Amorphous phosphatized ruthenium-iron bimetallic nanoclusters with Pt-like activity for hydrogen evolution reaction
Amorphous phosphatized ruthenium-iron bimetallic nanoclusters with Pt-like activity for hydrogen evolution reaction
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DOI：
10.1016/j.apcatb.2020.119583
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发表时间：
2021-04
影响因子：
22.1
通讯作者：
Beibei Yang;Junyuan Xu;Duan Bin;Jin Wang;Jinzhi Zhao;Yixin Liu;Binxiao Li;Xiaoni Fang;Yun Liu
中科院分区：
文献类型：
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作者：
Beibei Yang;Junyuan Xu;Duan Bin;Jin Wang;Jinzhi Zhao;Yixin Liu;Binxiao Li;Xiaoni Fang;Yun Liu
过渡金属磷化物（TMPs）作为一种高效、耐用的析氢反应电催化剂，受到了广泛的关注。然而，对于TMPs来说，要达到与最先进的铂（Pt）催化剂相似的HER性能仍然是一个挑战。在此，我们报道了一种新的基于石墨化碳纳米纤维（CNF）的非晶磷化钌铁双金属纳米团簇（RuxFeyP-NCs），通过简单的两步法合成，结合了几种催化剂设计策略的优点。无定形结构允许更多的催化活性位点暴露，Ru和Fe之间的协同作用可能提高本构催化活性。此外，导电CNF支持促进电子传递并牢固地固定ruxfep - nc，从而实现长期稳定性。ruxfep - ncs /CNF具有最佳等摩尔Ru和Fe（即RuFeP-NCs/CNF），表现出优异的pt类HER性能，在酸性和碱性溶液中分别需要65.8和16.0 mV的低过电位才能提供10 mA cm - 2的电流密度，并表现出100 h的长期稳定性。密度功能理论（DFT）计算表明，RuFeP-NCs/CNF的氢吸附吉布斯自由能接近Pt，远小于FeP-NCs/CNF和RuxFey-NCs/CNF非等量Ru/Fe对照，这合理地解释了RuFeP-NCs/CNF具有突出的HER性能。
Transition metallic phosphides (TMPs) have attracted considerable attention for use as efficient and durable electrocatalysts for the hydrogen evolution reaction (HER). However, it is still challenging for TMPs to achieve HER performance similar to that of the state-of-the-art platinum (Pt) catalysts. Herein, we report new amorphous phosphatized ruthenium-iron bimetallic nanoclusters (RuxFeyP-NCs) supported on graphitized carbon nanofibers (CNF), synthesized through a facile two-step method, which combine the merits of several catalyst design strategies. The amorphous structure allows more catalytically active sites to be exposed, and the synergy between Ru and Fe may boost the intrinsic catalytic activity. Moreover, the conductive CNF support facilitates electron transport and firmly immobilizes RuxFeyP-NCs enabling a long-term stability. The resulting RuxFeyP-NCs/CNF with optimal equimolar Ru and Fe (i.e. RuFeP-NCs/CNF) exhibits outstanding Pt-like HER performance, requiring low overpotentials of 65.8 and 16.0 mV to deliver a current density of 10 mA cm−2in acidic and alkaline solutions, respectively, and showing a long-term stability of 100 h. The density functional theory (DFT) calculations demonstrate that RuFeP-NCs/CNF shows Gibbs free energy of hydrogen adsorption close to that of Pt and much smaller than that of FeP-NCs/CNF and RuxFey-NCs/CNF controls with non-equimolar Ru/Fe, which rationally explains the experimentally observed prominent HER performance of RuFeP-NCs/CNF.