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 Thompson; Mustafa Bayazit; Stephen Shevlin; James Durrant; Zhengxiao Guo; Junwang Tang

doi:10.1038/s41467-020-16227-3

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 Thompson, Mustafa Bayazit, Stephen Shevlin, James Durrant, Zhengxiao Guo, Junwang Tang

Research output: Contribution to journal › Article › peer-review

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 (t_50%) 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.

Original language	English
Article number	2531
Number of pages	9
Journal	Nature Communications
Volume	11
DOIs	https://doi.org/10.1038/s41467-020-16227-3
Publication status	Published - 21 May 2020

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title = "Unique hole-accepting carbon-dots promoting selective carbon dioxide reduction nearly 100\% to methanol by pure water",

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.",

author = "Yiou Wang and Xu Liu and Xiaoyu Han and Robert Godin and Jialu Chen and Wuzong Zhou and Chaoran Jiang and Jamie Thompson and Mustafa Bayazit and Stephen Shevlin and James Durrant and Zhengxiao Guo and Junwang Tang",

note = "X.L., M.K.B., J.T. acknowledge EPSRC (EP/S018204/2/1), Leverhulme Trust (Grant No: RPG-2017-122) and Newton Advanced Fellowship grant ((NA170422 and NAF\textbackslash{}R1\textbackslash{}191163).). X.H., Z.X.G. and S.A.S. acknowledge UCL Grace High-Performance Computing Facility (Grace@UCL) and EPSRC (EP/K021192/1, EP/L018330/1). R.G. thanks the FRQNT for postdoctoral funding and NSERC for operational funding. Y.W., J.C. and C.J., acknowledge CSC Scholarship. R.G., J.F.T. and J.R.D. acknowledge ERC AdG Intersolar grant (291482). J.F.T. acknowledges EPSRC CDT (EP/L015277/1). W.Z. thanks EPSRC for Titan Themis S/TEM microscope (EP/L017008/01). We also thank Dr. Jijia Xie for constructive comments on experimental design.",

year = "2020",

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doi = "10.1038/s41467-020-16227-3",

language = "English",

volume = "11",

journal = "Nature Communications",

issn = "2041-1723",

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T1 - Unique hole-accepting carbon-dots promoting selective carbon dioxide reduction nearly 100% to methanol by pure water

AU - Wang, Yiou

AU - Liu, Xu

AU - Han, Xiaoyu

AU - Godin, Robert

AU - Chen, Jialu

AU - Zhou, Wuzong

AU - Jiang, Chaoran

AU - Thompson, Jamie

AU - Bayazit, Mustafa

AU - Shevlin, Stephen

AU - Durrant, James

AU - Guo, Zhengxiao

AU - Tang, Junwang

N1 - X.L., M.K.B., J.T. acknowledge EPSRC (EP/S018204/2/1), Leverhulme Trust (Grant No: RPG-2017-122) and Newton Advanced Fellowship grant ((NA170422 and NAF\R1\191163).). X.H., Z.X.G. and S.A.S. acknowledge UCL Grace High-Performance Computing Facility (Grace@UCL) and EPSRC (EP/K021192/1, EP/L018330/1). R.G. thanks the FRQNT for postdoctoral funding and NSERC for operational funding. Y.W., J.C. and C.J., acknowledge CSC Scholarship. R.G., J.F.T. and J.R.D. acknowledge ERC AdG Intersolar grant (291482). J.F.T. acknowledges EPSRC CDT (EP/L015277/1). W.Z. thanks EPSRC for Titan Themis S/TEM microscope (EP/L017008/01). We also thank Dr. Jijia Xie for constructive comments on experimental design.

PY - 2020/5/21

Y1 - 2020/5/21

N2 - 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.

AB - 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.

UR - https://www.scopus.com/pages/publications/85085154783

U2 - 10.1038/s41467-020-16227-3

DO - 10.1038/s41467-020-16227-3

M3 - Article

SN - 2041-1723

VL - 11

JO - Nature Communications

JF - Nature Communications

M1 - 2531

ER -

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

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