摘要
石墨炔由于其高载流子迁移率和有序的孔隙结构被认为是一种很有应用前景的光催化材料.本研究通过交叉偶联合成了一种新型球状石墨炔,并与棒状Mn_(0.2)Cd_(0.8)S耦合构建了S型异质结用于光催化析氢.结果表明,Mn_(0.2)Cd_(0.8)S/石墨炔异质结光催化剂表现出优异的光催化活性,产氢性能分别较Mn_(0.2)Cd_(0.8)S和球形石墨炔单体催化剂提升了16.78和613.2倍.同时,该催化剂应用于平米级规模产氢取得较好效果.其优异的光催化活性可归因于石墨炔的独特性能及S-scheme异质结的有效构建.通过紫外光电子能谱、原位辐射X射线光电子能谱、电子顺磁共振能谱、密度泛函理论计算和其他表征技术探究了S-scheme异质结的形成和光催化活性的增强.该工作可为石墨炔的形貌可调性制备以及高效异质结光催化剂的设计和合成提供新参考.
Graphdiyne is a promising photocatalytic material for solar energy conversion because of its high carrier mobility and ordered pore structure.In this work,a novel spherical graphdiyne(S-GDY)was prepared by crosscoupling and cleverly coupled with rod-like Mn_(0.2)Cd_(0.8)S to form an Sscheme heterojunction for photocatalytic hydrogen evolution,which is applied for the first time in this field.As anticipated,the Mn_(0.2)Cd_(0.8)S/S-GDY heterojunction photocatalyst showed remarkable photocatalytic activity,exceeding the individual catalysts Mn_(0.2)Cd_(0.8)S and S-GDY by factors of 16.78 and 613.2,respectively.Moreover,it was successfully applied to hydrogen production on the square meter scale.The exceptional photocatalytic activity can be ascribed to the introduction of the unique morphology of graphdiyne and the formation of the Sscheme heterojunction.The formation of the S-scheme heterojunction and improvement of photocatalytic activity were revealed by ultraviolet photoelectron spectroscopy,in-situ irradiation X-ray photoelectron spectroscopy,density functional theory calculations,electron paramagnetic resonance,and other basic characterization methods.This work offers insights into the preparation of morphologically tunable graphdiyne and the design and synthesis of efficient heterojunction photocatalysts.
作者
杨成
李小红
靳治良
Cheng Yang;Xiaohong Li;Zhiliang Jin(School of Chemistry and Chemical Engineering,Ningxia Key Laboratory of Solar Chemical Conversion Technology,Key Laboratory for Chemical Engineering and Technology,State Ethnic Affairs Commission,North Minzu University,Yinchuan 750021,China)
基金
supported by the Natural Science Foundation of the Ningxia Hui Autonomous Region(2023AAC02046)。
作者简介
Cheng Yang is currently pursuing an MS in Jin Zhiliang’s research group at the School of Chemistry and Chemical Engineering,North Minzu University.His research focuses on the construction of semiconductor heterojunction photocatalysts and their application in photocatalytic hydrogen production;Xiaohong Li is currently pursuing an MS in Jin Zhiliang’s research group at the School of Chemistry and Chemical Engineering,North Minzu University.Her research focuses on the preparation of photocatalysts and their application in photocatalytic hydrogen production;Corresponding author:Zhiliang Jin received his PhD in 2006 from Lanzhou Institute of Chemical Physics,Chinese Academy of Sciences.From 2006 to 2014,he worked at the State Key Laboratory of Carbonyl Synthesis and Selective Oxidation,Lanzhou Institute of Chemical Physics,Chinese Academy of Sciences.He is currently a professor at the North Minzu University for nationalities.He is mainly engaged in the research on clean energy(photocatalytic hydrogen production),environmental chemical industry(catalytic elimination of environmental pollutants),and cultural heritage protection.email:zl-jin@nun.edu.cn。
