Enhanced Activity in Methane Dry Reforming by Carbon Dioxide Induced Metal‐Oxide Interface Restructuring of Nickel/Zirconia

Enhanced Activity in Methane Dry Reforming by Carbon Dioxide Induced Metal‐Oxide Interface Restructuring of Nickel/Zirconia
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通过二氧化碳诱导镍/氧化锆金属氧化物界面重构增强甲烷干重整活性

DOI:
10.1002/cctc.201700686
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发表时间:
2017
期刊:
影响因子:
4.5
通讯作者:
J. A. Lercher
J. A. Lercher
中科院分区:
化学3区
文献类型:
--
作者:
Y. Lou;M. Steib;A. Jentys;J. A. Lercher

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在CO2存在下对Ni/ZrO 2催化剂进行活化和再生,可显著提高催化剂的甲烷干重整反应活性。暴露于CO2最大化和动态重构的Ni-ZrO 2界面,这是获得稳定的催化剂的关键。在这个界面上的ZrO 2 − x物种被发现通过接受和转移CO2中的一个氧原子到Ni表面来起催化作用,这导致在瞬时形成的碳酸盐分解中释放CO。这被发现打开了一个快速的额外的反应途径,以转换CO2,掩盖直接CO2解离镍。通过该途径的原子氧的动力学控制的可用性降低了表面上的碳浓度,这导致更少的难熔碳沉积和更容易的再生。
The activity of the Ni/ZrO2catalyst for the dry reforming of methane was significantly enhanced by activation and regeneration in the presence of CO2. Exposure to CO2maximized and dynamically restructured the Ni–ZrO2interface, which was critical to obtain a stable catalyst. The ZrO2−xspecies at this interface was found to act catalytically by accepting and transferring one oxygen atom of CO2to the Ni surface, which resulted in the release of CO in the decomposition of transiently formed carbonates. This was found to open a fast additional reaction pathway to convert CO2that eclipsed direct CO2dissociation on Ni. The kinetically controlled availability of atomic oxygen by this pathway reduced the carbon concentration on the surface, which led to less refractory carbon deposition and more facile regeneration.
DOI: 10.1006/jcat.1998.2022
发表时间: 1998-05-15
影响因子: 7.3
作者:
Bitter, JH;Seshan, K;Lercher, JA
通讯作者: Lercher, JA
DOI: 10.1039/c6ra20450c
发表时间: 2016-01-01
期刊: RSC ADVANCES
影响因子: 3.9
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通讯作者: Prasad, R.
DOI: --
发表时间: 2002
期刊:
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通讯作者: V. Korchak