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Integration of partially phosphatized bimetal centers into trifunctional catalyst for high-performance hydrogen production and flexible Zn-air battery

部分磷化双金属中心集成制备高性能三功能催化剂用于制氢和柔性锌-空气电池

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Abstract

The development of robust and efficient trifunctional catalysts showing excellent oxygen evolution reaction (OER), oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) kinetics has been challenging. Herein, we prepared a hybrid iron and cobalt-based metal alloy phosphide on a phosphorus and nitrogen co-doped carbon substrate (FeCo-P/PNC) as a catalyst using a one-step Pregulation method. The catalyst exhibited a positive half-wave potential of 0.86 V versus the reversible hydrogen electrode (RHE) for ORR, and low overpotentials of 350 and 158 mV for OER and HER, respectively, to achieve a current density of 10 mA cm-2. Density functional theory calculations demonstrated the dominant role of P in both FeCo phosphide and carbon matrix, which led to the good ORR, OER and HER kinetics. The assembled aqueous and flexible Zn-air batteries with FeCo-P/PNC as the air cathode displayed excellent peak power densities of 195.1 and 90.8 mW cm–2, respectively, as well as outstanding charging-discharging performance, long lifetime, and high flexibility. Moreover, the self-powered overall water-splitting cell exhibited a low working voltage of 1.71 V to achieve a current density of 10 mA cm-2, confirming its excellent multifunctional OER/ORR/HER activity.

摘要

摘要开发高效且性能稳定的氧析出(OER)、氧还原(ORR)和氢析出 (HER)三功能催化剂是制备能源存储与转换设备的关键. 本文使用一步 磷化法, 在氮磷共掺杂碳基上制备了FeCo金属合金/磷化物催化剂 (FeCo-P/PNC). 该催化剂显示了良好的ORR性能, 展现了0.86 V (vs. RHE, 相对于可逆氢电极)的半波电位; 在OER和HER反应中, 催化剂在 10 mA cm-2的电流密度下的过电位分别为350和158 mV. 密度泛函理 论计算表明, 磷在FeCo磷化物和碳基体中皆起主导作用, 使得该催化 剂同时具有良好的ORR、OER和HER功能. 以FeCo-P/PNC为空气阴极 组装的水系电池和柔性锌-空气电池的峰值功率密度分别为195.1和 90.8 mW cm-2, 且两种电池均具有优异的充放电性能、长寿命和高柔性. 此外, 自供能的整体水分解系统表现出较低的(1.71 V)工作电压以驱动10 mA cm-2的电流密度, 进一步证实了该催化剂出色的多功能性.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (22075211, 62005173 and 21601136), Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800), the Research Fund of State Key Laboratory for Marine Corrosion and Protection of Luoyang Ship Material Research Institute (LSMRI) under the contract No. KF190411, and the Science and Technology Development Fund of Tianjin Education Commission for Higher Education (2018KJ126). The authors also thank Beijing Super Cloud Computing Center for providing the computational resources and materials studio.

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Authors and Affiliations

  1. School of Chemical Engineering, Northeast Electric Power University, Jilin, 132012, China

    Miaosen Yang  (杨淼森)

  2. Nanchang Institute of Technology, Nanchang, 330044, China

    Miaosen Yang  (杨淼森)

  3. College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen, 518060, China

    Yifan Liu  (刘亦帆)

  4. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001, China

    Jiaqiang Sun  (孙甲强)

  5. College of Chemistry, Zhengzhou University, Zhengzhou, 450000, China

    Shusheng Zhang  (张书胜)

  6. Institute for New Energy Materials & Low-Carbon Technologies and Tianjin Key Lab for Photoelectric Materials & Devices, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin, 300384, China

    Xijun Liu  (刘熙俊) & Jun Luo  (罗俊)

  7. MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials, and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, School of Resource, Environments and Materials, Guangxi University, Nanning, 530004, China

    Xijun Liu  (刘熙俊)

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  1. Miaosen Yang  (杨淼森)
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Contributions

Liu X, Liu Y, and Zhang S designed the project; Yang M performed the experiments; Sun J and Luo J co-analyzed the data; Liu X, and Zhang S co-wrote the manuscript; Liu Y revised the manuscript. All the authors discussed and commented on the data and contributed to the manuscript.

Corresponding authors

Correspondence to Yifan Liu  (刘亦帆), Shusheng Zhang  (张书胜) or Xijun Liu  (刘熙俊).

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The authors declare that they have no conflict of interest.

Supplementary information

Supporting data are available in the online version of this paper.

Miaosen Yang received her PhD degree in chemical engineering and technology from Beijing University of Chemical Technology in 2012. Her current scientific interests focus on the design, preparation and application of inorganic functional materials and organic-inorganic composite materials.

Xijun Liu received his PhD degree from the College of Science, Beijing University of Chemical Technology in 2014. His current scientific interests focus on nanomaterials, heterogeneous catalysis, and materials design for catalysts and energy conversion/storage.

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40843_2021_1902_MOESM1_ESM.pdf

Integration of partially phosphatized bimetal centers into trifunctional catalyst for high-performance hydrogen production and flexible Zn-air battery

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Yang, M., Liu, Y., Sun, J. et al. Integration of partially phosphatized bimetal centers into trifunctional catalyst for high-performance hydrogen production and flexible Zn-air battery. Sci. China Mater. 65, 1176–1186 (2022). https://doi.org/10.1007/s40843-021-1902-2

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