Engineering nanoscale H supply chain to accelerate methanol synthesis on ZnZrOx

Kyungho Lee, Paulo C. D. Mendes, Hyungmin Jeon, Yizhen Song, Maxim Park Dickieson, Uzma Anjum, Luwei Chen, Tsung-Cheng Yang, Chia-Min Yang, Minkee Choi, Sergey M. Kozlov () and Ning Yan ()
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Kyungho Lee: National University of Singapore
Paulo C. D. Mendes: National University of Singapore
Hyungmin Jeon: Department of Chemical and Biomolecular Engineering, KAIST
Yizhen Song: National University of Singapore
Maxim Park Dickieson: National University of Singapore
Uzma Anjum: National University of Singapore
Luwei Chen: Agency for Science, Technology and Research (A*STAR)
Tsung-Cheng Yang: National Tsing Hua University
Chia-Min Yang: National Tsing Hua University
Minkee Choi: Department of Chemical and Biomolecular Engineering, KAIST
Sergey M. Kozlov: National University of Singapore
Ning Yan: National University of Singapore

Nature Communications, 2023, vol. 14, issue 1, 1-11

Abstract: Abstract Metal promotion is the most widely adopted strategy for enhancing the hydrogenation functionality of an oxide catalyst. Typically, metal nanoparticles or dopants are located directly on the catalyst surface to create interfacial synergy with active sites on the oxide, but the enhancement effect may be compromised by insufficient hydrogen delivery to these sites. Here, we introduce a strategy to promote a ZnZrOx methanol synthesis catalyst by incorporating hydrogen activation and delivery functions through optimized integration of ZnZrOx and Pd supported on carbon nanotube (Pd/CNT). The CNT in the Pd/CNT + ZnZrOx system delivers hydrogen activated on Pd to a broad area on the ZnZrOx surface, with an enhancement factor of 10 compared to the conventional Pd-promoted ZnZrOx catalyst, which only transfers hydrogen to Pd-adjacent sites. In CO2 hydrogenation to methanol, Pd/CNT + ZnZrOx exhibits drastically boosted activity—the highest among reported ZnZrOx-based catalysts—and excellent stability over 600 h on stream test, showing potential for practical implementation.

Date: 2023
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DOI: 10.1038/s41467-023-36407-1

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