Wang, Hui; Qi, Haifeng; Sun, Xiao; Jia, Shuya; Li, Xiyi; Miao, Tina Jingyan; Xiong, Lunqiao; ... Tang, Junwang; + view all Wang, Hui; Qi, Haifeng; Sun, Xiao; Jia, Shuya; Li, Xiyi; Miao, Tina Jingyan; Xiong, Lunqiao; Wang, Shihao; Zhang, Xiaolei; Liu, Xiaoyan; Wang, Aiqin; Zhang, Tao; Huang, Weixin; Tang, Junwang; - view fewer (2023) High quantum efficiency of hydrogen production from methanol aqueous solution with PtCu–TiO₂ photocatalysts. Nature Materials , 22 pp. 619-626. 10.1038/s41563-023-01519-y.

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Abstract

Methanol with 12.5 wt% H2 content is widely considered a liquid hydrogen medium. Taking into account water with 11.1 wt% H2 content, H2 synthesis from the mixture of water and methanol is a promising method for on-demand hydrogen production. We demonstrate an atomic-level catalyst design strategy using the synergy between single atoms and nanodots for H2 production. The PtCu-TiO2 sandwich photocatalyst achieves a remarkable H2 formation rate (2,383.9 µmol h-1) with a high apparent quantum efficiency (99.2%). Furthermore, the oxidation product is a high-value chemical formaldehyde with 98.6% selectivity instead of CO2, leading to a nearly zero-carbon-emission process. Detailed investigations indicate a dual role of the copper atoms: an electron acceptor to facilitate photoelectron transfer to Pt, and a hole acceptor for the selective oxidation of methanol to formaldehyde, thus avoiding over-oxidation to CO2. The synergy between Pt nanodots and Cu single atoms together reduces the activation energy of this process to 13.2 kJ mol-1.

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