Frederik C. Østergaard , Frank Abild-Pedersen , Jan Rossmeisl
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引用次数: 0
摘要
在 IrPdPtRhRu(1 1 1) 高熵合金上建立氢进化反应(HER)活性概率模型。基于配体效应和广义氢-氢排斥力确定氢覆盖率。为了寻找最佳催化特性,高熵合金(HEA)是利用多种元素组成空间的有前途的候选材料。根据对具有一系列氢覆盖率的 HEA 模型 (1 1 1) 表面的模拟,结合能分布被用来构建一个框架,该框架近似地表示吸附氢可能导致形成 H2 的概率与应用电势的函数关系。通过优化合金成分,使其在给定电势下具有最高的活性概率,从而确定最佳和最有效的 HER 候选催化剂。在分别处理氢-氢排斥效应和结合能时,我们发现氢-氢排斥效应对于 HEAs 比对于纯金属更大。平均吸附能和解吸能的等温线斜率不同,这表明氢吸收在 HEAs 上可能存在滞后现象。
Coverage, repulsion, and reactivity of hydrogen on High-Entropy alloys
Modeling hydrogen evolution reaction (HER) activity probability on IrPdPtRhRu(1 1 1) high-entropy alloys. Determining hydrogen coverages based on ligand effects and generalized hydrogen–hydrogen repulsion.
The rate of H2 formation is highly impacted by the level of hydrogen coverage on the catalyst surface. In search of optimal catalytic properties high-entropy alloys (HEA) are promising candidates that utilize the compositional space of multiple elements. Based on simulations of HEA model (1 1 1) surfaces with a range of hydrogen coverages, distributions of binding energies are used to construct a framework that approximates the probability that adsorbed hydrogen may lead to the formation of H2 as a function of applied potential. By optimizing the alloy compositions for the highest activity probability at given potentials the best and most efficient catalyst candidates for HER can be identified. Treating hydrogen–hydrogen repulsion effects and binding energy separately, we find that the repulsion is larger for HEAs than for pure metals. Differing isotherm slopes in the mean adsorption and desorption energies demonstrate a possible hysteresis for hydrogen adsorption on HEAs.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.