Mixed Close-Packed Cobalt Molybdenum Nitrides as Non-noble Metal Electrocatalysts for the Hydrogen Evolution Reaction,Journal of the American Chemical Society

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Mixed Close-Packed Cobalt Molybdenum Nitrides as Non-noble Metal Electrocatalysts for the Hydrogen Evolution Reaction
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2013-12-11 , DOI: 10.1021/ja4081056
Bingfei Cao _{1,

2} , Gabriel M. Veith , Joerg C. Neuefeind , Radoslav R. Adzic ₂ , Peter G. Khalifah _{1,

2}

Affiliation

A two-step solid-state reaction for preparing cobalt molybdenum nitride with a nanoscale morphology has been used to produce a highly active and stable electrocatalyst for the hydrogen evolution reaction (HER) under acidic conditions that achieves an iR-corrected current density of 10 mA cm(-2) at -0.20 V vs RHE at low catalyst loadings of 0.24 mg/cm(2) in rotating disk experiments under a H2 atmosphere. Neutron powder diffraction and pair distribution function (PDF) studies have been used to overcome the insensitivity of X-ray diffraction data to different transition-metal nitride structural polytypes and show that this cobalt molybdenum nitride crystallizes in space group P63/mmc with lattice parameters of a = 2.85176(2) Å and c = 10.9862(3) Å and a formula of Co0.6Mo1.4N2. This space group results from the four-layered stacking sequence of a mixed close-packed structure with alternating layers of transition metals in octahedral and trigonal prismatic coordination and is a structure type for which HER activity has not previously been reported. Based on the accurate bond distances obtained from time-of-flight neutron diffraction data, it is determined that the octahedral sites contain a mixture of divalent Co and trivalent Mo, while the trigonal prismatic sites contain Mo in a higher oxidation state. X-ray photoelectron spectroscopy (XPS) studies confirm that at the sample surface nitrogen is present and N-H moieties are abundant.

中文翻译：

混合密堆积钴钼氮化物作为非贵金属电催化剂用于析氢反应

用于制备具有纳米级形态的钴钼氮化物的两步固态反应已被用于在酸性条件下为析氢反应 (HER) 生产高活性和稳定的电催化剂，该反应可实现 10 mA 的 iR 校正电流密度cm(-2) 在 -0.20 V 与 RHE 在 0.24 mg/cm(2) 的低催化剂负载下在 H2 气氛下的旋转圆盘实验中。中子粉末衍射和对分布函数 (PDF) 研究已被用于克服 X 射线衍射数据对不同过渡金属氮化物结构多型体的不敏感性，并表明这种氮化钴钼在 P63/mmc 空间群中结晶，晶格参数为a = 2.85176(2) Å 和 c = 10.9862(3) Å 以及 Co0.6Mo1.4N2 的分子式。该空间群是由混合密堆积结构的四层堆叠序列产生的，其中过渡金属层以八面体和三棱柱配位交替排列，是一种先前未报道过 HER 活性的结构类型。基于从飞行时间中子衍射数据获得的准确键距，确定八面体位点包含二价 Co 和三价 Mo 的混合物，而三棱柱位点包含更高氧化态的 Mo。X 射线光电子能谱 (XPS) 研究证实，样品表面存在氮且 NH 部分丰富。

更新日期：2013-12-11

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