Novel carbon-nitride based catalysts for enhanced CH_(4) reforming under visible light: From morphology to heterojunction design principles
作者机构：Joint International Center for CO_(2)Capture and Storage(iCCS)The Engineering Research Center of Advanced CatalysisMinistry of Education ProvincialHunan Key Laboratory for Cost-effective Utilization of Fossil Fuel Aimed at Reducing CO_(2)EmissionsCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082HunanChina
出 版 物：《能源化学:英文版》 (Journal of Energy Chemistry)
年 卷 期：2023年第83卷第8期
页 面：423-432,I0011页
核心收录：
学科分类：0830[工学-环境科学与工程（可授工学、理学、农学学位）] 0201[经济学-理论经济学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 0703[理学-化学] 0702[理学-物理学]
基 金：The financial support from the National Natural Science Foundation of China (22178089) the Hunan Provincial Innovation Foundation for Postgraduate (CX20220392)。
主 题：Photocatalytic CO_(2) CH_(4) 2D/2DTiO_(2)/g-C_(3)N_(4) Conversion
摘 要：The synthesis of high value-added chemical products using CO_(2)and CH_(4)is a promising CO_(2)conversion technology that can reduce greenhouse gas emissions while also alleviating the energy crisis.However,problems such as high energy consumption and strict reaction conditions in reforming process hinder the further development of the technology.In this work,carbon-nitrogen based composites were prepared for the first time according to the design principle from morphology to heterojunction,which is innovatively applied in the process of photocatalytic CH4reforming.Firstly,C_(3)N_(4)materials with different dimensions(D) are prepared and applied to a CO_(2)-CH_(4)photocatalytic system.Additionally,the 2D/2D TiO_(2)/g-C_(3)N_(4)heterostructure is constructed with the ultrasonic impregnation method to further improve charge generation,transfer,and separation efficiency.It is worth noting that the yield of CO reaches173.80 μmol g^(-1),and the catalytic performance is improved by 1546% compared to bulk C_(3)N_(4).Moreover,the physical and chemical properties of 2D/2D TiO_(2)/g-C_(3)N_(4)materials are studied using a variety of cha racterization methods.Furthermore,the work fu nction and adsorption energy of different C3N4/TiO_(2)models for CO_(2)adsorption are calculated by density functional theory(DFT).Then,a possible catalytic mechanism for photocatalytic CO_(2)and CH_(4) conversion is proposed based on DFT calculations and experimental results.This work provides a new technical route for the rapid conversion of CO_(2)and CH_(4) at room temperature,as well as a new research concept for achieving carbon neutrality.
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