Elucidating the Effect of Nitrogen Occupancy on the Hydrogen Evolution Reaction for a Series of Titanium Oxynitride Electrocatalysts
Elucidating the Effect of Nitrogen Occupancy on the Hydrogen Evolution Reaction for a Series of Titanium Oxynitride Electrocatalysts
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阐明氮占据对一系列氮氧化钛电催化剂析氢反应的影响
DOI：
10.1002/cctc.202300687
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发表时间：
2023
期刊：
影响因子：
4.5
通讯作者：
Yang G
中科院分区：
文献类型：
--
作者：
Yang G
氮化钛（TiN）显示出用作电催化剂和催化剂载体的理想性质，因为它具有高导电性和优异的耐腐蚀性。然而，氮化物晶格中的氧含量对其驱动析氢反应（HER）的能力的影响还没有很好地理解。本文采用氨解法制备了一系列具有不同氮占有率（0.53≤x≤1.0）的氮氧化钛（TiNxO 1-x）。它们对HER的比活性通过BET和电化学方法测定的表面积归一化。我们发现，这些氮氧化物的比活度与体氮占有率密切相关，尽管来自XPS分析的类似的表面组合物。此外，本体或表面处的氧含量的去除归因于在扩展计时电流法（CA）测试期间看到的升级的性能（高达25%的增加）。我们的研究结果表明，最大限度地减少这类材料中的体氧含量是实现HER的导电性和活性更高的材料的关键。
Titanium nitride (TiN) shows desirable properties for use as an electrocatalyst and catalyst support, as it possesses high electrical conductivity and excellent corrosion resistance. However, the effect of oxygen content in the nitride lattice on its ability to drive the hydrogen evolution reaction (HER) is not well understood. Here, a series of titanium oxynitrides (TiNxO1‐x) with varied nitrogen occupancy (0.53≤x≤1.0) in the bulk have been fabricated by ammonolysis. Their specific activities towards the HER were normalised by the surface areas determined by BET and electrochemical methods. We show that the specific activities of these oxynitrides are strongly correlated with the bulk nitrogen occupancy, despite the similar surface composition derived from XPS analysis. Furthermore, a removal of the oxygen content in the bulk or at the surface was attributed to the upgraded performance (up to 25 % increase) seen during extended chronoamperometry (CA) tests. Our results show that minimising bulk oxygen content in this class of material is critical to achieve a more conductive and active material for the HER.