermore,we evaluate the CCN/cadmium sulfide hybrid as a z-scheme configuration,promoting the visible HER yield to 9.02 mmol g^(−1) h^(−1),which is the highest ever reported among all CCN systems.This work adds to the rapidly expanding field of manipulation strategies and supports further development of mediating served for photocatalysis.

关键词： acetate-assisted cesium doping multifunctional photocatalysis z-scheme

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Efficient photocatalytic NADH regeneration with Rh-loaded z-scheme mediator-free system

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Chinese Chemical Letters 2024年第2期35卷 496-500页

作者： Yi zhou Yiling He Ming Gao Ningkai Ding Juying Lei Yanbo zhou State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process East China University of Science and TechnologyShanghai 200237China National Engineering Research Center of Industrial Wastewater Detoxication and Resource Recovery East China University of Science and TechnologyShanghai 200237China Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization East China University of Science and TechnologyShanghai 200237China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

Nicotinamide adenine dinucleotide(NADH)regeneration is necessary for the sustainable application of enzymatic industry.The Rh-based complex[Cp^(*)Rh(bpy)(H)]+has been widely used as an important mediator in NADH regeneration systems,but it is limited by complexity and high cost.Here,a z-scheme was constructed by loading Rh onto carbon nitride nanosheets/carbon nitride quantum dots(CN-CNQD).The resultant catalyst achieved a high yield of NADH in a mediator-free(M-free)system of 0.283 mmol L^(−1) g^(−1) min^(−1),which is 5.29 times that of pure CN.ADH enzyme introduction experiments confirmed that the enzyme active product 1,4-NADH could reach 34.21%selectivity in the M-free system.Mechanism research revealed that the heterojunction between CNs and CNQDs improved the NADH regeneration activity in the traditional M-involved system,while Rh loading was proved to optimize the yield and selectivity of 1,4-NADH in M-free system.The immobilized Rh shows more competitiveness than[Cp^(*)Rh(bpy)(H)]^(+).This study contributes to the construction of an M-free system for further application in greener,lower-cost enzymatic processes.

关键词： Photocatalysis NADH regeneration Mediator-free Carbon nitride z-scheme

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Reconcile the contradictory wettability requirements for the reduction and oxidation half-reactions in overall CO_(2) photoreduction via alternately hydrophobic surfaces

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Journal of Energy Chemistry 2024年第6期93卷 202-212,I0006页

作者： Hailing Huo Ting Hu Chengxi Huang Fang Wu Tongyu Wang Xuan Liu Liang zhang Qiang Ju zhiqing zhong Hongbin Xing Erjun Kan Ang Li MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing Nanjing University of Science and TechnologyNanjing 210094JiangsuChina College of Information Science and Technology Nanjing Forestry UniversityNanjing 210037JiangsuChina

The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of catalysts.However,there is a contradiction in wettability requirements for the two half-reactions.Specifically,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)reactants.Conversely,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic catalyst.This was achieved through a selectively hydrophobic modification method and a charge-transfer-control strategy.Consequently,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark catalyst.This innovative approach holds great potential for application in universal overall reactions involving gas participation.

关键词： Hydrophobic Hydrophilic Gas transport Overall CO_(2)photoreduction z-scheme

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NH_(4)Cl-assisted synthesis of TaON nanoparticle applied to photocatalytic hydrogen and oxygen evolution from water

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Journal of Energy Chemistry 2024年第7期94卷 541-550页

作者： Xu Kaiwei Liu Jifang zhang Boyang zhang Jiaming zhang Ke Shi Haifeng Wang Guijun Ma of Physical Science and Technology Shanghaitech UniversityShanghai 201210China

