Topological Transformation of Mg‐Containing Layered Double Hydroxide Nanosheets for Efficient Photodriven CH4 Coupling

Abstract Direct conversion of methane (CH 4 ) to fuels and other high value‐added chemicals is an attractive technology in the chemical industry; however, practical challenges to sustainable processes remain. Herein, we report the preparation of a heterostructured Co‐doped MgO‐based catalyst through topological transformation of a MgCo‐layered double hydroxide (LDH) calcination from 200 to 1100 °C. Remarkably, the catalyst can activate CH 4 coupling to produce C 2 H 6 with a selectivity of 41.60 % within 3 h under full‐spectrum irradiation through calcination of LDH at 800 °C. Characterization studies and catalytic results suggest that the highly dispersed active sites and large interfaces amongst the Co‐doped MgO‐based catalysts enable surface activation of CH 4 to methyl (CH 3 *), in turn promoting coupling of CH 3 * to C 2 H 6 . This study introduces a promising pathway for photodriven CH 4 coupling to give high value‐added chemicals by using layered double hydroxides as a precursor.