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Electron deficiency modulates hydrogen adsorption strength of Ru single-atomic catalyst for efficient hydrogen evolution

Author

Listed:
  • Cao, Baoyue
  • Shi, Hu
  • Sun, Qiangqiang
  • Yu, Yan
  • Chang, Liangliang
  • Xu, Shan
  • Zhou, Chunsheng
  • Zhang, Hongxia
  • Zhao, Jianghong
  • Zhu, Yanyan
  • Yang, Pengju

Abstract

It was found that the Na modification is beneficial to the synthesis of Ru single-atomic catalyst anchored on GONa, which was prepared by one-step hydrothermal process. Importantly, the strong metal-support interaction facilitates the electron transfer from Ru SA to GONa via d-π conjugation, thus lowering the electron density of Ru SA. Experimental results and DFT calculations confirmed that the low electron density of Ru SA can significantly weaken the absorption of H* intermediates and simultaneously accelerate the desorption of generated H2 from catalyst surface. As a result, the Ru SA/GONa displayed exceptional HER activity with an extremely low over-potential of 20 mV at 10 mA cm−2, outperforming the benchmark commercial Pt (21 mV over-potential) and Ru nanoparticles (212 mV over-potential) catalysts. When Eosin Y was employed as a light harvester, this Ru SA/GONa achieves outstanding photocatalytic hydrogen production with a record-high apparent quantum efficiency of 65.2% at 520 nm. Moreover, single-atomic Pt, Pd, Au and Rh were also successfully anchored on the Na-functionalized GO support, suggesting the universality of Na-induced single-atomic synthesis. This work not only provides an effective method for the synthesis of single-atomic metal catalysts but also establishes the connection between the electronic structures of catalyst and performances.

Suggested Citation

  • Cao, Baoyue & Shi, Hu & Sun, Qiangqiang & Yu, Yan & Chang, Liangliang & Xu, Shan & Zhou, Chunsheng & Zhang, Hongxia & Zhao, Jianghong & Zhu, Yanyan & Yang, Pengju, 2023. "Electron deficiency modulates hydrogen adsorption strength of Ru single-atomic catalyst for efficient hydrogen evolution," Renewable Energy, Elsevier, vol. 210(C), pages 258-268.
  • Handle: RePEc:eee:renene:v:210:y:2023:i:c:p:258-268
    DOI: 10.1016/j.renene.2023.03.136
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    References listed on IDEAS

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    1. Jianwei Su & Yang Yang & Guoliang Xia & Jitang Chen & Peng Jiang & Qianwang Chen, 2017. "Erratum: Ruthenium-cobalt nanoalloys encapsulated in nitrogen-doped graphene as active electrocatalysts for producing hydrogen in alkaline media," Nature Communications, Nature, vol. 8(1), pages 1-1, December.
    2. Jianwei Su & Yang Yang & Guoliang Xia & Jitang Chen & Peng Jiang & Qianwang Chen, 2017. "Correction: Corrigendum: Ruthenium-cobalt nanoalloys encapsulated in nitrogen-doped graphene as active electrocatalysts for producing hydrogen in alkaline media," Nature Communications, Nature, vol. 8(1), pages 1-1, December.
    3. Jianwei Su & Yang Yang & Guoliang Xia & Jitang Chen & Peng Jiang & Qianwang Chen, 2017. "Ruthenium-cobalt nanoalloys encapsulated in nitrogen-doped graphene as active electrocatalysts for producing hydrogen in alkaline media," Nature Communications, Nature, vol. 8(1), pages 1-12, April.
    4. Lili Zhu & Haiping Lin & Youyong Li & Fan Liao & Yeshayahu Lifshitz & Minqi Sheng & Shuit-Tong Lee & Mingwang Shao, 2016. "A rhodium/silicon co-electrocatalyst design concept to surpass platinum hydrogen evolution activity at high overpotentials," Nature Communications, Nature, vol. 7(1), pages 1-7, November.
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