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| 1 | 2D/2D covalent organic framework/CdS Z-scheme heterojunction for enhanced photocatalytic H_(2) evolution:Insights into interfacial charge transfer mechanism显示文摘Covalent organic frameworks(COFs)with high crystallinity and flexible designability have been consid-ered as promising candidates for photocatalytic hydrogen evolution.However,the existence of unpropi-tious exciton effects in COFs leads to poor charge separation,and thus results in low photocatalytic effi-ciency.Herein,to improve the photoelectron migration efficiency,we designed a 2D/2D organic/inorganic direct Z-scheme COF-based heterojunction(TpTAP/CdS),by the in-situ growing of CdS nanosheets on the COF copolymerized via 2,4,6-tris(4-aminophenyl)-1,3,5-triazine(TAP)and 1,3,5-triformylphloroglucinol(Tp).The femtosecond transient absorption(fs-TA)decay kinetics of TpTAP-COF and TpTAP/CdS further reveal the processes of shallow electron trapping and the recombination of the free photogenerated electron-hole pairs.In particular,the transient absorption traces for TpTAP-COF and TpTAP/CdS normal-ized to the photoinduced absorption peak can effectively verify the Z-scheme charge transfer between TpTAP-COF and CdS,which could enhance the charge mobility and separation,thus reducing the pho-tocorrosion of CdS.Additionally,ultraviolet photoelectron spectroscopy(UPS),in-situ X-ray photoelec-tron spectroscopy(XPS),transient photovoltage measurements,and electron spin resonance(ESR)spec-troscopy further confirm the establishment of the internal electric field(IEF).This work demonstrates the important role of COFs in the construction of 2D/2D organic/inorganic direct Z-scheme heterojunctions and offers a new avenue to explain the criticality of dynamics of the photogenerated carriers for the construction of Z-scheme heterojunctions. | Ruiqi Gao Junxian Bai Rongchen Shen Lei Hao Can Huang Lei Wang Guijie Liang Peng Zhang Xin Li | 2023 | Journal of Materials Science & Technology2023，，6： | 1 |
| 2 | Regulating interfacial morphology and charge-carrier utilization of Ti_(3)C_(2)modified all-sulfide CdS/ZnIn_(2)S_(4)S-scheme heterojunctions for effective photocatalytic H_(2) evolution显示文摘The separation efficiency of electrons and holes and the enhancement of the surface reductive reaction in the metal sulfide semiconductor photocatalysts are important factors in boosting photocatalytic H_(2)evolution from water.The control of both interface morphology and the charge-carrier utilization of metal sulfide-based photocatalysts can effectively improve the separation efficiency of electrons and holes and increase the surface reaction active sites,which are considered to be effective methods to improve the photocatalytic activity of semiconductors.Here,the Ti_(3)C_(2)(Mxene)modified all-sulfide 2D/2D Sscheme heterojunction Ti_(3)C_(2)/Zn In_(2)S_(4)(ZIS)/CdS composite material was firstly synthesized by a two-step solvothermal method.The formation of all-sulfide S-scheme heterojunction improves the efficiency of electron-hole separation.The intimate 2D/2D van der Waals structure provides a strong interaction force and a large contact area to enhance charge transfer.The addition of 2D Ti_(3)C_(2)forms the accumulation layer,reducing the recombination of electrons and holes.Under the synergistic promotion,the highest hydrogen production of the prepared Ti_(3)C_(2)/ZIS/CdS composite photocatalyst could reach 8.93 mmol/h/g.This work not only enriches the photocatalytic systems through integrating the ohmic junction and the 2D/2D all-sulfide S-scheme heterojunction,but also provides a satisfactory design strategy for engineering interfacial morphology and charge-carrier utilization. | Junxian Bai Weilin Chen Rongchen Shen Zhimin Jiang Peng Zhang Wei Liu Xin Li | 2022 | Journal of Materials Science & Technology2022，，17： | 0 |
| 3 | Pyrene-benzothiadiazole-based Polymer/CdS 2D/2D Organic/Inorganic Hybrid S-scheme Heterojunction for Efficient Photocatalytic H_(2) Evolution显示文摘Nowadays,conjugated polymers have garnered numerous attention as a new class of organic photocatalysts due to their tunable electronic properties,low cost,excellent stability and sufficient light-absorption performance.In particular,pyrene-benzothiadiazole-based conjugated polymer(PBBP)has been considered to be a new type of conjugated polymers for photocatalytic H_(2)evolution.However,the poor charge separation seriously limits its practical application in H_(2)evolution.In this work,a PBBP-based polymer/CdS 2D/2D organic/inorganic S-scheme heterojunction photocatalyst with a strong internal electric field is,for the first time,prepared for efficient photo-catalytic hydrogen evolution.The pyrene-benzothiadiazole-based conjugated polymers(PBBP)are synthesized by the Suzuki-Miyaura reactions.Then,the hybrid heterojunction photocatalysts are fabricated by coupling CdS with it through the ultrasonic mixing method.As a result,the highest H_(2)-production rate of 15.83 mmolh^(-1)g^(-1)is achieved on 20%PBBP/CdS composite under visible-light irradiation,nearly 2.7 times higher than that of pure CdS.The apparent quantum efficiency(AQE)of 20%PBBP/CdS composite could reach 8.66%atλ=420 nm.The enhanced activity could be attributed to the construction of S-scheme heterojunction,which accelerates the recombination of carriers with weaker redox ability and maintains the strong reducibility of electrons in CdS.This work provides a protocol for pyrene-benzothiadiazole-based conjugated polymers to prepare S-scheme heterojunction photocatalysts based on organic/inorganic coupling. | Ruiqi Gao Huan He Junxian Bai Lei Hao Rongchen Shen Peng Zhang Youji Li Xin Li | 2022 | Chinese Journal of Structural Chemistry2022，41，6： | 0 |
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