Nanostructured Ternary Nickel‐Based Mixed Anionic (Telluro)‐Selenide as a Superior Catalyst for Oxygen Evolution Reaction
Nanostructured Ternary Nickel‐Based Mixed Anionic (Telluro)‐Selenide as a Superior Catalyst for Oxygen Evolution Reaction
复制标题
纳米结构三元镍基混合阴离子 (Telluro) 硒化物作为析氧反应的优质催化剂
DOI：
10.1002/ente.202300177
复制
发表时间：
2023
影响因子：
3.8
通讯作者：
Nath, Manashi
中科院分区：
文献类型：
--
作者：
Abdullahi, Ibrahim Munkaila;Thomas, Siby;Gagliardi, Alessio;Zaeem, Mohsen Asle;Nath, Manashi
开发设计高效、耐用、经济高效的析氧反应电催化剂(OER)的方案需要更深入地了解作为组成函数的结构-性能相关性。在这里，已经证明，在二元硫化物镍(NiSE)中掺入Te并产生混合阴离子相会扰乱其电子结构，并显著提高OER活性。采用简单的水热合成方法，在具有不同形貌的泡沫镍上， 原位生长了一系列具有层层结构和混合阴离子三元相的纳米结构镍硫化物。综合的X射线衍射、X射线光电子能谱和 原位拉曼光谱分析证实，形成了一种真正混合的阴离子组成的三角单相纳米晶镍(碲)-硒(NiSeTe)。NiSeTe电催化剂表现出良好的过电流变性能，在50 mA cm−2时，过电位为300 mV，在1mKOH电解液中，Tafel斜率为98 mV −1。其周转频率和质量活度分别为0.047 S−1和90.3 Ag−1。详细的电化学测量还显示，与二元混合物相比，NiSeTe相的电荷转移性能更强。密度泛函理论计算表明，与二元硫族化合物相比，混合阴离子相具有更好的OH吸附能，从而证实了其优异的电催化性能。
Developing protocols for designing high‐efficiency, durable, cost‐effective electrocatalysts for oxygen evolution reaction (OER) necessitates deeper understanding of structure–property correlation as a function of composition. Herein, it has been demonstrated that incorporating tellurium into binary nickel chalcogenide (NiSe) and creating a mixed anionic phase perturbs its electronic structure and significantly enhances the OER activity. A series of nanostructured nickel chalcogenides comprising a layer‐by‐layer morphology along with mixed anionic ternary phase are grown in situ on nickel foam with varying morphological textures using simple hydrothermal synthesis route. Comprehensive X‐ray diffraction, X‐ray photoelectron spectroscopy, and in situ Raman spectroscopy analysis confirms the formation of a trigonal single‐phase nanocrystalline nickel (telluro)‐selenide (NiSeTe) as a truly mixed anionic composition. The NiSeTe electrocatalyst exhibits excellent OER performance, with a low overpotential of 300 mV at 50 mA cm−2and a small Tafel slope of 98 mV dec−1in 1mKOH electrolyte. The turnover frequency and mass activity are 0.047 s−1and 90.3 Ag−1, respectively. Detailed electrochemical measurements also reveal enhanced charge transfer properties of the NiSeTe phase compared to the mixture of binaries. Density functional theory calculations reveal favorable OH adsorption energy in the mixed anionic phase compared to the binary chalcogenides confirming superior electrocatalytic property.