合成气
部分氧化
催化作用
合金
化学工程
甲烷
吸附
材料科学
密度泛函理论
选择性
金属
化学
物理化学
冶金
计算化学
有机化学
工程类
作者
Zheyuan Ding,Sai Chen,Tingting Yang,Zunrong Sheng,Xianhua Zhang,Chunlei Pei,Donglong Fu,Zhi‐Jian Zhao,Jinlong Gong
标识
DOI:10.1038/s41467-024-49038-x
摘要
Abstract The catalytic partial oxidation of methane (POM) presents a promising technology for synthesizing syngas. However, it faces severe over-oxidation over catalyst surface. Attempts to modify metal surfaces by incorporating a secondary metal towards C–H bond activation of CH 4 with moderate O* adsorption have remained the subject of intense research yet challenging. Herein, we report that high catalytic performance for POM can be achieved by the regulation of O* occupation in the atomically dispersed (AD) MoNi alloy, with over 95% CH 4 conversion and 97% syngas selectivity at 800 °C. The combination of ex-situ/in-situ characterizations, kinetic analysis and DFT (density functional theory) calculations reveal that Mo-Ni dual sites in AD MoNi alloy afford the declined O 2 poisoning on Ni sites with rarely weaken CH 4 activation for partial oxidation pathway following the combustion reforming reaction (CRR) mechanism. These results underscore the effectiveness of CH 4 turnovers by the design of atomically dispersed alloys with tunable O* adsorption.
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