Engineering the Atomic Configurations of Surface-Active Sites for Retuning the Photoreduction CO<sub>2</sub> Selectivity
Min Shen, Ye Yan, Mingyue Wang, Xiaocong Liang, Hao Tang, Yulan Wang, Chuchu Zhou, Shilan Zhang, Sikang Xue, Can Yang, Wandong Xing, Zhiyang Yu
Abstract
The photoreduction of the CO 2 reaction is a potential technique for converting solar energy to fuel at room temperature, which speeds up the recycling and conversion of carbon compounds. Based on a highly active photocatalyst, however, disentangling the chemical environments of surface structures on the selectivity of the product at the atomic scale is challenging. Herein, we have explored a sulfur-assisted heat treatment strategy to induce the reconstruction from surface-ordered line defects to polygonal tungsten line defects, changing the main product from CH 4 (8.2 μmol h –1, 5 mg) to CO (13.0 μmol h –1, 5 mg) without any additive sacrificial agents. The experimental results reveal that the active sites are the surface terminations of the hexagonal-tungsten line defect, where the in-plane-neighboring W atoms can break the C–O bonds inside the *COOH intermediates, thereby promoting the desorption of CO gas.