High Alcohols Synthesis via Fischer-Tropsch Reaction at Cobalt Metal/Carbide Interface
High Alcohols Synthesis via Fischer-Tropsch Reaction at Cobalt Metal/Carbide Interface
复制标题
通过钴金属/碳化物界面的费托反应合成高级醇
DOI：
10.1021/acscatal.5b00791
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发表时间：
2015-06-01
期刊：
影响因子：
12.9
通讯作者：
Li, Wei-Xue
中科院分区：
文献类型：
--
作者：
Pei, Yan-Peng;Liu, Jin-Xun;Li, Wei-Xue
利用非贵金属过渡金属合成高级醇在多相催化中具有重要意义。我们成功地合成了金属碳化钴(Co-Co2C)催化剂，该催化剂通过Fischer-Tropsch反应对高级醇具有良好的活性和选择性。稳定的钴碳化物和Co-Co2C界面的形成对观察到的反应活性是必不可少的。密度泛函理论计算表明，Co2C对CO的非解离吸附是高效的，表现为类贵金属，而Co金属对CO解离吸附和随后的碳链生长具有很高的活性。金属钴和碳化物之间的界面，以及界面上存在的CO易插入碳氢化合物的双位，可用于合理设计合成气转化中含氧化合物的非贵金属过渡金属催化剂。
Utilization of nonprecious transition metals for high alcohols synthesis is of a great importance in heterogeneous catalysis. We synthesized successfully cobalt metal-carbide (Co-Co2C) catalysts, which present remarkable activity and selectivity for high alpha-alcohols via the Fischer-Tropsch reaction. The formation of the stable cobalt carbide and the Co-Co2C interface are found to be essential for the observed reactivity. Density functional theory calculations show that Co2C is highly efficient for CO nondissociative adsorption, behaving as noble-metal-like, whereas the Co metal is highly active for CO dissociative adsorption and the subsequent carbon-chain growth. The interface between the cobalt metal and its carbide phase, as well as the dual sites available at the interface for facile CO insertion to hydrocarbon, could be used to rationalize the design of the nonprecious transition metal catalysts for the oxygenates in syngas conversion.