Unraveling the Role of Atomically Dispersed Ga Species in the Selective Hydrogenation of CO<sub>2</sub> to Methanol over Cu/ZrO<sub>2</sub>
Xiaoyu Han, Maoshuai Li, Ziwen Hao, Jiyi Chen, Shixiong Tang, Zhenmei Zhang, Tiantian Xiao, Wenyan Jia, Mingcan Chen, Pengju Gao, Yurou Bai, Shengyu Wang, Shibo Xi, Kang Hui Lim, Yue Wang, Sibudjing Kawi, Xinbin Ma
Abstract
Synergistic interactions between active sites have been widely explored to enhance the catalytic performance of hydrogenation of CO 2 to methanol, yet the fundamental mechanisms, especially at the atomic level, remain unclear. Herein, we demonstrate that atomically dispersed Ga species incorporated into the ZrO 2 lattice significantly enhanced the catalytic performance of Cu/ZrO 2 for CO 2 hydrogenation to methanol. The optimized Cu/3GaZrO x catalyst exhibited a high methanol selectivity of 87% with a CO 2 conversion of 7.6% and a methanol space-time yield of up to 424 mg g cat –1 h –1 at 300 °C. In situ experiments combined with computational analyses revealed that the synergistic interaction between atomic Ga species and Cu nanoparticles enhanced H 2 dissociation, created additional CO 2 adsorption sites, and promoted the transformation of formate to methoxy species via the formate pathway over Cu/GaZrO x . This work provides a promising strategy for rationalizing an efficient catalyst for the hydrogenation of CO 2 to methanol.