ABSTRACT To improve the efficiency of existing Cu‐layered double oxide (LDO) catalysts for hydrogenation of CO 2 to methanol, graphene oxide (GO)‐doped Cu‐LDO/xGO catalysts were successfully prepared by coprecipitation method, and the influence of GO doping on the structure and reaction performance of Cu‐LDO catalysts was deeply investigated. Characterizations including XRD, SEM, ICP‐OES, N 2 physical adsorption‐desorption, TEM, N 2 O chemisorption, H 2 ‐TPR, and H 2 /CO 2 ‐TPD reveal that optimal GO loading (2 wt%) promoted the formation of highly dispersed Cu particles and abundant Cu─MgO interfaces, enhancing H 2 adsorption/dissociation and CO 2 activation. The Cu‐LDO/2.0GO catalyst achieved a CO 2 conversion of 22.4%, CH 3 OH selectivity of 94.5%, and methanol space‐time yield (STY) of 652.1 g·kgcat −1 ·h −1 at 240°C and 2.5 MPa‐outperforming the GO‐free Cu‐LDO/0GO catalyst, and long‐term stability tests show that the incorporation of GO mitigated Cu sintering, maintaining catalytic activity over 200 h. The results of structure‐activity relationship analysis show that the main reason 2 wt% GO doping significantly improved the activity and stability of the catalyst lies in the synergistic effect: GO improved Cu sites dispersion boosting H 2 activation and Cu─MgO interface formation. Meanwhile, GO can also act as a conductive bridge for H spillover, enabling hydrogenation of formate and other intermediates adsorbed on Cu–MgO interfaces that are not in direct contact with conventional Cu surfaces, potentially involving isolated Cu species. The study establishes that rational GO incorporation optimizes active site utilization, providing a strategy for designing efficient catalysts for CO 2 conversion.
Huang et al. (Thu,) studied this question.