Oxynitride semiconductors are promising photocatalyst materials for visible light-driven water splitting,while the synthesis of well crystalized oxynitride still remains challenge.In present work,narrow-bandgap TaON nanoparticles are synthesized via heating a vacuum-sealed mixture of KTaO_(3),Ta and NHaCl.This method possesses multiple advantages in terms of lower calcination parameter,higher N conversion efficiency and superior photocatalytic activity in comparison with the traditional thermal ammonolysis using NH_(3) gas as a nitrogen source.Through the analysis of intermediates produced upon the elevation of heating temperature,a gas-solid-phase reaction between TaCl_(5) and Ta_(2)O_(5) is demon-strated as the final step,which is conducive to decreasing thermal energy barrier and accelerating nitri-dation process.Precise control of preparation conditions,including calcination temperature and duration,allows for the regulation of surface O/N ratio of TaoN particles to unity,resulting in optimized photocat-alytic activity.Photoelectrochemical assessment and intensity modulated photocurrent spectroscopy provide convincing evidence for improved charge transfer effciency of photoexcited holes at TaoN sur-face.A z-scheme overall water splitting is accomplished by employing the TaON as an effective oxygen evolution photocatalyst,SrTiO_(3):Rh as a hydrogen evolution photocatalyst,and reduced graphene oxide(rGO)as a solid-state electron mediator.This work presents a promising strategy for the synthesis of high-quality oxynitride materials in application to photocatalytic water splitting.

关键词： TaON Oxynitride synthesis Photocatalyst Water splitting,Hydrogen z-scheme

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Removal of hexavalent chromium from water by z-scheme photocatalysis using TiO_(2)(rutile)nanorods loaded with Au core-Cu_(2)0 shell particles

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Journal of Environmental Sciences 2022年第5期34卷 173-189页

作者： Sayaka Yanagida Takumi Yajima Takahiro Takei Nobuhiro Kumada Center for Crystal Science and Technology University of YamanashiKofu 400-8511Japan Advanced Materials Development Sector Tokyo Metropolitan Industrial Technology Research Institute2-4-10AomiKoto-kuTokyo 135-0064Japan

All-solid-state z-scheme photocatalysts,containing Cu_(2)O,TiO_(2)(rutile),and Au as the elec-tron mediator,were prepared and applied to the reduction of Cr(Ⅵ)in aqueous solutions.The Cu_(2)O-Au-TiO_(2) composites were prepared by loading Au core-Cu_(2)O shell hemisphere particles on TiO_(2)(rutile)nanorods using a two-step photocatalytic deposition process.Un-der ultraviolet-visible(UV-vis)light illumination,the Cu_(2)O-Au-TiO_(2) composites exhibited higher photocatalytic Cr(Ⅵ)reduction activities than those exhibited by single TiO_(2)(rutile)and Cu_(2)O.In this reaction,a precipitate containing Cr,which was considered to be Cr(OH)_(3),was deposited site-selectively on the Au core-Cu_(2)O shell particles of the composites,indi-cating that the reduction site of the composite was Cu_(2)O,and the reaction proceeded accord-ing to the z-scheme.The Cu_(2)O-Au-TiO_(2) composites also exhibited photocatalytic activity under visible light illumination.The oxidation state of Cu in the Cu_(2)O-Au-TiO_(2) composite gradually changed from Cu(Ⅰ)to Cu(Ⅱ)during the photocatalytic Cr(Ⅵ)reduction.However the composite maintained its high photocatalytic performance even after oxidation.The role of Au in the Cu_(2)O-Au-TiO_(2) composite was examined by comparing the properties of the Cu_(2)O-Au-TiO_(2) composite with those of the Cu_(2)O-TiO_(2) composite prepared via direct Cu_(2)O deposition on TiO_(2).

