Synergy of Ag and AgBr in a Pressurized Flow Reactor for Selective Photocatalytic Oxidative Coupling of Methane

被引:38
作者
Wang, Chao [1 ]
Li, Xiyi [1 ]
Ren, Yifei [1 ]
Jiao, Haimiao [1 ]
Wang, Feng Ryan [1 ]
Tang, Junwang [1 ,2 ]
机构
[1] UCL, Dept Chem Engn, London WC1E 7JE, England
[2] Tsinghua Univ, Ind Catalysis Ctr, Dept Chem Engn, Beijing 100084, Peoples R China
基金
英国工程与自然科学研究理事会;
关键词
oxidative coupling of methane; pressurized flow reactor; synergy of Ag and AgBr; ethane; photocatalysis; AMBIENT CONDITIONS; CONVERSION; SILVER; OXYGEN; O-2;
D O I
10.1021/acscatal.2c06093
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Oxidation of methane into valuable chemicals, such as C2+ molecules, has been long sought after but the dilemma between high yield and high selectivity of desired products remains. Herein, methane is upgraded through the photocatalytic oxidative coupling of methane (OCM) over a ternary Ag-AgBr/TiO2 catalyst in a pressurized flow reactor. The ethane yield of 35.4 mu mol/h with a high C2+ selectivity of 79% has been obtained under 6 bar pressure. These are much better than most of the previous benchmark performance in photocatalytic OCM processes. These results are attributed to the synergy between Ag and AgBr, where Ag serves as an electron acceptor and promotes the charge transfer and AgBr forms a heterostructure with TiO2 not only to facilitate charge separation but also to avoid the overoxidation process. This work thus demonstrates an efficient strategy for photocatalytic methane conversion by both the rational design of the catalyst for the high selectivity and reactor engineering for the high conversion.
引用
收藏
页码:3768 / 3774
页数:7
相关论文
共 38 条
[1]   Oxidation of Methane to Methanol with Hydrogen Peroxide Using Supported Gold-Palladium Alloy Nanoparticles [J].
Ab Rahim, Mohd Hasbi ;
Forde, Michael M. ;
Jenkins, Robert L. ;
Hammond, Ceri ;
He, Qian ;
Dimitratos, Nikolaos ;
Lopez-Sanchez, Jose Antonio ;
Carley, Albert F. ;
Taylor, Stuart H. ;
Willock, David J. ;
Murphy, Damien M. ;
Kiely, Christopher J. ;
Hutchings, Graham J. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2013, 52 (04) :1280-1284
[2]   Photocatalytic oxidation of methane over silver decorated zinc oxide nanocatalysts [J].
Chen, Xuxing ;
Li, Yunpeng ;
Pan, Xiaoyang ;
Cortie, David ;
Huang, Xintang ;
Yi, Zhiguo .
NATURE COMMUNICATIONS, 2016, 7
[3]   Spontaneous Bulk-Surface Charge Separation of TiO2-{001} Nanocrystals Leads to High Activity in Photocatalytic Methane Combustion [J].
Fu, Cong ;
Li, Fei ;
Yang, Jianlong ;
Xie, Jijia ;
Zhang, Yunshang ;
Sun, Xiao ;
Zheng, Xusheng ;
Liu, Yuanxu ;
Zhu, Junfa ;
Tang, Junwang ;
Gong, Xue-Qing ;
Huang, Weixin .
ACS CATALYSIS, 2022, 12 (11) :6457-6463
[4]   Direct, Nonoxidative Conversion of Methane to Ethylene, Aromatics, and Hydrogen [J].
Guo, Xiaoguang ;
Fang, Guangzong ;
Li, Gang ;
Ma, Hao ;
Fan, Hongjun ;
Yu, Liang ;
Ma, Chao ;
Wu, Xing ;
Deng, Dehui ;
Wei, Mingming ;
Tan, Dali ;
Si, Rui ;
Zhang, Shuo ;
Li, Jianqi ;
Sun, Litao ;
Tang, Zichao ;
Pan, Xiulian ;
Bao, Xinhe .
SCIENCE, 2014, 344 (6184) :616-619
[5]   Major routes in the photocatalytic methane conversion into chemicals and fuels under mild conditions [J].
Hu, Di ;
Ordomsky, Vitaly V. ;
Khodakov, Andrei Y. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2021, 286
[6]   OXIDATIVE COUPLING OF METHANE USING OXIDE CATALYSTS [J].
HUTCHINGS, GJ ;
SCURRELL, MS ;
WOODHOUSE, JR .
CHEMICAL SOCIETY REVIEWS, 1989, 18 (03) :251-283
[7]   Pd-Modified ZnO-Au Enabling Alkoxy Intermediates Formation and Dehydrogenation for Photocatalytic Conversion of Methane to Ethylene [J].
Jiang, Wenbin ;
Low, Jingxiang ;
Mao, Keke ;
Duan, Delong ;
Chen, Shuangming ;
Liu, Wei ;
Pao, Chih-Wen ;
Ma, Jun ;
Sang, Shuaikang ;
Shu, Chang ;
Zhan, Xiaoyi ;
Qi, Zeming ;
Zhang, Hui ;
Liu, Zhi ;
Wu, Xiaojun ;
Long, Ran ;
Song, Li ;
Xiong, Yujie .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2021, 143 (01) :269-278
[8]   Highly efficient visible-light driven AgBr/Ag3PO4 hybrid photocatalysts with enhanced photocatalytic activity [J].
Katsumata, Hideyuki ;
Hayashi, Takahiro ;
Taniguchi, Masanao ;
Suzuki, Tohru ;
Kaneco, Satoshi .
MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING, 2014, 25 :68-75
[9]   Highly efficient light-driven methane coupling under ambient conditions based on an integrated design of a photocatalytic system [J].
Lang, Junyu ;
Ma, Yuli ;
Wu, Xuechen ;
Jiang, Yueyue ;
Hu, Yun Hang .
GREEN CHEMISTRY, 2020, 22 (14) :4669-4675
[10]   RELATIVE CONTRIBUTIONS OF GREENHOUSE GAS EMISSIONS TO GLOBAL WARMING [J].
LASHOF, DA ;
AHUJA, DR .
NATURE, 1990, 344 (6266) :529-531