C60 Fullerenol to Stabilize and Activate Ru Nanoparticles for Highly Efficient Hydrogen Evolution Reaction in Alkaline Media,ACS Catalysis

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C60 Fullerenol to Stabilize and Activate Ru Nanoparticles for Highly Efficient Hydrogen Evolution Reaction in Alkaline Media
ACS Catalysis ( IF 11.3 ) Pub Date : 2023-05-22 , DOI: 10.1021/acscatal.3c01610
Yaozhou Li ₁ , Tingting Xu ₁ , Qi Huang ₁ , Longtao Zhu ₁ , Yingying Yan ₁ , Ping Peng ₁ , Fang-Fang Li ₁

Affiliation

Ruthenium (Ru)-based catalysts exhibited great potential for the alkaline hydrogen evolution reaction. However, the strong adsorption of H on the Ru surface and the undesirable agglomeration of Ru are obstacles to further boosting their hydrogen evolution reaction (HER) performance. Herein, we develop C₆₀ fullerenol C₆₀(OH)₂₄ to stabilize, disperse, and activate Ru nanoparticles through Ru–O–C₆₀ connections. Despite the ultrahigh Ru content (38.6 wt %), Ru nanoparticles are densely and uniformly dispersed on the C₆₀ substrate due to the anchoring and confinement effects of C₆₀ fullerenols. Moreover, the electron-withdrawing properties of C₆₀ induce the electrons to flow from Ru to C₆₀ through the Ru–O–C₆₀ interface, which enhances the electronic metal–support interaction, thereby optimizing the adsorption behavior of different intermediates. The synthesized Ru–OC₆₀-300 has a remarkably small overpotential (4.6 mV at 10 mA cm^–2) and Tafel slope (24.7 mV dec^–1), showing high activity and stability toward alkaline HER. Density functional theory simulations reveal that the Ru–O–C₆₀ interface engineering weakens the Ru–H affinity, promotes water dissociation, and accelerates the hydrogen evolution kinetics.

中文翻译：

C60 富勒烯醇可稳定和激活 Ru 纳米粒子，用于碱性介质中的高效析氢反应

钌 (Ru) 基催化剂在碱性析氢反应中表现出巨大的潜力。然而，H 在 Ru 表面的强烈吸附和 Ru 的不良团聚是进一步提高其析氢反应 (HER) 性能的障碍。在此，我们开发了 C ₆₀富勒烯醇 C ₆₀ (OH) _{24以通过 Ru–O–C}₆₀连接来稳定、分散和激活 Ru 纳米粒子。尽管 Ru 含量超高 (38.6 wt%)，但由于C ₆₀富勒烯醇的锚定和限制效应，Ru 纳米粒子致密且均匀地分散在 C ₆₀基底上。_{此外，C 60}的吸电子特性诱导电子通过Ru-O-C ₆₀界面从Ru流向C ₆₀，增强电子金属-载体相互作用，从而优化不同中间体的吸附行为。合成的 Ru–OC ₆₀ -300 具有非常小的过电势（在 10 mA cm ^–2时为 4.6 mV ）和 Tafel 斜率（24.7 mV dec ^–1），显示出对碱性 HER 的高活性和稳定性。密度泛函理论模拟表明，Ru-O-C ₆₀界面工程削弱了 Ru-H 亲和力，促进了水离解，并加速了析氢动力学。

更新日期：2023-05-22

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