Atomically dispersed low-valent Au boosts photocatalytic hydroxyl radical production

Zhenyuan Teng; Hongbin Yang; Qitao Zhang; Wenan Cai; Ying-Rui Lu; Kosaku Kato; Zhenzong Zhang; Jie Ding; Han Sun; Sixiao Liu; Chengyin Wang; Peng Chen; Akira Yamakata; Ting-Shan Chan; Chenliang Su; Teruhisa Ohno; Bin Liu

doi:10.1038/s41557-024-01553-6

Atomically dispersed low-valent Au boosts photocatalytic hydroxyl radical production

Zhenyuan Teng
, Hongbin Yang
, Qitao Zhang
, Wenan Cai
, Ying-Rui Lu
, Kosaku Kato
, Zhenzong Zhang
, Jie Ding
, Han Sun
, Sixiao Liu
, Chengyin Wang
, Peng Chen
, Akira Yamakata
, Ting-Shan Chan
, Chenliang Su^*
, Teruhisa Ohno^*
, Bin Liu^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

189 Citations (Scopus)

Abstract

Providing affordable, safe drinking water and universal sanitation poses a grand societal challenge. Here we developed atomically dispersed Au on potassium-incorporated polymeric carbon nitride material that could simultaneously boost photocatalytic generation of ·OH and H₂O₂ with an apparent quantum efficiency over 85% at 420 nm. Potassium introduction into the poly(heptazine imide) matrix formed strong K–N bonds and rendered Au with an oxidation number close to 0. Extensive experimental characterization and computational simulations revealed that the low-valent Au altered the materials’ band structure to trap highly localized holes produced under photoexcitation. These highly localized holes could boost the 1e⁻ water oxidation reaction to form highly oxidative ·OH and simultaneously dissociate the hydrogen atom in H₂O, which greatly promoted the reduction of oxygen to H₂O₂. The photogenerated ·OH led to an efficiency enhancement for visible-light-response superhydrophilicity. Furthermore, photo-illumination in an onsite fixed-bed reactor could disinfect water at a rate of 66 L H₂O m⁻² per day. © The Author(s), under exclusive licence to Springer Nature Limited 2024.

Original language	English
Pages (from-to)	1250-1260
Journal	Nature Chemistry
Volume	16
Issue number	8
Online published	25 Jun 2024
DOIs	https://doi.org/10.1038/s41557-024-01553-6
Publication status	Published - Aug 2024

Funding

The authors acknowledge the financial support of City University of Kong Hong startup fund (9020003, B.L.), ITF–RTH - Global STEM Professorship (9446006, B.L.), Mitsubishi Chemical Corporation, JSPS Grant-in-Aid for Scientific Research (B, no. 20H02847, T.O.), The National Key Research and Development Program of China (2021YFA1600800, C.S.), Grant-in-Aid for JSPS Fellows (DC2, 20J13064), Project National Natural Science Foundation of China (22372102, C.S.; 21805191, Q.Z.; 21972094, C.S.), the Guangdong Basic and Applied Basic Research Foundation (2024A1515010976 and 2020A1515010982), Shenzhen Science and Technology Program (RCJC20200714114434086, C.S.), and Shenzhen Peacock Plan (202108022524B, Q.Z.). Research Team Cultivation Program of Shenzhen University (2023QNT013, C.S.). National Science and Technology Council (NSTC, 110-2112-M-213-019-MY3). The authors thank J. Xiao, T. Hisatomi and K. Domen from Shinshu University for their help in ·OH detection and D2O experiments. The authors also thank X. Cai (Nanyang Technological University), C. Chen (King Abdullah University of Science and Technology), Y. Han (King Abdullah University of Science and Technology), L. Gu (Institute of Physics, Chinese Academy of Sciences), R. Luo (University of Chinese Academy of Sciences), X. Peng (University of Chinese Academy of Sciences), W. Zhou (University of Chinese Academy of Sciences), K. Niu (Southern University of Science and Technology), W. Wang (Southern University of Science and Technology), J. Lin (Southern University of Science and Technology) and, especially, N. Jian (Electron Microscope Center of the Shenzhen University) for their help in HR-TEM measurements. The authors thank X. Zheng (National Synchrotron Radiation Laboratory, University of Science and Technology of China) for his help in analysing data of soft X-ray absorption.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 6 Clean Water and Sanitation

RGC Funding Information

RGC-funded

ESI Highly Cited Papers

Highly Cited Paper 2026
Highly Cited Paper 2025

ESI Highly Cited Paper Designation Date(s)

