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Nano Research 2024, 17(3): 1209-1216 https://doi.org/10.1007/s12274-023-5997-z
Research Article | Issue | Published: 14 August 2023

Au nanoclusters anchored on TiO2 nanosheets for high-efficiency electroreduction of nitrate to ammonia

Show Author's Information Miaosen Yang1,2,  Tianran Wei3,4,  Jia He5( ),  Qian Liu6,  Ligang Feng7,  Hongyi Li3,8( ),  Jun Luo9,  Xijun Liu4( )
School of Chemical Engineering, Northeast Electric Power University, Jilin 132012, China
Nanchang Institute of Technology, Nanchang 330044, China
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830017, China
State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, School of Resources, Environment and Materials, Guangxi University, Nanning 530004, China
Institute for New Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
Institute for Advanced Study, Chengdu University, Chengdu 610106, China
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, China
Guangzhou Panyu Polytechnic, Guangzhou 511483, China
ShenSi Lab, Shenzhen Institute for Advanced Study, University of Electronic Science and Technology of China, Longhua District, Shenzhen 518110, China
Keywords:
NH3 electrosynthesis, Au nanoclusters, TiO2 nanosheets, Zn-nitrate battery, nitrate reduction reaction (NRR)
Topics:
Electrocatalysts
Cite this article:
Yang M, Wei T, He J, et al. Au nanoclusters anchored on TiO2 nanosheets for high-efficiency electroreduction of nitrate to ammonia. Nano Research, 2024, 17(3): 1209-1216. https://doi.org/10.1007/s12274-023-5997-z
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Abstract Full text Electronic supplementary material About this article

Electrocatalytic nitrate reduction reaction (NO3RR) offers a unique rationale for green NH3 synthesis, yet the lack of high-efficiency NO3RR catalysts remains a great challenge. In this work, we show that Au nanoclusters anchored on TiO2 nanosheets can efficiently catalyze the conversion of NO3RR-to-NH3 under ambient conditions, achieving a maximal Faradic efficiency of 91%, a peak yield rate of 1923 μg·h−1·mgcat.−1, and high durability over 10 consecutive cycles, all of which are comparable to the recently reported metrics (including transition metal and noble metal-based catalysts) and exceed those of pristine TiO2. Moreover, a galvanic Zn-nitrate battery using the catalyst as the cathode was proposed, which shows a power density of 3.62 mW·cm−2 and a yield rate of 452 μg·h−1·mgcat.−1. Theoretical simulations further indicate that the atomically dispersed Au clusters can promote the adsorption and activation of NO3− species, and reduce the NO3RR-to-NH3 barrier, thus leading to an accelerated cathodic reaction. This work highlights the importance of metal clusters for the NH3 electrosynthesis and nitrate removal.


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Abstract
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Electronic supplementary material
About this article

Au nanoclusters anchored on TiO2 nanosheets for high-efficiency electroreduction of nitrate to ammonia

Show Author's information Miaosen Yang1,2, Tianran Wei3,4, Jia He5( ), Qian Liu6, Ligang Feng7, Hongyi Li3,8( ), Jun Luo9, Xijun Liu4( )
School of Chemical Engineering, Northeast Electric Power University, Jilin 132012, China
Nanchang Institute of Technology, Nanchang 330044, China
State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources, College of Chemistry, Xinjiang University, Urumqi 830017, China
State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, School of Resources, Environment and Materials, Guangxi University, Nanning 530004, China
Institute for New Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
Institute for Advanced Study, Chengdu University, Chengdu 610106, China
School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, China
Guangzhou Panyu Polytechnic, Guangzhou 511483, China
ShenSi Lab, Shenzhen Institute for Advanced Study, University of Electronic Science and Technology of China, Longhua District, Shenzhen 518110, China

Abstract

Electrocatalytic nitrate reduction reaction (NO3RR) offers a unique rationale for green NH3 synthesis, yet the lack of high-efficiency NO3RR catalysts remains a great challenge. In this work, we show that Au nanoclusters anchored on TiO2 nanosheets can efficiently catalyze the conversion of NO3RR-to-NH3 under ambient conditions, achieving a maximal Faradic efficiency of 91%, a peak yield rate of 1923 μg·h−1·mgcat.−1, and high durability over 10 consecutive cycles, all of which are comparable to the recently reported metrics (including transition metal and noble metal-based catalysts) and exceed those of pristine TiO2. Moreover, a galvanic Zn-nitrate battery using the catalyst as the cathode was proposed, which shows a power density of 3.62 mW·cm−2 and a yield rate of 452 μg·h−1·mgcat.−1. Theoretical simulations further indicate that the atomically dispersed Au clusters can promote the adsorption and activation of NO3− species, and reduce the NO3RR-to-NH3 barrier, thus leading to an accelerated cathodic reaction. This work highlights the importance of metal clusters for the NH3 electrosynthesis and nitrate removal.

Keywords: NH3 electrosynthesis, Au nanoclusters, TiO2 nanosheets, Zn-nitrate battery, nitrate reduction reaction (NRR)

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Publication history
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Acknowledgements

Publication history

Received: 10 May 2023
Revised: 04 July 2023
Accepted: 10 July 2023
Published: 14 August 2023
Issue date: March 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 22075211 and 51971157), the Guangzhou Basic & Applied Basic Research Project (No. 202201011853), the Shenzhen Science and Technology Program (Nos. JCYJ20210324115412035, JCYJ20210324123202008, JCYJ20210324122803009, and ZDSYS20210813095534001), the Guangdong Basic and Applied Basic Research Foundation (No. 2021A1515110880), and the Tianjin Science Fund for Distinguished Young Scholars (No. 19JCJQJC61800).

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