Fullerene Lattice-Confined Ru Nanoparticles and Single Atoms Synergistically Boost Electrocatalytic Hydrogen Evolution Reaction,Advanced Functional Materials

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Fullerene Lattice-Confined Ru Nanoparticles and Single Atoms Synergistically Boost Electrocatalytic Hydrogen Evolution Reaction
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-01-05 , DOI: 10.1002/adfm.202213058
Tianmi Luo ₁ , Jianfeng Huang ₁ , Yuzhu Hu ₁ , Chengke Yuan ₁ , Junsheng Chen ₁ , Liyun Cao ₁ , Koji Kajiyoshi ₂ , Yijun Liu ₃ , Yong Zhao ₃ , Zhenjiang Li ₄ , Yongqiang Feng ₁

Affiliation

The design and construction of electrocatalysts with high efficiency, low cost and large current output suitable for industrial hydrogen production is the current development trend for water electrolysis. Herein, a lattice-confined in situ reduction effect of the 3D crystalline fullerene network (CFN) is developed to trap Ru nanoparticle (NP) and single atom (SA) via a solvothermal-pyrolysis process. The optimized product (Ru_NP-Ru_SA@CFN-800) exhibits outstanding electrocatalytic performance for alkaline hydrogen evolution reactions. To deliver a current density of 10 mA cm⁻², the Ru_NP-Ru_SA@CFN-800 merely required an overpotential of 33 mV, along with a robust electrocatalytic durability for 1400 h. Even at large current densities of 500 and 1000 mA cm⁻², the overpotentials are only 154 and 251 mV, respectively. Density function theorey calculation results indicated that the electronic synergetic effect between Ru NP and SA enable to regulate the charge distribution of Ru_NP-Ru_SA@CFN-800 and reduce the Gibbs free energy of intermediate species for water dissociation process, thereby accelerating the hydrogen evolution process. Moreover, the robust CFN matrix render this strategy patulous to other transition metals, e.g., Cu, Ni, and Co. The present study provides a new clue for the construction of novel electrocatalyst in the field of energy storage and conversion.

中文翻译：

富勒烯晶格限制的 Ru 纳米粒子和单原子协同促进电催化析氢反应

设计和构建适用于工业制氢的高效、低成本、大电流输出的电催化剂是当前水电解的发展趋势。在此，开发了 3D 结晶富勒烯网络 (CFN) 的晶格限制原位还原效应，以通过溶剂热-热解过程捕获 Ru 纳米颗粒 (NP) 和单原子 (SA)。优化后的产物 (Ru _NP -Ru _SA @CFN-800) 对碱性析氢反应表现出出色的电催化性能。^{为了提供 10 mA cm -2}的电流密度，Ru _NP -Ru _SA@CFN-800 仅需要 33 mV 的过电位，以及 1400 小时的强大电催化耐久性。即使在 500 和 1000 mA cm ^-2的大电流密度下，过电位也分别仅为 154 和 251 mV。密度函数理论计算结果表明，Ru NP和SA之间的电子协同作用能够调节Ru _NP -Ru _{SA的电荷分布}@CFN-800 降低水离解过程中中间物种的吉布斯自由能，从而加速析氢过程。此外，强大的 CFN 矩阵使该策略对其他过渡金属（例如 Cu、Ni 和 Co）具有扩展性。本研究为在能量存储和转换领域构建新型电催化剂提供了新线索。

更新日期：2023-01-05

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