Unique hole-accepting carbon-dots promoting selective carbon dioxide reduction nearly 100% to methanol by pure water

Yiou Wang, Xu Liu, Xiaoyu Han, Robert Godin (), Jialu Chen, Wuzong Zhou, Chaoran Jiang, Jamie F. Thompson, K. Bayazit Mustafa, Stephen A. Shevlin, James R. Durrant, Zhengxiao Guo () and Junwang Tang ()
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Yiou Wang: University College London
Xu Liu: University College London
Xiaoyu Han: University College London
Robert Godin: Imperial College London
Jialu Chen: University of St. Andrews
Wuzong Zhou: University of St. Andrews
Chaoran Jiang: University College London
Jamie F. Thompson: Imperial College London
K. Bayazit Mustafa: University College London
Stephen A. Shevlin: University College London
James R. Durrant: Imperial College London
Zhengxiao Guo: University College London
Junwang Tang: University College London

Nature Communications, 2020, vol. 11, issue 1, 1-9

Abstract: Abstract Solar-driven CO2 reduction by abundant water to alcohols can supply sustainable liquid fuels and alleviate global warming. However, the sluggish water oxidation reaction has been hardly reported to be efficient and selective in CO2 conversion due to fast charge recombination. Here, using transient absorption spectroscopy, we demonstrate that microwave-synthesised carbon-dots (mCD) possess unique hole-accepting nature, prolonging the electron lifetime (t50%) of carbon nitride (CN) by six folds, favouring a six-electron product. mCD-decorated CN stably produces stoichiometric oxygen and methanol from water and CO2 with nearly 100% selectivity to methanol and internal quantum efficiency of 2.1% in the visible region, further confirmed by isotopic labelling. Such mCD rapidly extracts holes from CN and prevents the surface adsorption of methanol, favourably oxidising water over methanol and enhancing the selective CO2 reduction to alcohols. This work provides a unique strategy for efficient and highly selective CO2 reduction by water to high-value chemicals.

Date: 2020
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DOI: 10.1038/s41467-020-16227-3

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