用于析氢反应的具有类铂活性的异质结钼基二元和三元氮化物催化剂,Chemical Engineering Journal |
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开发地球上储量丰富的具有类Pt催化活性的析氢反应(HER)电催化剂对于绿色制氢具有重要意义。本文描述了一种新策略,通过Ni 2+插层MoO 3纳米带(NB)的氮化来构建由Mo 2 N和Ni 0.2 Mo 0.8 N组成的双相氮化物纳米带。Mo 2 N/Ni 0.2 Mo 0.8 N催化剂表现出优异的稳定性和在10 mA cm -2下26 mV的低过电势和31 mV dec -1的塔菲尔斜率在碱性电解液和模拟海水中,其性能与基准 Pt/C 催化剂相当或更好。优异的碱性HER特性归因于Mo 2 N/Ni 0.2 Mo 0.8 N异质结构,其含量可调且界面牢固,并且在氮化过程中没有金属Ni偏析和结构崩溃。密度泛函理论 (DFT) 计算和实验表明,具有强电子相互作用的Mo 2 N/Ni 0.2 Mo 0.8 N 界面可优化 H 吸附/解吸,产生具有正 ΔG H*的中等弱键合金属位点作为催化中心,从而加速 HER 动力学并提高 HER 活性。结果揭示了一种制备具有类似 Pt 析氢活性的异质结构氮化物基催化剂的简单策略。
"点击查看英文标题和摘要" Heterojunction Mo-based binary and ternary nitride catalysts with Pt-like activity for the hydrogen evolution reaction
The development of earth-abundant electrocatalysts with Pt-like catalytic activity for the hydrogen evolution reaction (HER) is of great significance to green hydrogen production. Herein, a novel strategy is described to construct dual-phase nitride nanobelts composed of Mo2N and Ni0.2Mo0.8N by nitridation of Ni2+ intercalated layered MoO3 nanobelts (NBs). The Mo2N/Ni0.2Mo0.8N catalyst exhibits superior stability and a low overpotential of 26 mV at 10 mA cm−2 and Tafel slope of 31 mV dec−1 in both the alkaline electrolyte and simulated seawater, which is comparable to or better than that of the benchmark Pt/C catalyst. The excellent alkaline HER characteristics is attributed to the Mo2N/Ni0.2Mo0.8N heterostructure with adjustable content and robust interfaces and without metal Ni segregation and structure collapse during nitridation. Density-functional theory (DFT) calculations and experiments reveal that the Mo2N/Ni0.2Mo0.8N interface with strong electronic interactions optimizes H adsorption/desorption yielding moderately weak bonding metal sites with positive ΔGH* as the catalytic centers, thereby accelerating the HER kinetics and boosting the HER activity. The results reveal a simple strategy for the preparation of heterostructured nitride-based catalysts with Pt-like activity for hydrogen evolution. |
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