Atomically dispersed MoNi alloy catalyst for partial oxidation of methane

• Published in: Nature communications Vol. 15; no. 1; pp. 4636 - 10
• Main Authors: Ding, Zheyuan, Chen, Sai, Yang, Tingting, Sheng, Zunrong, Zhang, Xianhua, Pei, Chunlei, Fu, Donglong, Zhao, Zhi-Jian, Gong, Jinlong
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 31.05.2024; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/146; 147/143; 639/166/898; 639/638/77/885; 639/638/77/887; Adsorption; Alloys; Catalysts; Density functional theory; Humanities and Social Sciences; Hydrogen bonds; Metal surfaces; Methane; multidisciplinary; Oxidation; Poisoning (reaction inhibition); Reforming; Science; Science (multidisciplinary); Synthesis gas
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-024-49038-x

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. The catalytic partial oxidation of methane (POM) is a promising technology for synthesizing syngas but suffers from severe over-oxidation on the catalyst surface. Here the authors demonstrate that regulating O* occupation in an atomically dispersed MoNi alloy can achieve high catalytic performance for POM.