Regulating the Coordination Environment of Ruthenium Cluster Catalysts for the Alkaline Hydrogen Evolution Reaction
Regulating the Coordination Environment of Ruthenium Cluster Catalysts for the Alkaline Hydrogen Evolution Reaction
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DOI：
10.1021/acs.jpclett.1c01936
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发表时间：
2021-08-17
影响因子：
5.7
通讯作者：
Yao, Tao
中科院分区：
文献类型：
--
作者：
Liu, Tong;Zhang, Wei;Yao, Tao
探索碱性环境下电化学析氢反应（HER）的高效催化剂是有吸引力的，但仍然具有挑战性。本文报道了一种协调调节策略，以调整Ti3C2Tx MXene负载的Ru簇催化剂（Ru-Ti3C2Tx）的原子结构。我们发现Ru-Ru的配位数（CN）可以通过调节合成温度从2.1略微调节到2.8，从而达到最佳的催化构型。CNRu-Ru为2.8的Ru-Ti3C2Tx表现出最佳的催化活性，在10 mA cm（-2）下过电位为96 mV，质量活性约为商用Pt/C催化剂的11.5倍。密度泛函理论计算表明，小Ru簇与Ti3C2Tx载体有较强的共价相互作用，导致最佳的δ GH*值。这项工作为调节HER催化剂的配位环境开辟了一条普遍的途径。
Exploring high-efficiency catalysts for the electrochemical hydrogen evolution reaction (HER) in alkaline environments is attractive but remains challenging. Here we report a coordination regulation strategy to tune the atomic structure of Ru cluster catalysts supported on Ti3C2Tx MXene (Ru-Ti3C2Tx) for the HER. We identify that the coordination number (CN) of Ru-Ru could be slightly regulated from 2.1 to 2.8 by adjusting the synthesized temperature so as to achieve an optimal catalytic configuration. The Ru-Ti3C2Tx with a CNRu-Ru of 2.8 exhibits the best catalytic activity with a low overpotential of 96 mV at 10 mA cm(-2) and a mass activity about 11.5 times greater than the commercial Pt/C catalyst. Density functional theory calculations demonstrated that the small Ru clusters have a stronger covalent interaction with Ti3C2Tx support leading to an optimal Delta GH* value. This work opens up a general avenue to modulate the coordination environment of catalysts for the HER.