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Temperature-controlled synthesis of heterostructured Ru-Ru2P nanoparticles embedded in carbon nanofibers for highly efficient hydrogen production

温度调控合成异质结构Ru-Ru2P纳米颗粒负载碳纳 米纤维用于高效电催化析氢反应

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Abstract

Developing highly efficient, cost-effective, and stable electrocatalysts for hydrogen evolution reaction (HER) is of considerable importance but remains challenging. Herein, we report the fabrication of a robust Ru-based electrocatalyst, which comprises heterostructured Ru-Ru2P nanoparticles that are embedded in the N,P-codoped carbon nanofibers (CNFs), through a synthetic strategy involving electrospinning and temperature-controlled pyrolysis treatment. The as-prepared Ru-Ru2P catalyst (Ru-Ru2P@CNFs) shows excellent HER catalytic activities with low overpotentials of 11 and 14 mV in acidic and alkaline media, respectively, to achieve a current density of 10 mA cm−2, which are superior to the individual components of pure Ru and Ru2P catalysts. Density functional theory calculations demonstrate the existence of electronic coupling effect between Ru and Ru2P at the heterointerfaces, leading to a well-modulated electronic structure with optimized hydrogen adsorption strength and enhanced electrical conductivity for efficient HER electrocatalysis. In addition, the overall synthetic strategy can be generalized for the synthesis of a series of transitional metal phosphide-based nanofibers, thereby holding a remarkable capacity for various potential applications.

摘要

开发高效、低价、稳定的析氢催化剂是实现电解水制氢规模产 业化的关键, 但仍面临巨大挑战. 在本文中, 我们通过静电纺丝和控温 热处理的合成路径制备了一种高活性Ru基催化剂材料, 该催化剂由异 质结构Ru-Ru2P纳米颗粒均匀负载于N、P共掺杂碳纳米纤维构成. 所 制备的Ru-Ru2P异质催化剂表现出优异的电催化析氢活性, 在酸性和碱 性电解液中产生10 mA cm−2的催化电流密度分别仅需11和14 mV的过 电位, 其性能优于对比样品纯Ru和纯Ru2P催化剂. 密度泛函理论计算结 果表明在Ru和Ru2P的异质界面处存在电子耦合效应, 从而有效调控催 化剂界面电子结构, 优化活性位点氢吸附能并提高导电性, 实现了高效 电催化析氢. 本合成策略适用于制备一系列过渡金属磷化物纳米纤维, 因而在催化和储能等领域具有广泛的应用前景.

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Acknowledgements

This work was financially supported by the Natural Science Foundation of Zhejiang Province (LQ20B030001 and LY20E020002) and China Postdoctoral Science Foundation (2021M702305).

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Authors and Affiliations

  1. School of Materials Science and Engineering, Zhejiang Sci-Tech University, Hangzhou, 310018, China

    Yue Wei  (韦悦), Yujie Wei  (韦渝洁), Lvlv Ji  (纪律律), Tao Wang  (王騊) & Sheng Wang  (王晟)

  2. Department of Physics, Shaoxing University, Shaoxing, 312000, China

    Gao Xu  (徐杲) & Zhun Liu  (刘准)

Authors
  1. Yue Wei  (韦悦)
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  2. Gao Xu  (徐杲)
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  3. Yujie Wei  (韦渝洁)
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  5. Tao Wang  (王騊)
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  6. Zhun Liu  (刘准)
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  7. Sheng Wang  (王晟)
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Contributions

Wei Y conducted the experiment and wrote the paper. Xu G conducted the DFT calculations and analyzed the data; Wei Y and Wang T did some characterizations; Ji L, Liu Z, and Wang S supervised this study and revised the paper. All authors contributed to the general discussion.

Corresponding authors

Correspondence to Lvlv Ji  (纪律律), Zhun Liu  (刘准) or Sheng Wang  (王晟).

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Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary information

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

Yue Wei received her BSc degree from Hubei Engineering University in 2019. She is currently an MSc degree student under the supervision of Prof. Sheng Wang and Dr. Lvlv Ji at Zhejiang Sci-Tech University. Her research interests focus on the nanofibrous materials for electrocatalytic hydrogen production.

Lvlv Ji is currently a lecturer at Zhejiang Sci-Tech University. He received his BSc degree from Huainan Normal University in 2012, MSc degree from Zhejiang University of Technology in 2015, and PhD degree from Tongji University in 2018. His research interests focus on electrocatalysis, and energy storage and conversion.

Zhun Liu received his PhD degree from Beijing University of Technology in 2017. He worked as an assistant researcher at Jilin University from 2017 to 2019, and then worked at the South China Normal University from 2019 to 2021. He joined the Department of Physics, Shaoxing University in 2021. His research interests focus on electronic materials and their devices for energy conversion, information functional materials, and computational materials science.

Sheng Wang received his PhD degree from Fukui University, Japan in 2003, and then worked as assistant lecturer at Hokkaido University for three years. He joined Zhejiang Sci-Tech University in 2006 and was promoted to a full professor in 2013. His research interests include nano photocatalysis, bio-inspired strategies for functional nanomaterials, and micro/nano fibrous composites.

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40843_2022_2001_MOESM1_ESM.pdf

Temperature-controlled synthesis of heterostructured Ru-Ru2P nanoparticles embedded in carbon nanofibers for highly efficient hydrogen production

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Wei, Y., Xu, G., Wei, Y. et al. Temperature-controlled synthesis of heterostructured Ru-Ru2P nanoparticles embedded in carbon nanofibers for highly efficient hydrogen production. Sci. China Mater. 65, 2675–2684 (2022). https://doi.org/10.1007/s40843-022-2001-7

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  • DOI: https://doi.org/10.1007/s40843-022-2001-7

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