Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation

Jianyun Zheng^{1

2

3}, Yanhong Lyu^{1

2}, Man Qiao⁴, Jean P Veder⁵, Roland D Marco^{3

6

7}, John Bradley⁶, Ruilun Wang^{1

2}, Yafei Li⁴, Aibin Huang^{8

9}, San Ping Jiang³, Shuangyin Wang^{1

2}

Affiliations

¹ State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, Hunan, China.
² The National Supercomputing Center in Changsha, Hunan University, Changsha, 410006, China.
³ Western Australian School of Mines: Minerals, Energy and Chemical Engineering and Fuels and Energy Technology Institute, Curtin University, Perth, WA, 6102, Australia.
⁴ Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing, 210023, China.
⁵ John de Laeter Centre, Curtin University, Perth, WA, 6102, Australia.
⁶ School of Science and Engineering, University of Sunshine Coast, 90 Sippy Downs Drive, Sippy Downs, Queensland, 4556, Australia.
⁷ School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, Queensland, 4072, Australia.
⁸ State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China.
⁹ University of Chinese Academy of Sciences, Beijing, 100049, China.

PMID: 31535425
DOI: 10.1002/anie.201909477

Review

Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation

Jianyun Zheng et al. Angew Chem Int Ed Engl. 2019.

. 2019 Dec 16;58(51):18604-18609.

doi: 10.1002/anie.201909477. Epub 2019 Nov 4.

Authors

Affiliations

¹ State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, 410082, Hunan, China.
² The National Supercomputing Center in Changsha, Hunan University, Changsha, 410006, China.
³ Western Australian School of Mines: Minerals, Energy and Chemical Engineering and Fuels and Energy Technology Institute, Curtin University, Perth, WA, 6102, Australia.
⁴ Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing, 210023, China.
⁵ John de Laeter Centre, Curtin University, Perth, WA, 6102, Australia.
⁶ School of Science and Engineering, University of Sunshine Coast, 90 Sippy Downs Drive, Sippy Downs, Queensland, 4556, Australia.
⁷ School of Chemistry and Molecular Biosciences, The University of Queensland, Brisbane, Queensland, 4072, Australia.
⁸ State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, China.
⁹ University of Chinese Academy of Sciences, Beijing, 100049, China.

PMID: 31535425
DOI: 10.1002/anie.201909477

Abstract

The (photo)electrochemical N₂ reduction reaction (NRR) provides a favorable avenue for the production of NH₃ using renewable energy in mild operating conditions. Understanding and building an efficient catalyst with high NH₃ selectivity represents an area of intense interest for the early stages of development for NRR. Herein, we introduce a CoO_x layer to tune the local electronic structure of Au nanoparticles with positive valence sites for boosting conversion of N₂ to NH₃ . The catalysts, possessing high average oxidation states (ca. 40 %), achieve a high NH₃ yield rate of 15.1 μg cm^-2 h^-1 and a good faradic efficiency of 19 % at -0.5 V versus reversible hydrogen electrode. Experimental results and simulations reveal that the ability to tune the oxidation state of Au enables the control of N₂ adsorption and the concomitant energy barrier of NRR. Altering the Au oxidation state provides a unique strategy for control of NRR in the production of valuable NH₃ .

Keywords: electrocatalysis; gold; nanoparticles; nitrogen reduction reaction; photoelectrochemistry.

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References

1. None
1. R. F. Service, Science 2014, 345, 610;
1. R. F. Service, Science 2018, 361, 120-123.
1. None
1. D. Bao, Q. Zhang, F. L. Meng, H. X. Zhong, M. M. Shi, Y. Zhang, J. M. Yan, Q. Jiang, X. B. Zhang, Adv. Mater. 2017, 29, 1604799;

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Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation

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Tuning the Electron Localization of Gold Enables the Control of Nitrogen-to-Ammonia Fixation

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