Role of non-metallic atoms in enhancing the catalytic activity of nickel-based compounds for hydrogen evolution reaction†,Chemical Science

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Role of non-metallic atoms in enhancing the catalytic activity of nickel-based compounds for hydrogen evolution reaction†
Chemical Science ( IF 7.6 ) Pub Date : 2018-01-04 00:00:00 , DOI: 10.1039/c7sc04851c
Xingqun Zheng ₁ , Lishan Peng ₁ , Li Li ₁ , Na Yang ₁ , Yanjun Yang ₁ , Jing Li ₁ , Jianchuan Wang _{1,

2} , Zidong Wei ₁

Affiliation

The transition-metal compounds (MX) have gained wide attention as hydrogen evolution reaction (HER) electrocatalysts; however, the interaction between the non-metallic atom (X) and the metal atom (M) in MX, and the role of X in the enhanced catalytic activity of MX, are still ambiguous. In this work, we constructed a simple model [X/Ni(100)] to decipher the contribution of X towards enhancing the catalytic activity of NiX, which allows us to accurately predict the trend in HER catalytic activity of NiX based on the easily accessible physico-chemical characteristics of X. Theoretical calculations showed that the electronegativity (χ_X) and the principle quantum number (n_X) of X are two important descriptors for evaluating and predicting the HER catalytic activity of NiX catalysts effectively. X atoms in the VIA group can enhance the HER activity of X/Ni(100) more significantly than those in the second period due to the large χ_X or n_X. At a relatively low X coverage, the S/Ni(100) possesses the best HER activity among all of the discussed X/Ni(100) models, and the optimum surface S : Ni atomic ratio is about 22–33%. Further experiments demonstrated that the Ni–Ni₃S₂ catalyst with a surface S : Ni atomic ratio of 28.9% exhibits the best catalytic activity and lowest charge transfer resistance. The trend in catalytic activity of NiX with differing X offers a new possible strategy to exploit MX materials and design new active catalysts rationally.

中文翻译：

非金属原子在增强镍基化合物析氢反应催化活性中的作用†

过渡金属化合物（MX）作为析氢反应（HER）电催化剂受到广泛关注；然而，MX中非金属原子(X)和金属原子(M)之间的相互作用，以及X在增强MX催化活性中的作用仍然不明确。在这项工作中，我们构建了一个简单的模型 [X/Ni(100)] 来解读 X 对增强 NiX 催化活性的贡献，这使我们能够根据易于获取的数据准确预测 NiX HER 催化活性的趋势理论计算表明，X的电负性（χ _X）和主量子数（n _X）是有效评估和预测NiX催化剂HER催化活性的两个重要描述符。_{由于较大的 χ X}或n _X，VIA基团中的X原子比第二阶段的X原子更能显着增强X/Ni(100)的HER活性。在相对较低的X覆盖率下，S/Ni(100)在所有讨论的X/Ni(100)模型中具有最好的HER活性，并且最佳表面S:Ni原子比约为22-33%。进一步的实验表明，表面S:Ni原子比为28.9%的Ni-Ni ₃ S ₂催化剂表现出最好的催化活性和最低的电荷转移阻力。不同X的NiX催化活性的趋势为开发MX材料和合理设计新型活性催化剂提供了新的可能策略。

更新日期：2018-01-04

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