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Electrochemical nitrogen reduction reaction (NRR) under ambient conditions is highly desirable to achieve sustainable ammonia (NH3) production via an alternative carbon free strategy. Single-atom catalysts (SACs) with super high atomic utilization and catalytic efficiency exhibit great potential for NRR. Herein, a high-performance NRR SAC is facilely prepared via a simple deposition method to anchor Au single atoms onto porous β-FeOOH nanotubes. The resulting Au-SA/FeOOH can efficiently drive NRR under ambient conditions, and the NH3 yield reaches as high as 2,860 μg·h−1·mgAu−1 at −0.4 V vs. reversible hydrogen electrode (RHE) with 14.2% faradaic efficiency, much superior to those of all the reported Au-based electrocatalysts. Systematic investigations demonstrate that the synergy of much enhanced N2 adsorption, directional electron export, and mass transfer ability in Au-SA/FeOOH greatly contributes to the superior NRR activity. This work highlights a new insight into the design of high efficient NRR electrocatalysts by combination of porous metal oxide matrix and highly active single-atom sites.


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Porous β-FeOOH nanotube stabilizing Au single atom for high-efficiency nitrogen fixation

Show Author's information Hao Sun1,§Hua-Qing Yin1,§Wenxiong Shi1,§Lu-Lu Yang1Xiang-Wei Guo1Hong Lin1Jiangwei Zhang2( )Tong-Bu Lu1Zhi-Ming Zhang( )
Institute for New Energy Materials & Low Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin 300384, China
Dalian National Laboratory for Clean Energy & State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences (CAS), Dalian 116023, China

§ Hao Sun, Hua-Qing Yin, and Wenxiong Shi contributed equally to this work.

Abstract

Electrochemical nitrogen reduction reaction (NRR) under ambient conditions is highly desirable to achieve sustainable ammonia (NH3) production via an alternative carbon free strategy. Single-atom catalysts (SACs) with super high atomic utilization and catalytic efficiency exhibit great potential for NRR. Herein, a high-performance NRR SAC is facilely prepared via a simple deposition method to anchor Au single atoms onto porous β-FeOOH nanotubes. The resulting Au-SA/FeOOH can efficiently drive NRR under ambient conditions, and the NH3 yield reaches as high as 2,860 μg·h−1·mgAu−1 at −0.4 V vs. reversible hydrogen electrode (RHE) with 14.2% faradaic efficiency, much superior to those of all the reported Au-based electrocatalysts. Systematic investigations demonstrate that the synergy of much enhanced N2 adsorption, directional electron export, and mass transfer ability in Au-SA/FeOOH greatly contributes to the superior NRR activity. This work highlights a new insight into the design of high efficient NRR electrocatalysts by combination of porous metal oxide matrix and highly active single-atom sites.

Keywords: electrocatalysis, single atom, dinitrogen (N2) reduction , porous iron oxyhydroxide

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Publication history
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Acknowledgements

Publication history

Received: 27 September 2021
Revised: 13 October 2021
Accepted: 14 October 2021
Published: 18 November 2021
Issue date: April 2022

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© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2021

Acknowledgements

Acknowledgements

This work was supported by the Natural Science Foundation of Tianjin City of China (No. 18JCJQJC47700), the Key Laboratory of Resource Chemistry of Chinese Ministry of Education (No. KLRC_ME1902), the Opening Project of Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Chinese Ministry of Education, the National Natural Science Foundation of China (No. 21701168), Dalian high level talent innovation project (No. 2019RQ063), the Open Project Foundation of State Key Laboratory of Structural Chemistry, and Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (No. 20200021). We gratefully acknowledge the BL14W1 beamline station of Shanghai Synchrotron Radiation Facility (SSRF) for providing the beam time.

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