High quantum efficiency of hydrogen production from methanol aqueous solution with PtCu–TiO2 photocatalysts

Wang, Hui and Qi, Haifeng and Sun, Xiao and Jia, Shuya and Li, Xiyi and Miao, Tina Jingyan and Xiong, Lunqiao and Wang, Shihao and Zhang, Xiaolei and Liu, Xiaoyan and Wang, Aiqin and Zhang, Tao and Huang, Weixin and Tang, Junwang (2023) High quantum efficiency of hydrogen production from methanol aqueous solution with PtCu–TiO2 photocatalysts. Nature Materials, 22 (5). pp. 619-626. ISSN 1476-1122 (https://doi.org/10.1038/s41563-023-01519-y)

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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.


Wang, Hui, Qi, Haifeng, Sun, Xiao, Jia, Shuya, Li, Xiyi, Miao, Tina Jingyan, Xiong, Lunqiao, Wang, Shihao, Zhang, Xiaolei ORCID logoORCID: https://orcid.org/0000-0001-9415-3136, Liu, Xiaoyan, Wang, Aiqin, Zhang, Tao, Huang, Weixin and Tang, Junwang;