20260108
20250508
20250911
20250710
20260514
20251113
20260312
20260709
20260923

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title = "Atomically dispersed low-valent Au boosts photocatalytic hydroxyl radical production",

abstract = "Providing affordable, safe drinking water and universal sanitation poses a grand societal challenge. Here we developed atomically dispersed Au on potassium-incorporated polymeric carbon nitride material that could simultaneously boost photocatalytic generation of ·OH and H2O2 with an apparent quantum efficiency over 85\% at 420 nm. Potassium introduction into the poly(heptazine imide) matrix formed strong K–N bonds and rendered Au with an oxidation number close to 0. Extensive experimental characterization and computational simulations revealed that the low-valent Au altered the materials{\textquoteright} band structure to trap highly localized holes produced under photoexcitation. These highly localized holes could boost the 1e− water oxidation reaction to form highly oxidative ·OH and simultaneously dissociate the hydrogen atom in H2O, which greatly promoted the reduction of oxygen to H2O2. The photogenerated ·OH led to an efficiency enhancement for visible-light-response superhydrophilicity. Furthermore, photo-illumination in an onsite fixed-bed reactor could disinfect water at a rate of 66 L H2O m−2 per day. {\textcopyright} The Author(s), under exclusive licence to Springer Nature Limited 2024.",

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language = "English",

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T1 - Atomically dispersed low-valent Au boosts photocatalytic hydroxyl radical production

AU - Teng, Zhenyuan

AU - Yang, Hongbin

AU - Zhang, Qitao

AU - Cai, Wenan

AU - Lu, Ying-Rui

AU - Kato, Kosaku

AU - Zhang, Zhenzong

AU - Ding, Jie

AU - Sun, Han

AU - Liu, Sixiao

AU - Wang, Chengyin

AU - Chen, Peng

AU - Yamakata, Akira

AU - Chan, Ting-Shan

AU - Su, Chenliang

AU - Ohno, Teruhisa

AU - Liu, Bin

PY - 2024/8

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N2 - Providing affordable, safe drinking water and universal sanitation poses a grand societal challenge. Here we developed atomically dispersed Au on potassium-incorporated polymeric carbon nitride material that could simultaneously boost photocatalytic generation of ·OH and H2O2 with an apparent quantum efficiency over 85% at 420 nm. Potassium introduction into the poly(heptazine imide) matrix formed strong K–N bonds and rendered Au with an oxidation number close to 0. Extensive experimental characterization and computational simulations revealed that the low-valent Au altered the materials’ band structure to trap highly localized holes produced under photoexcitation. These highly localized holes could boost the 1e− water oxidation reaction to form highly oxidative ·OH and simultaneously dissociate the hydrogen atom in H2O, which greatly promoted the reduction of oxygen to H2O2. The photogenerated ·OH led to an efficiency enhancement for visible-light-response superhydrophilicity. Furthermore, photo-illumination in an onsite fixed-bed reactor could disinfect water at a rate of 66 L H2O m−2 per day. © The Author(s), under exclusive licence to Springer Nature Limited 2024.

AB - Providing affordable, safe drinking water and universal sanitation poses a grand societal challenge. Here we developed atomically dispersed Au on potassium-incorporated polymeric carbon nitride material that could simultaneously boost photocatalytic generation of ·OH and H2O2 with an apparent quantum efficiency over 85% at 420 nm. Potassium introduction into the poly(heptazine imide) matrix formed strong K–N bonds and rendered Au with an oxidation number close to 0. Extensive experimental characterization and computational simulations revealed that the low-valent Au altered the materials’ band structure to trap highly localized holes produced under photoexcitation. These highly localized holes could boost the 1e− water oxidation reaction to form highly oxidative ·OH and simultaneously dissociate the hydrogen atom in H2O, which greatly promoted the reduction of oxygen to H2O2. The photogenerated ·OH led to an efficiency enhancement for visible-light-response superhydrophilicity. Furthermore, photo-illumination in an onsite fixed-bed reactor could disinfect water at a rate of 66 L H2O m−2 per day. © The Author(s), under exclusive licence to Springer Nature Limited 2024.

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M3 - RGC 21 - Publication in refereed journal

SN - 1755-4330

VL - 16

SP - 1250

EP - 1260

JO - Nature Chemistry

JF - Nature Chemistry

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ER -

Atomically dispersed low-valent Au boosts photocatalytic hydroxyl radical production

Abstract

Funding

UN SDGs

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ESI Highly Cited Paper Designation Date(s)

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Other Access Options

Permanent Link

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ITF-RTH: GSP212 - Research Talent Hub

RMGS: On-site Green Hydrogen Production and Storage for Distributed Carbon Neutral Applications

Cite this

Atomically dispersed low-valent Au boosts photocatalytic hydroxyl radical production

Abstract

Funding

UN SDGs

RGC Funding Information

ESI Highly Cited Papers

ESI Highly Cited Paper Designation Date(s)

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Projects

ITF-RTH: GSP212 - Research Talent Hub

RMGS: On-site Green Hydrogen Production and Storage for Distributed Carbon Neutral Applications

Cite this