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Electro-triggered Joule heating method to synthesize single-phase CuNi nano-alloy catalyst for efficient electrocatalytic nitrate reduction toward ammonia

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Abstract

Electrochemical nitrate reduction reaction (NO3RR) has great potential for ammonia (NH3) synthesis benefiting from its environmental friendliness and sustainability. Cu-based alloys with elemental diversity and adsorption tunability are widely used as electrocatalyst to lower the reaction overpotential for NO3RR catalysis. However, phase separation commonly found in alloys leads to uneven distribution of elements, which limits the possibility of further optimizing the catalytic activity. Herein, an electro-triggered Joule heating method, possessing unique superiority of flash heating and cooling that lead to well-dispersed nanoparticles and uniform mixing of various elements, was adopted to synthesize a single-phase CuNi nano-alloy catalyst evenly dispersed on carbon fiber paper, CFP-Cu1Ni1, which exhibited a more positive NO3RR initial potential of 0.1 V versus reversible hydrogen electrode (vs. RHE) than that of pure copper nanoparticles at 10 mA·cm−2 in 0.5 mol·L−1 Na2SO4 + 0.1 mol·L−1 KNO3 solution. Importantly, CFP-Cu1Ni1 presented high electrocatalytic activity with a Faradaic efficiency of 95.7% and NH3 yield rate of 180.58 µmol·h−1·cm−2 (2550 µmol·h−1·mg −1cat ) at −0.22 V vs. RHE. Theoretical calculations showed that alloying Cu with Ni into single-phase caused an upshift of its d-band center, which promoted the adsorption of NO −3 and weakened the adsorption of NH3. Moreover, the competitive adsorption of hydrogen ions was restrained until −0.24 V. This work offers a rational design concept with clear guidance for rapid synthesis of uniformly dispersed single-phase nano-alloy catalyst for efficient electrochemical NO3RR toward ammonia.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. U1804255 and U22A20253) and the Key Research & Development and Promotion Projects in Henan Province (Nos. 222102520038 and 212102310060). The computational resources were provided by Shanxi Supercomputing Center of China.

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  1. Zunjie Zhang and Yang Liu contributed equally to this work.

Authors and Affiliations

  1. School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang, 453007, China

    Zunjie Zhang, Yaling Zhao & Shuyan Gao

  2. School of Materials Science and Engineering, Henan Normal University, Xinxiang, 453007, China

    Yang Liu, Ziwei Zhao, Zhenkun Mo, Chenyi Wang, Ye Chen & Shuyan Gao

  3. Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, 201204, China

    Xiaozhi Su

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  1. Zunjie Zhang
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Electro-triggered Joule heating method to synthesize single-phase CuNi nano-alloy catalyst for efficient electrocatalytic nitrate reduction toward ammonia

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Zhang, Z., Liu, Y., Su, X. et al. Electro-triggered Joule heating method to synthesize single-phase CuNi nano-alloy catalyst for efficient electrocatalytic nitrate reduction toward ammonia. Nano Res. 16, 6632–6641 (2023). https://doi.org/10.1007/s12274-023-5402-y

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