Tin-Assisted Fully Exposed Platinum Clusters Stabilized on Defect-Rich Graphene for Dehydrogenation Reaction

被引:179
作者
Zhang, Jiayun [1 ,2 ]
Deng, Yuchen [3 ,4 ,5 ]
Cai, Xiangbin [6 ,7 ]
Chen, Yunlei [8 ,9 ]
Peng, Mi [3 ,4 ,5 ]
Jia, Zhimin [1 ,2 ]
Jiang, Zheng [10 ]
Ren, Pengju [8 ,9 ]
Yao, Siyu [3 ,4 ,5 ]
Xie, Jinglin [3 ,4 ,5 ]
Xiao, Dequan [11 ]
Wen, Xiaodong [8 ,9 ]
Wang, Ning [6 ,7 ]
Liu, Hongyang [1 ,2 ]
Ma, Ding [3 ,4 ,5 ]
机构
[1] Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Liaoning, Peoples R China
[2] Univ Sci & Technol China, Sch Mat Sci & Engn, Hefei 230026, Anhui, Peoples R China
[3] Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
[4] Peking Univ, Coll Engn, Beijing 100871, Peoples R China
[5] Peking Univ, BIC ESAT, Beijing 100871, Peoples R China
[6] Hong Kong Univ Sci & Technol, Dept Phys, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
[7] Hong Kong Univ Sci & Technol, Ctr Quantum Mat, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
[8] Chinese Acad Sci, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Shanxi, Peoples R China
[9] Univ Chinese Acad Sci, 19A Yuanquan Rd, Beijing 100049, Peoples R China
[10] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China
[11] Univ New Haven, Dept Chem & Chem Engn, Ctr Integrat Mat Discovery, 300 Boston Post Rd, West Haven, CT 06516 USA
关键词
atomic dispersion; defect-rich graphene; Pt nanocluster; dehydrogenation; heterogeneous catalysis; TOTAL-ENERGY CALCULATIONS; CATALYSTS; ADSORPTION; METALS; WATER; MOC;
D O I
10.1021/acscatal.9b00601
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
Tin-assisted fully exposed Pt clusters are fabricated on the core-shell nanodiamond@graphene (ND@G) hybrid support (a-PtSn/ND@G). The obtained atomically dispersed Pt clusters, with an average Pt atom number of 3, were anchored over the ND@G support by the assistance of Sn atoms as a partition agent and through the Pt-C bond between Pt clusters and defect-rich graphene nanoshell. The atomically dispersed Pt clusters guaranteed a full metal availability to the reactants, a high thermal stability, and an optimized adsorption/desorption behavior. It inhibits the side reactions and enhances catalytic performance in direct dehydrogenation of n-butane at a low temperature of 450 degrees C, leading to >98% selectivity toward olefin products, and the turnover frequency (TOF) of a-PtSn/ND@G is similar to 3.9 times higher than that of the traditional Pt3Sn alloy catalyst supported on Al2O3 (Pt3Sn/Al2O3).
引用
收藏
页码:5998 / 6005
页数:15
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