关键词： Cu_(2)O TiO_(2)(rutile) z-scheme Photocatalyst Chromium

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Construction of BiVO_(4)/BiOCl@C z-scheme heterojunction for enhanced photoelectrochemical performance

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International Journal of Minerals,Metallurgy and Materials 2022年第11期29卷 1971-1980页

作者： Jiaxin Li Hao Yuan Wenjie zhang Ruijie zhu zhengbo Jiao Institute of Materials for Energy and Environment College of Material Science and EngineeringQingdao UniversityQingdao 266071China

A z-scheme heterostructure of Mo,W co-doped BiVO_(4)(Mo,W:BVO/BiOCl@C)was fabricated by a simple solid solution drying and calcination(SSDC)method.The heterostructure was characterized by X-ray diffraction(XRD),Fourier transform infrared(FTIR),X-ray photoelectron spectroscopy(XPS),etc.Under visible light irradiation,Mo,W:BVO/BiOCl@C heterostructure exhibits excellent photoelectrochemical capability compared with other as-prepared samples.The photocurrent density and the incident photon-to-electron conversion efficiency(IPCE)are about 5.4 and 9.0 times higher than those of pure BiVO_(4),respectively.The enhancement of the photoelectrochemical performance can be attributed to the construct of z-scheme system,which is deduced from the radical trapping experiments.The Mo,W:BVO/BiOCl@C z-scheme heterojunction enhances the visible-light absorption and reduces the recombination rate of charge carriers.This work provides an effective strategy to construct z-scheme photoelectrodes for the application of photoelectrochemical water splitting.

关键词： photoelectrochemical bismuth vanadate BiOCl z-scheme carbon

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CdS nanoparticles decorated hexagonal Fe_(2)O_(3) nanosheets with a z-scheme photogenerated electron transfer path for improved visible-light photocatalytic hydrogen production

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Chinese Journal of Chemical Engineering 2022年第3期35卷 266-274页

作者： Feng Guo Haoran Sun Yuxing Shi Fengyu zhou Weilong Shi School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003China School of Material Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China

Photocatalytic water splitting for hydrogen production(H_(2))is one of the main potential applications of photocatalytic technology,which can use solar energy as the energy required for chemical reactions to alleviate the energy crisis.In this work,zero-dimensional/two-dimensional(0D/2D)contact surface CdS/α-Fe_(2)O_(3)(CF)heterojunction photocatalyst was synthesized via a simple solvothermal method.Photocatalytic hydrogen production experiments revealed that the CF-15 sample shows the optimal photocatalytic H_(2)rate(1806μmol·h^(-1)·g^(-1))and apparent quantum efficiency(AQE=13.7%atλ=420 nm).The enhancement of photocatalytic performance is mainly attributed to the contact of 0D/2D interface and the synergistic effect of z-scheme electron transfer mechanism.This work provides an effective way for modified composite semiconductor photocatalyst by constructing special interface heterojunction to achieve highly efficiently catalysis.

关键词： Photocatalysis Hydrogen production 0D/2D CdS α-Fe_(2)O_(3) z-scheme

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Highly ordered Janus CdS-Au-TiO_(2) z-scheme structure with high efficiency in photocatalysis

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Science China Chemistry 2023年第6期66卷 1722-1730页

作者： Ruixue Xiao Jie zhang Tingting Jiang Yefan zhou Yun Wang Wenjia Xu Yuhua Feng Institute of Advanced Synthesis School of Chemistry and Molecular EngineeringNanjing Tech UniversityNanjing 211816China School of Physical and Mathematical Science Nanjing Tech UniversityNanjing 211816China

Precise structural control had attracted tremendous interest in nanosynthesis due to its great importance in tailoring the physical properties of nanomaterials.Here we report the synthesis of highly ordered Cd S-Au-TiO_(2) ternary Janus structure via templateprotected sequential growth and conversion method.Arising from the integration of the rectification effect of Au-CdS and AuTiO_(2) Schottky barriers,the Janus configuration of the Cd S-TiO_(2) domains,the plasmonic effect of Au nanosphere,and the zscheme charge transportation,the Cd S-Au-TiO_(2) Janus structure showed high efficiency in the model photocatalytic degradation of methyl orange(MO)dye.Importantly,the well-defined structural order allowed the identification of the correlation between the structure and the catalytic performance.We believe that the synthetic control and the mechanism insights would help the design and synthesis of sophisticated nanostructures,and would eventually promote their applications in photocatalysis fields.

