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Copper oxide nanosheets for efficient electrochemical reduction of nitric oxide

纳米氧化铜片用于高效电化学还原一氧化氮

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  • Special Topic: Advanced Energy Catalytic Materials
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Abstract

The removal of nitric oxide (NO) is deemed essential due to its environmental detrimental effects, and electrocatalytic NO reduction reaction (NORR) for ammonia synthesis presents a sustainable approach. In this work, we synthesized copper oxide (CuO) nanosheet catalyst with a high specific surface area and abundant defects. This catalyst exhibited a remarkable 92.1% ammonia Faradaic efficiency (FE) in a flow cell, accompanied by a current density of 1.1 A cm−2 and an ammonia production rate of 7356 µmol cm−2 h−1 at −0.26 V vs. reversible hydrogen electrode. The FE of ammonia remained above 80% during stability test for 50 h at a current density of more than 400 mA cm−2. Quasi in situ X-ray photoelectron spectroscopy and in situ X-ray absorption spectroscopy revealed that the CuO nanosheets were electrochemically reduced to monomeric copper during NORR. Compared with Cu nanoparticles, the CuO nanosheets showed a high electrochemical surface area and high intrinsic activity for NORR.

摘要

一氧化氮电还原反应将工业废气转化为有价值的氨, 表现出极 具潜力的应用前景. 在本工作中, 我们合成了具有高比表面积和丰富缺 陷的氧化铜纳米片催化剂, 在流动池中氨法拉第效率达到92.1%, 在 −0.2 V vs. RHE时, 一氧化氮电还原电流密度和氨的生产速率分别达到 1.1 A cm−2和7356 µmol cm−2 h−1. 在电流密度超过400 m A cm−2 时, 氨 法拉第效率在50 小时保持在80%以上. 准原位X 射线光电子能谱和原 位X 射线吸收光谱结果表明氧化铜纳米片在一氧化氮电还原过程中被 电化学还原成单质铜. 与铜纳米颗粒相比, 氧化铜纳米片展现出较高的 电化学表面积和一氧化氮电还原的内在活性.

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Acknowledgements

This work was supported by the National Key R&D Program of China (2023YFA1508002), the National Natural Science Foundation of China (22125205 and 92015302), the Fundamental Research Funds for the Central Universities (20720220008), Dalian National Laboratory for Clean Energy (DNL201923), and the Photon Science Center for Carbon Neutrality. We thank staff at the BL14W1 beamline of Shanghai Synchrotron Radiation Facility for their technical assistance during the XAS measurements.

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Authors and Affiliations

  1. State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China

    Jiaqi Shao  (邵加奇), Pengfei Wei  (魏鹏飞), Shuo Wang  (王硕), Yanpeng Song  (宋延鹏), Yunfan Fu  (付云凡), Rongtan Li  (李荣坦), Xiaomin Zhang  (张小敏), Guoxiong Wang  (汪国雄) & Xinhe Bao  (包信和)

  2. University of Chinese Academy of Sciences, Beijing, 100049, China

    Jiaqi Shao  (邵加奇) & Yunfan Fu  (付云凡)

Authors
  1. Jiaqi Shao  (邵加奇)
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  2. Pengfei Wei  (魏鹏飞)
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  3. Shuo Wang  (王硕)
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  4. Yanpeng Song  (宋延鹏)
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  5. Yunfan Fu  (付云凡)
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  6. Rongtan Li  (李荣坦)
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  7. Xiaomin Zhang  (张小敏)
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  8. Guoxiong Wang  (汪国雄)
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  9. Xinhe Bao  (包信和)
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Contributions

Author contributions Shao J synthesized the catalysts and performed the electrochemical measurements and characterizations. Wei P conducted the XAFS experiments. Wang S, Song Y, Fu Y and Zhang X contributed to the data analysis. Li R helped with the XPS study. Wang G designed the work and revised the manuscript. All authors have given approval to the final version of the manuscript.

Corresponding author

Correspondence to Guoxiong Wang  (汪国雄).

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Conflict of interest The authors declare that they have no conflict of interest.

Additional information

Supplementary information Supporting data are available in the online version of the paper.

Jiaqi Shao is a PhD candidate in materials physics and chemistry at Dalian Institute of Chemical Physics, Chinese Academy of Sciences. He is dedicated to the design of advanced nanomaterials for electrochemical ammonia production from nitric oxide.

Guoxiong Wang is a professor in physical chemistry at Dalian Institute of Chemical Physics, Chinese Academy of Sciences. His research is electrocatalysis fundamentals and electrolysis technologies for fuels and chemicals production.

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Shao, J., Wei, P., Wang, S. et al. Copper oxide nanosheets for efficient electrochemical reduction of nitric oxide. Sci. China Mater. (2024). https://doi.org/10.1007/s40843-024-2830-5

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  • DOI: https://doi.org/10.1007/s40843-024-2830-5

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