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porous heterostructure of graphene/hexagonal boron nitride as an efficient electrocatalyst for hydrogen peroxide generation

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Carbon Energy 2023年第5期5卷 138-151页

作者： Mengmeng Fan Zeming Wang Yuying Zhao Qixin Yuan Jian Cui Jithu Raj Kang Sun Ao Wang Jingjie Wu Hao Sun Bei Li Liang Wang Jianchun Jiang Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjingChina Key Lab of Biomass Energy and Material Jiangsu ProvinceJiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest ResourcesInstitute of Chemical Industry of Forest ProductsChinese Academy of ForestryNanjingChina School of Environmental and Chemical Engineering Institute of Nanochemistry and NanobiologyShanghai UniversityShanghaiChina Chemicobiology and Functional Materials Institute Nanjing University of Science and TechnologyNanjingChina Department of Chemical and Environmental Engineering University of CincinnatiCincinnatiOhioUSA

Compared with the traditional heteroatom doping,employing heterostructure is a new modulating approach for carbon-based electrocatalysts.Herein,a facile ball milling-assisted route is proposed to synthesize porous carbon materials composed of abundant graphene/hexagonal boron nitride(G/h-BN)heterostructures.Metal Ni powder and nanoscale h-BN sheets are used as a catalytic substrate/hard template and“nucleation seed”for the formation of the heterostructure,respectively.As-prepared G/h-BN heterostructures exhibit enhanced electrocatalytic activity toward H_(2)O_(2) generation with 86%-95%selectivity at the range of 0.45-0.75 V versus reversible hydrogen electrode(RHE)and a positive onset potential of 0.79 versus RHE(defined at a ring current density of 0.3 mA cm^(-2))in the alkaline solution.In a flow cell,G/h-BN heterostructured electrocatalyst has a H_(2)O_(2) production rate of up to 762 mmol g_(catalyst)^(-1) h^(-1) and Faradaic efficiency of over 75%during 12 h testing,superior to the reported carbon-based electrocatalysts.The density functional theory simulation suggests that the B atoms at the interface of the G/h-BN heterostructure are the key active sites.This research provides a new route to activate carbon catalysts toward highly active and selective O_(2)-to-H_(2)O_(2) conversion.

关键词： efficient electrocatalyst graphene H_(2)O_(2)generation hexagonal boron nitride porous heterostructure

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Novel Ag-bridged dual Z-scheme g-C_(3)N_(4)/BiOI/AgI plasmonic heterojunction: Exceptional photocatalytic activity towards tetracycline and the mechanism insight

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Journal of Environmental Sciences 2023年第9期131卷 123-140页

作者： Wenxia Wang Zhen Li Kailin Wu Guodong Dai Qingping Chen Lihua Zhou Junxia Zheng Liang Ma Guiying Li Wanjun Wang Taicheng An School of Biomedical and Pharmaceutical Sciences Guangdong University of TechnologyGuangzhou 510006China Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and HealthInstitute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Guangzhou Key lab of Clean Transport Energy and Chemistry Guangdong University of TechnologyGuangzhou 510006China Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control Guangdong Technology Research Center for Photocatalytic Technology Integration and Equipment EngineeringSchool of Environmental Science and EngineeringGuangdong University of TechnologyGuangzhou 510006China

Rational design and synthesis of highly efficient and robust photocatalysts with positive exciton splitting and interfacial charge transfer for environmental applications is critical.Herein,aiming at overcoming the common shortcomings of traditional photocatalysts such as weak photoresponsivity,rapid combination of photo-generated carriers and unstable structure,a novel Ag-bridged dual Z-scheme g-C_(3)N_(4)/BiOI/AgI plasmonic heterojunction was successfully synthesized using a facile method.Results showed that Ag-AgI nanoparticles and three-dimensional(3D)BiOI microspheres were decorated highly uniformly on the 3D porous g-C_(3)N_(4) nanosheet,resulting in a higher specific surface area and abundant active sites.The optimized 3D porous dual Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI manifested exceptional photocatalytic degradation efficiency of tetracycline(TC)in water with approximately 91.8%degradation efficiency within 165 min,outperforming majority of the reported g-C_(3)N_(4)-based photocatalysts.Moreover,g-C_(3)N_(4)/BiOI/Ag-AgI exhibited good stability in terms of activity and structure.In-depth radical scavenging and electron paramagnetic resonance(EPR)analyses confirmed the relative contributions of various scavengers.Mechanism analysis indicated that the improved photocatalytic performance and stability were ascribed to the highly ordered 3D porous framework,fast electron transfer of dual Z-scheme heterojunction,desirable photocatalytic performance of BiOI/AgI and synergistic effect of Ag plasmas.Therefore,the 3D porous Z-scheme g-C_(3)N_(4)/BiOI/Ag-AgI heterojunction had a good prospect for applications in water remediation.The current work provides new insight and useful guidance for designing novel structural photocatalysts for environment-related applications.

关键词： Three-dimensional porous heterostructure Graphitic carbon nitride(g-C_(3)N_(4)) Dual Z-scheme heterojunction Tetracycline(TC)degradation Mechanism insight

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