关键词： z-scheme photocatalysis Janus structure Schottky barrier plasmonic effect ternary hybrid

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Ternary Ni_(2)P/Bi_(2)MoO_(6)/g-C_(3)N_(4)composite with z-scheme electron transfer path for enhanced removal broad-spectrum antibiotics by the synergistic effect of adsorption and photocatalysis

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Chinese Journal of Chemical Engineering 2022年第4期35卷 157-168页

作者： Feng Guo zhihao Chen Xiliu Huang Longwen Cao Xiaofang Cheng Weilong Shi Lizhuang Chen School of Energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003China School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Material Science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China College of Chemistry Zhengzhou UniversityZhengzhou 450001China

Constructing the stable,low-cost,efficient,and highly adaptable visible light-driven photocatalyst to implement the synergistic effect of photocatalysis and adsorption has been excavated a promising strategy to deal with antibiotic pollution in water bodies.Herein,a novel 3 D ternary z-scheme heterojunction photocatalyst Ni_(2)P/Bi_(2)MoO_(6)/g-C_(3)N_(4)(Ni_(2)P/BMO/CN)was fabricated by a simple solvothermal method in which the broad spectrum antibiotics(mainly tetracyclines and supplemented by quinolones)were used as target pollution sources to evaluate its adsorption and photocatalytic performance.Notably,the zscheme composite significantly exhibit the enhancement for degradation efficiency of tetracycline and other antibiotic by using Ni_(2)P nanoparticles as electron conductor.Active species capture experiment and electron spin resonance(ESR)technology reveal the mechanism of z-scheme Ni_(2)P/BMO/CN photocatalytic reaction in detail.In addition,based on the identification of intermediates by liquid chromatography–mass spectroscopy(LC–MS),the possible photocatalytic degradation pathways of TC were proposed.

关键词： Ni_(2)P/Bi_(2)MoO_(6)/g-C_(3)N_(4) z-scheme Photocatalysis Adsorption

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Construction of TiO_(2)-covalent organic framework z-scheme hybrid through coordination bond for photocatalytic CO_(2) conversion

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Journal of Energy Chemistry 2022年第1期31卷 85-92,I0003页

作者： Lei Wang Guofang Huang Liang zhang Rui Lian Jingwei Huang Houde She Chunli Liu Qizhao Wang Key Laboratory of Eco-Environment-Related Polymer Materials Gansu International Scientific and Technological Cooperation Base of Water-Retention Chemical Functional MaterialsCollege of Chemistry and Chemical EngineeringNorthwest Normal UniversityLanzhou 730070GansuChina Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025HeilongjiangChina School of Environmental Science and Engineering Key Laboratory of Subsurface Hydrology and Ecological Effects in Arid Region of Ministry of EducationChang'an University.Xi'an 710054ShaanxiChina Department of Physics Oxide Research Centerand Memory and Catalyst Research CenterHankuk University of Foreign StudiesYongin 17035Republic of Korea

In this work,a covalent organic framework(COF),which is constructed by the building blocks of[5,10,15,20-tetrakis(4-aminophenyl)porphinato]copper(Ⅱ)(CuTAPP)and p-benzaldehyde,is employed to integrate with TiO_(2) for the purpose of establishing a z-scheme hybrid.Within the system,isonicotinic acid performs the role of a bridge that connects the two components through a coordination bond.Further photocatalytic application reveals the hybrid framework is able to catalyze CO_(2) conversion under simulated solar light,resulting in CO production rate of 50.5 μmol g^(-1)·h^(-1),about 9.9 and 24.5 times that of COF and pristine TiO_(2),respectively.The ameliorated catalytic performance owes much to the por-phyrin block acting as photosensitizer that augments the light absorbance,and the establishment of z-scheme system between the inorganic and orga nic comp on ents that enhances the separati on of the carriers.In addition,the chemical bridge also ensures a steady usage and stable charge delivery in the catalysis.Our study sheds light on the development of versatile approaches to covalently in corporate COFs with inorga nic semic on ductors.

关键词： CuP-Ph COF TiO_(2) Sensitization z-scheme CO_(2)reduction Photocatalysis

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