Filling metal–organic framework mesopores with TiO2 for CO2 photoreduction

Zhuo Jiang, Xiaohui Xu, Yanhang Ma, Hae Sung Cho, Deng Ding, Chao Wang, Jie Wu, Peter Oleynikov, Mei Jia, Jun Cheng, Yi Zhou, Osamu Terasaki (), Tianyou Peng, Ling Zan () and Hexiang Deng ()
Additional contact information
Zhuo Jiang: Wuhan University
Xiaohui Xu: Wuhan University
Yanhang Ma: ShanghaiTech University
Hae Sung Cho: ShanghaiTech University
Deng Ding: Wuhan University
Chao Wang: Wuhan University
Jie Wu: Wuhan University
Peter Oleynikov: ShanghaiTech University
Mei Jia: Xiamen University
Jun Cheng: Xiamen University
Yi Zhou: Wuhan University
Osamu Terasaki: ShanghaiTech University
Tianyou Peng: Wuhan University
Ling Zan: Wuhan University
Hexiang Deng: Wuhan University

Nature, 2020, vol. 586, issue 7830, 549-554

Abstract: Abstract Metal–organic frameworks (MOFs)1–3 are known for their specific interactions with gas molecules4,5; this, combined with their rich and ordered porosity, makes them promising candidates for the photocatalytic conversion of gas molecules to useful products6. However, attempts to use MOFs or MOF-based composites for CO2 photoreduction6–13 usually result in far lower CO2 conversion efficiency than that obtained from state-of-the-art solid-state or molecular catalysts14–18, even when facilitated by sacrificial reagents. Here we create ‘molecular compartments’ inside MOF crystals by growing TiO2 inside different pores of a chromium terephthalate-based MOF (MIL-101) and its derivatives. This allows for synergy between the light-absorbing/electron-generating TiO2 units and the catalytic metal clusters in the backbones of MOFs, and therefore facilitates photocatalytic CO2 reduction, concurrent with production of O2. An apparent quantum efficiency for CO2 photoreduction of 11.3 per cent at a wavelength of 350 nanometres is observed in a composite that consists of 42 per cent TiO2 in a MIL-101 derivative, namely, 42%-TiO2-in-MIL-101-Cr-NO2. TiO2 units in one type of compartment in this composite are estimated to be 44 times more active than those in the other type, underlining the role of precise positioning of TiO2 in this system.

Date: 2020
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DOI: 10.1038/s41586-020-2738-2

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