Activating and Converting CH4 to CH3OH via the CuPdO2/CuO Nanointerface

被引：71

作者：

Bai, Shuxing ^{[1
]}

Xu, Yong ^{[2
]}

Wang, Pengtang ^{[1
]}

Shao, Qi ^{[1
]}

Huan, Xiaoqing ^{[1
]}

机构：

[1] Soochow Univ, Coll Chem Chem Engn & Mat Sci, Suzhou 215123, Jiangsu, Peoples R China

[2] Soochow Univ, Inst Funct Nano & Soft Mat FUNSOM, Jiangsu Key Lab Carbon Based Funct Mat & Devices, Suzhou 215123, Jiangsu, Peoples R China

来源：

ACS CATALYSIS | 2019年 / 9卷 / 08期

基金：

中国国家自然科学基金;

关键词：

CuPdO2; CuO; interface; methane conversion; methanol; RAY PHOTOELECTRON-SPECTROSCOPY; CATALYTIC-OXIDATION; METHANE; CONVERSION; MILD; NANOPARTICLES; ACETALDEHYDE;

D O I：

10.1021/acscatal.9b00714

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：

The activation and conversion of methane (CH4) is one of the most challenging processes, because of the high chemical inertness of CH4 and the subsequent uncontrollable overoxidation. Herein, we report that the CuPdO2/CuO interface in PdxCu1-xO/C can efficiently activate and convert CH4 to CH3OH using H2O2 or O-2 as the oxidant under mild conditions, where the CH3OH yield (4076.5 mu mol g(-1)) and selectivity (93.9%) of the optimized Pd0.3Cu0.7O/C are much higher than those of PdO/C, CuPdO2/C, and the mixture of CuPdO2/C and CuO/C. Structural characterizations and mechanism studies reveal that the highly activity of Pd0.3Cu0.7O/C is attributed to the strong synergistic effects in PdxCu1-xO/C. The formation of Pd4+ species at the interfaces of CuPdO2 and CuO, which is promoted by the electron transfer from Cu to Pd, can selectively oxidize CH4 to produce CH3OH. This work highlights the importance of controlled interface in Pd-based catalysts for heterogeneous catalysis and beyond.

引用

页码：6938 / 6944

页数：13

共 39 条

[1] Aqueous Au-Pd colloids catalyze selective CH4 oxidation to CH3OH with O2 under mild conditions [J].

Agarwal, Nishtha ;

Freakley, Simon J. ;

McVicker, Rebecca U. ;

Althahban, Sultan M. ;

Dimitratos, Nikolaos ;

He, Qian ;

Morgan, David J. ;

Jenkins, Robert L. ;

Willock, David J. ;

Taylor, Stuart H. ;

Kiely, Christopher J. ;

Hutchings, Graham J. .

SCIENCE, 2017, 358 (6360) :223-226

[2] Toward Enhanced Photocatalytic Oxygen Evolution: Synergetic Utilization of Plasmonic Effect and Schottky Junction via Interfacing Facet Selection [J].

Bai, Song ;

Li, Xiyu ;

Kong, Qiao ;

Long, Ran ;

Wang, Chengming ;

Jiang, Jun ;

Xiong, Yujie .

ADVANCED MATERIALS, 2015, 27 (22) :3444-3452

[3] Mild, aqueous, aerobic, catalytic oxidation of methane to methanol and acetaldehyde catalyzed by a supported bipyrimidinylplatinum-polyoxometalate hybrid compound [J].

Bar-Nahum, I ;

Khenkin, AM ;

Neumann, R .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (33) :10236-10237

[4] Silica-Supported Au-CuOx Hybrid Nanocrystals as Active and Selective Catalysts for the Formation of Acetaldehyde from the Oxidation of Ethanol [J].

Bauer, J. Chris ;

Veith, Gabriel M. ;

Allard, Lawrence F. ;

Oyola, Yatsandra ;

Overbury, Steve H. ;

Dai, Sheng .

ACS CATALYSIS, 2012, 2 (12) :2537-2546

[5] Facile Dehydrogenation of Ethane on the IrO2(110) Surface [J].

Bian, Yingxue ;

Kim, Minkyu ;

Li, Tao ;

Asthagiri, Aravind ;

Weaver, Jason F. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2018, 140 (07) :2665-2672

[6] 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

[7] Unoccupied states and charge transfer in Cu-Pd alloys studied by bremsstrahlung isochromat spectroscopy, x-ray photoelectron spectroscopy, and L(III) absorption spectroscopy [J].

Cho, EJ ;

Lee, S ;

Oh, SJ ;

Han, M ;

Lee, YS ;

Whang, CN .

PHYSICAL REVIEW B, 1995, 52 (23) :16443-16450

[8] Characterization of Copper Palladium Oxide Solid Solutions by X-ray Diffraction, X-ray Photoelectron Spectroscopy, and Auger Electron Spectroscopy [J].

Christensen, Gregory L. ;

Langell, Marjorie A. .

JOURNAL OF PHYSICAL CHEMISTRY C, 2013, 117 (14) :7039-7049

[9] ASPECTS OF METHANE CHEMISTRY [J].

CRABTREE, RH .

CHEMICAL REVIEWS, 1995, 95 (04) :987-1007

[10] Synergistic Effects in Bimetallic Palladium-Copper Catalysts Improve Selectivity in Oxygenate Coupling Reactions [J].

Goulas, Konstantinos A. ;

Sreekumar, Sanil ;

Song, Yuying ;

Kharidehal, Purnima ;

Gunbas, Gorkem ;

Dietrich, Paul J. ;

Johnson, Gregory R. ;

Wang, Y. C. ;

Grippo, Adam M. ;

Grabow, Lars C. ;

Gokhale, Amit A. ;

Toste, F. Dean .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2016, 138 (21) :6805-6812

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