Ti3C2Tx MXene Catalyzed Ethylbenzene Dehydrogenation: Active Sites and Mechanism Exploration from both Experimental and Theoretical Aspects

被引：95

作者：

Diao, Jiangyong ^{[1
]}

Hu, Minmin ^{[1
,2
]}

Lian, Zan ^{[1
,2
]}

Li, Zhaojin ^{[1
]}

Zhang, Hui ^{[1
]}

Huang, Fei ^{[1
,2
]}

Li, Bo ^{[1
]}

Wang, Xiaohui ^{[1
]}

Su, Dang Sheng ^{[1
]}

Liu, Hongyang ^{[1
]}

机构：

[1] Chinese Acad Sci, Shenyang Natl Lab Mat Sci, Inst Met Res, 72 Wenhua Rd, Shenyang 110016, Liaoning, Peoples R China

[2] Univ Sci & Technol China, Sch Mat Sci & Engn, 96 Jinzhai Rd, Hefei 230026, Anhui, Peoples R China

来源：

ACS CATALYSIS | 2018年 / 8卷 / 11期

基金：

中国国家自然科学基金;

关键词：

MXene; direct dehydrogenation; ethylbenzene; styrene; heterogeneous catalysis; TRANSITION-METAL CARBIDES; OXIDATIVE DEHYDROGENATION; STABLE CATALYSTS; N-BUTANE; STYRENE; PERFORMANCE; TI3ALC2; DEACTIVATION; FABRICATION; ELECTRODES;

D O I：

10.1021/acscatal.8b02002

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：

Two-dimensional materials (such as graphene, MXenes) usually perform remarkably well as catalysts in comparison with their three-dimensional counterparts. In this work, Ti3AlC2-derived Ti3C2Tx MXene (T = O, OH, F) was prepared and employed in the direct dehydrogenation of ethylbenzene. A 92 mu mol m(-2) h(-1) reactivity and a 40 h stability with almost no deactivation were observed, which is much better than those of the previously reported nanocarbon catalysts. The graphene-like layered structure and the C-Ti-O termination groups induced by the preparation process were thought to account for the good catalytic performance of Ti3C2Tx MXene from both experimental and computational perspectives. The discovery expands the application of two-dimensional MXenes and provides more choices in exploring high activity catalysts for hydrocarbon dehydrogenation reactions.

引用

页码：10051 / 10057

页数：13

共 41 条

[1] Key aspects of catalyst design for the selective oxidation of paraffins [J].

Albonetti, S ;

Cavani, F ;

Trifiro, F .

CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1996, 38 (04) :413-438

[2] N-Doped Food-Grade-Derived 3D Mesoporous Foams as Metal-Free Systems for Catalysis [J].

Ba, Housseinou ;

Liu, Yuefeng ;

Lai Truong-Phuoc ;

Cuong Duong-Viet ;

Nhut, Jean -Mario ;

Dinh Lam Nguyen ;

Ersen, Ovidiu ;

Tuci, Giulia ;

Giambastiani, Giuliano ;

Cuong Pham-Huu .

ACS CATALYSIS, 2016, 6 (03) :1408-1419

[3] Onion-Like Graphene Carbon Nanospheres as Stable Catalysts for Carbon Monoxide and Methane Chlorination [J].

Centi, Gabriele ;

Barbera, Katia ;

Perathoner, Siglinda ;

Gupta, Navneet K. ;

Ember, Erika E. ;

Lercher, Johannes A. .

CHEMCATCHEM, 2015, 7 (18) :3036-3046

[4] Immobilized carbon nanofibers as industrial catalyst for ODH reactions [J].

Delgado, J. J. ;

Su, D. S. ;

Rebmann, G. ;

Keller, N. ;

Gajovic, A. ;

Schloegl, R. .

JOURNAL OF CATALYSIS, 2006, 244 (01) :126-129

[5]

Deng DH, 2016, NAT NANOTECHNOL, V11, P218, DOI [10.1038/nnano.2015.340, 10.1038/NNANO.2015.340]

[6] Fabrication of MgO-rGO hybrid catalysts with a sandwich structure for enhanced ethylbenzene dehydrogenation performance [J].

Diao, Jiangyong ;

Zhang, Yajie ;

Zhang, Jiayun ;

Wang, Jia ;

Liu, Hongyang ;

Su, Dang Sheng .

CHEMICAL COMMUNICATIONS, 2017, 53 (82) :11322-11325

[7] Selective and Stable Ethylbenzene Dehydrogenation to Styrene over Nanodiamonds under Oxygen-lean Conditions [J].

Diao, Jiangyong ;

Feng, Zhenbao ;

Huang, Rui ;

Liu, Hongyang ;

Abd Hamid, Sharifah Bee ;

Su, Dang Sheng .

CHEMSUSCHEM, 2016, 9 (07) :662-666

[8] Highly dispersed nanodiamonds supported on few-layer graphene as robust metal-free catalysts for ethylbenzene dehydrogenation reaction [J].

Diao, Jiangyong ;

Liu, Hongyang ;

Feng, Zhenbao ;

Zhang, Yajie ;

Chen, Tong ;

Miao, Changxi ;

Yang, Weimin ;

Su, Dang Sheng .

CATALYSIS SCIENCE & TECHNOLOGY, 2015, 5 (11) :4950-4953

[9] Porous graphene-based material as an efficient metal free catalyst for the oxidative dehydrogenation of ethylbenzene to styrene [J].

Diao, Jiangyong ;

Liu, Hongyang ;

Wang, Jia ;

Feng, Zhenbao ;

Chen, Tong ;

Miao, Changxi ;

Yang, Weimin ;

Su, Dang Sheng .

CHEMICAL COMMUNICATIONS, 2015, 51 (16) :3423-3425

[10] Mesoporous and Graphitic Carbide-Derived Carbons as Selective and Stable Catalysts for the Dehydrogenation Reaction [J].

Glaesel, Jan ;

Diao, Jiangyong ;

Feng, Zhenbao ;

Hilgart, Markus ;

Wolker, Thomas ;

Su, Dang Sheng ;

Etzold, Bastian J. M. .

CHEMISTRY OF MATERIALS, 2015, 27 (16) :5719-5725

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