Atomically dispersed MoNi alloy catalyst for partial oxidation of methane.

Ding, Zheyuan; Chen, Sai; Yang, Tingting; Sheng, Zunrong; Zhang, Xianhua; Pei, Chunlei; Fu, Donglong; Zhao, Zhi-Jian et al. · Nat Commun · 2024

basic_science · Level V

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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<sub>4</sub> 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<sub>4</sub> 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<sub>2</sub> poisoning on Ni sites with rarely weaken CH<sub>4</sub> activation for partial oxidation pathway following the combustion reforming reaction (CRR) mechanism. These results underscore the effectiveness of CH<sub>4</sub> turnovers by the design of atomically dispersed alloys with tunable O* adsorption.