多孔石墨烯用作丁烷氧化脱氢催化剂  

Oxidative Dehydrogenation of Butane Catalyzed by Porous Graphene

作　　者：宁国庆[1] 唐晓丽 Ning Guoqing;Tang Xiaoli(State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Beijing 102249,China;Research Institute of Safety Engineering,SINOPEC,Qingdao 266071,China)

机构地区：[1]中国石油大学(北京)重质油国家重点实验室,北京102249 [2]中国石油化工股份有限公司青岛安全工程研究院,山东青岛266071

出　　处：《山东化工》2019年第24期1-4,6,共5页Shandong Chemical Industry

基　　金：国家自然科学基金青年基金项目(No.21206191)资助

摘　　要：碳材料作为丁烷氧化脱氢催化剂具有活性高、氧化深度可控的优点,具有高比表面积、丰富缺陷结构的多孔石墨烯是碳材料催化剂的理想选择。本文首次将化学气相沉积(CVD)法制备的多孔石墨烯作为催化剂应用于正丁烷氧化脱氢反应过程中。结果表明,多孔石墨烯对正丁烷氧化脱氢反应表现出显著催化活性,相对于碳纳米管,采用多孔石墨烯作为催化剂得到了更高的正丁烷转化率与C4烯烃选择性。当反应温度小于550℃时,C4烯烃的选择性较高(>40%);在550℃时,C4烯烃的收率达到最大值21.1%。在7.5 h的稳定性考察中,多孔石墨烯保持了良好的催化稳定性。反应后多孔石墨烯的表面缺陷度及C=O含量下降,这说明多孔石墨烯表面的C=O键是催化正丁烷氧化脱氢反应的活性中心。Carbon materials have exhibited high catalytic activity for oxidative dehydrogenation(ODH) of n-butane.Porous graphene is expected to be an ideal catalyst for the ODH process because of its high specific surface area and containing plenty of defects.Here,porous graphene prepared by a chemical vapor deposition is applied for the first time to catalyze the ODH of n-butane.Compared to carbon nanotubes,porous graphene shows better catalytic performance for the ODH of n-butane,including higher conversion of n-butane and C4 alkenes yield.The C4 alkenes selectivity is higher than 40% when the temperature is below 550 ℃,and the highest C4 alkenes yield of 21.1 % is obtained at 550 ℃.The porous graphene exhibits good catalytical stability in a 7.5 h continuous reaction.Raman and XPS characterization for the fresh and used graphene shows that the surface defects and the amount of C=O decrease.Thus we spectulated that C=O is the active sites to catalyze the ODH reaction.

关 键 词：氧化脱氢 石墨烯 催化剂 丁烷 

分 类 号：O643.3[理学—物理化学]