Improving alkaline hydrogen evolution reaction kinetics on molybdenum carbide: Introducing Ru dopant
Improving alkaline hydrogen evolution reaction kinetics on molybdenum carbide: Introducing Ru dopant
复制标题
改善碳化钼的碱性析氢反应动力学：引入 Ru 掺杂剂
DOI：
10.1016/j.jcat.2020.10.020
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发表时间：
2020-12-01
影响因子：
7.3
通讯作者：
Wang, Yong
中科院分区：
文献类型：
--
作者：
Chen, Jiadong;Chen, Chunhong;Wang, Yong
碱性介质下的析氢反应（HER）在工业电催化制氢中发挥着关键作用，但即使是铂基电催化剂，由于水离解的高能垒，也存在高过电位和低动力学问题。在这里，通过采用原位生成的石墨氮化碳（g-C3N4）作为模板诱导层状结构的形成，我们报道了在超薄氮掺杂碳纳米片（RuMo2C/CN）上均匀分散的Ru掺杂Mo2C纳米颗粒作为高效碱性HER电催化剂。最优的Ru-Mo2C/CN表现出显着的活性，仅34 mV的低过电位即可提供10 mA cm(-2)，并且稳定性超过30 h，远优于商业Pt/C和最近在里程碑文献中报道的电催化剂。密度泛函理论（DFT）计算表明，Mo2C上引入的Ru掺杂剂显着降低了HER的水解离能垒，并抑制了H*和OH*在周围Mo位点上的竞争吸附。这项工作突出了一种简单而有效的策略，用于设计在碱性介质中具有优异析氢反应性能的电催化剂。 (C) 2020 Elsevier Inc. 保留所有权利。
Hydrogen evolution reaction (HER) under alkaline media plays a pivotal role in industrial electrocatalytic hydrogen production but even the platinum-based electrocatalysts suffer from high overpotential and low kinetics due to the high energy barrier of water dissociation. Here, by employing in-situ produced graphitic carbon nitride (g-C3N4) as template to induce the formation of a lamellar structure, we reported evenly dispersed Ru-doped Mo2C nanoparticles on ultrathin nitrogen-doped carbon nanosheets (RuMo2C/CN) as a highly efficient alkaline HER electrocatalyst. The optimal Ru-Mo2C/CN displays a remarkable activity with a low overpotential of only 34 mV to afford 10 mA cm(-2) and good stability of more than 30 h, which is much better than that of commercial Pt/C and recently reported electrocatalysts in the landmark literatures. Density functional theory (DFT) calculations show that the introduced Ru dopant on Mo2C significantly reduce the water dissociation energy barrier of HER and inhibit the competitive adsorption between H* and OH* on the surrounding Mo sites. This work highlights a simple yet effective strategy for designing electrocatalysts with excellent performance of hydrogen evolution reaction in alkaline media. (C) 2020 Elsevier Inc. All rights reserved.