Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 13, Issue 36, Pages 8397-8402Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.2c01983
Keywords
-
Categories
Funding
- National Key Research and Development Program of China [2017YFA0403402, 2019YFA0405602, 2021YFA1600800, 2018 Y F A 0 2 0 8 7 0 2, 2016 Y F A 0 2 0 0 6 0 2, 2017YFA0303500]
- National Natural Science Foundation of China [21673214, U1732272, 92045301, 22173090, 91950207, 21633007, 21573211]
- Fundamental Research Funds for the Central Universities [20720220010]
- innovation Program for Quantum Science and Technology [2021ZD0303303]
- Excellence Program of Hefei Science Center of CAS [2020HSC-UE00]
- Hefei Municipal Natural Science Foundation [2021018]
- Anhui Initiative in Quantum Information Technologies [AHY090200]
- USTC Key Directions Project Incubation Fund [WK2340000106]
Ask authors/readers for more resources
This study proposes a novel strategy of unpaired electron engineering to achieve photocatalytic CO2 reduction to CH4. The strategy improves the selectivity and conversion efficiency of CH4 production.
The photocatalytic CO2 reduction to CH4 reaction is a long process of proton-coupled charge transfer accompanied by various reaction intermediates. Achieving high CH4 selectivity with satisfactory conversion efficiency therefore remains rather challenging. Herein, we propose a novel strategy of unpaired electron engineering to break through such a demanding bottleneck. By taking TiO2 as a photocatalyst prototype, we prove that unpaired electrons stabilize the key intermediate of CH4 production, i.e., CHO*, via chemical bonding, which converts the endothermic step of CHO* formation to an exothermic process, thereby altering the reaction pathway to selectively produce CH4. Meanwhile, these unpaired electrons generate midgap states to restrict charge recombination by trapping free electrons. As an outcome, such an unpaired electron engineered TiO2 achieves an electron-consumption rate as high as 28.3 mu mol.g-1.h(-1) (15.7 fold with respect to normal TiO2) with a 97% CH(4 )selectivity. This work demonstrates that electron regulation holds great promise in attaining efficient and selective heterogeneous photocatalytic conversion.
Authors
I am an author on this paper
Click your name to claim this paper and add it to your profile.
Reviews
Recommended
No Data Available