Cu-supported nano-ZrZnOx as a highly active inverse catalyst for low temperature methanol synthesis from CO2 hydrogenation

• Published in: Applied catalysis. B, Environmental Vol. 344; p. 123656
• Main Authors: Xu, Yangzhi, Gao, Zirui, Xu, Yao, Qin, Xuetao, Tang, Xin, Xie, Zhiwei, Zhang, Jinrong, Song, Chuqiao, Yao, Siyu, Zhou, Wu, Ma, Ding, Lin, Lili
• Format: Journal Article
• Language: English
• Published: Elsevier B.V 05-05-2024
• Subjects: CO2 hydrogenation; Cu-based inverse catalyst; In situ DRIFTS; Low-temperature methanol synthesis; ZrZnOx mixed nano-oxides; Cu-based inverse catalyst; Low-temperature methanol synthesis; ZrZnOx mixed nano-oxides; In situ DRIFTS; CO2 hydrogenation
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2023.123656

Hydrogenation of CO2 into methanol at low-temperature on Cu-based catalysts is of great significance, but remains challenging to enhance activity. In this paper, we report an inverse catalyst constructed with nano-ZrZnOx supported on Cu particles with outstanding methanol synthesis performance at 220 ℃, two times higher than that of commercial Cu/ZnO/Al2O3 catalysts under the same conditions. Detailed structure characterization and performance evaluation demonstrate that the ZrZnOx mixed oxide serves as the most active oxide-metal interface site for CO2 hydrogenation. The ZrZnOx/Cu inverse catalyst increases the weak and medium CO2 adsorption sites which are further demonstrated responsible to the methanol productivity. In situ DRIFTs studies reveal that the inverse interface accelerates the reduction of asymmetric formate intermediates and prevents the generation of CO. The combination of enhanced CO2 activation capability and accelerated hydrogenation rate of intermediates over the ZrZnOx/Cu inverse catalyst probably contribute to the remarkable methanol synthesis performance from CO2.
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•Inverse ZrZnOx/Cu is highly active for methanol synthesis from CO2 hydrogenation.•The inverse catalyst shows room temperature methanol synthesis ability.•The formation of ZrZnOx nano-oxide is responsible for the extraordinary activity.•Inverse interface accelerates the reduction of adsorbed oxygenate intermediates.•Inverse interface inhibits the formation of CO intermediates.