Litcius/Paper detail

Radiocatalytic Synthesis of Acetic Acid from CH<sub>4</sub> and CO<sub>2</sub>

Bo‐Shuai Mu, Yugang Zhang, Mi Peng, Zhiyu Tu, Zhenbo Guo, Siyong Shen, Yang Xu, Weiqiu Liang, Xianglin Wang, Meng Wang, Ding Ma, Zhibo Liu, Zhibo Liu

2024Angewandte Chemie International Edition20 citationsDOI

Abstract

Abstract The C−C coupling of methane (CH 4 ) and carbon dioxide (CO 2 ) to generate acetic acid (CH 3 COOH) represents a highly atom‐efficient chemical conversion, fostering the comprehensive utilization of greenhouse gases. However, the inherent thermodynamic stability and kinetic inertness of CH 4 and CO 2 present obstacles to achieving efficient and selective conversion at room temperature. Our study reveals that hydroxyl radicals (⋅OH) and hydrated electrons (e aq − ) produced by water radiolysis can effectively activate CH 4 and CO 2 , yielding methyl radicals (⋅CH 3 ) and carbon dioxide radical anions(⋅CO 2 − ) that facilitate the production of CH 3 COOH at ambient temperature. The introduction of radiation‐synthesized CuO‐anchored TiO 2 bifunctional catalyst could further enhance reaction efficiency and selectivity remarkably by boosting radiation absorption and radical stability, resulting in a concentration of 7.1 mmol ⋅ L −1 of CH 3 COOH with near‐unity selectivity (&gt;95 %). These findings offer valuable insights for catalyst design and implementation in radiation‐induced chemical conversion.

Topics & Concepts

RadicalChemistryCatalysisSelectivityRadiolysisAcetic acidMethaneCarbon dioxideBifunctionalChemical stabilityPhotochemistryOrganic chemistryCatalytic Processes in Materials ScienceCarbon dioxide utilization in catalysisCatalysis and Oxidation Reactions