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DOI10.1021/jacs.8b13552
Room Temperature Methane Capture and Activation by Ni Clusters Supported on TiC(001): Effects of Metal-Carbide Interactions on the Cleavage of the C-H Bond
Prats, Hector1,2; Gutierrez, Ramon A.3,4; Jose Pinero, Juan1,2; Vines, Francesc1,2; Bromley, Stefan T.1,2,5; Ramirez, Pedro J.4; Rodriguez, Jose A.3; Illas, Francesc1,2
发表日期2019
ISSN0002-7863
卷号141期号:13页码:5303-5313
英文摘要

Methane is an extremely stable molecule, a major component of natural gas, and also one of the most potent greenhouse gases contributing to global warming. Consequently, the capture and activation of methane is a challenging and intensively studied topic. A major research goal is to find systems that can activate methane, even at low temperatures. Here, combining ultrahigh vacuum catalytic experiments, X-ray photoemission spectra, and accurate density functional theory (DFT) based calculations, we show that small Ni clusters dispersed on the (001) surface of TiC are able to capture and dissociate methane at room temperature. Our DFT calculations reveal that two-dimensional Ni clusters are responsible for this chemical transformation, confirming that the lability of the supported clusters appears to be a critical aspect in the strong adsorption of methane. A small energy barrier of 0.18 eV is predicted for CH4 dissociation into adsorbed methyl and atomic hydrogen species. In addition, the calculated reaction free energy profile at 300 K and 1 atm of CH4 shows no effective energy barriers in the system. Comparison with other reported systems which activate methane at room temperature, including oxide and zeolite-based materials, indicates that a different chemistry takes place on our metal/carbide system. The discovery of a carbide-based surface able to activate methane at low temperatures paves the road for the design of new types of catalysts which can efficiently convert this hydrocarbon into other added-value chemicals, with implications in climate change mitigation.


WOS研究方向Chemistry
来源期刊JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/96306
作者单位1.Univ Barcelona, Dept Ciencia Mat & Quim Fis, Marti i Franques 1-11, E-08028 Barcelona, Spain;
2.Univ Barcelona, Inst Quim Teor & Computac IQTCUB, Marti i Franques 1-11, E-08028 Barcelona, Spain;
3.Brookhaven Natl Lab, Chem Dept, Upton, NY 11973 USA;
4.Univ Cent Venezuela, Fac Ciencias, Caracas 1020A, Venezuela;
5.ICREA, Barcelona 08010, Spain
推荐引用方式
GB/T 7714
Prats, Hector,Gutierrez, Ramon A.,Jose Pinero, Juan,et al. Room Temperature Methane Capture and Activation by Ni Clusters Supported on TiC(001): Effects of Metal-Carbide Interactions on the Cleavage of the C-H Bond[J],2019,141(13):5303-5313.
APA Prats, Hector.,Gutierrez, Ramon A..,Jose Pinero, Juan.,Vines, Francesc.,Bromley, Stefan T..,...&Illas, Francesc.(2019).Room Temperature Methane Capture and Activation by Ni Clusters Supported on TiC(001): Effects of Metal-Carbide Interactions on the Cleavage of the C-H Bond.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(13),5303-5313.
MLA Prats, Hector,et al."Room Temperature Methane Capture and Activation by Ni Clusters Supported on TiC(001): Effects of Metal-Carbide Interactions on the Cleavage of the C-H Bond".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.13(2019):5303-5313.
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