通过同核双原子催化剂的异源化了解高性能电催化固氮的内在机制

IF 13 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Yuefei Zhang, Yu Yang, Yu Zhang, Xuefei Liu, Wenjun Xiao, Degui Wang, Gang Wang, Zhen Wang, Jinshun Bi, Jincheng Liu, Xun Zhou, Wentao Wang
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引用次数: 0

摘要

异核双过渡金属原子催化剂是解决和缓解日益严重的能源和环境危机的一种可行策略。然而,在考虑异核诱导原子差异对各过渡金属原子的影响时,由于各过渡金属原子在协同催化过程中活性高但可探测性低,因此仍无法有效区分各原子的作用,从而严重阻碍了内在机理的发现。在此,我们提出了同核双过渡金属的坐标环境变化诱导异质化,既继承了异核过渡金属原子催化的优势,又控制了两个原子的变量,从而探索其内在机理。在此基础上,利用密度泛函理论研究和机器学习,在四种不对称 C3N 中掺杂了 23 种同核过渡金属进行异质化,以评估其催化机理。结果表明,五种催化剂的催化性能优异,极限电位低至-0.28 至-0.48 V。同时,针对侧向和端向构型,我们提出了 "捕获-电荷分布-捕获-电荷再分布 "的新机制。更重要的是,根据这一机制确定了第一次氢化的代酸位点。我们的工作不仅初步加深了对过渡双金属基异核催化剂的间接理解,而且拓宽了未来复杂同核双原子催化剂的发展方向。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Understanding the Intrinsic Mechanism of High-Performance Electrocatalytic Nitrogen Fixation by Heterogenization of Homonuclear Dual-Atom Catalysts

Understanding the Intrinsic Mechanism of High-Performance Electrocatalytic Nitrogen Fixation by Heterogenization of Homonuclear Dual-Atom Catalysts
A heteronuclear dual transition metal atom catalyst is a promising strategy to solve and relieve the increasing energy and environment crisis. However, the role of each atom still does not efficiently differentiate due to the high activity but low detectability of each transition metal in the synergistic catalytic process when considering the influence of heteronuclear induced atomic difference for each transition metal atom, thus seriously hindering intrinsic mechanism finding. Herein, we proposed coordinate environment vary induced heterogenization of homonuclear dual-transition metal, which inherits the advantage of heteronuclear transition metal atom catalyst but also controls the variable of the two atoms to explore the underlying mechanism. Based on this proposal, employing density functional theory study and machine learning, 23 kinds of homonuclear transition metals are doping in four asymmetric C3N for heterogenization to evaluate the underlying catalytic mechanism. Our results demonstrate that five catalysts exhibit excellent catalytic performance with a low limiting potential of −0.28 to −0.48 V. In the meantime, a new mechanism, “capture–charge distribution–recapture–charge redistribution”, is developed for both side-on and end-on configuration. More importantly, the pronate site of the first hydrogenation is identified based on this mechanism. Our work not only initially makes a deep understanding of the transition dual metal-based heteronuclear catalyst indirectly but also broadens the development of complicated homonuclear dual-atom catalysts in the future.
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来源期刊
Energy & Environmental Materials
Energy & Environmental Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
17.60
自引率
6.00%
发文量
66
期刊介绍: Energy & Environmental Materials (EEM) is an international journal published by Zhengzhou University in collaboration with John Wiley & Sons, Inc. The journal aims to publish high quality research related to materials for energy harvesting, conversion, storage, and transport, as well as for creating a cleaner environment. EEM welcomes research work of significant general interest that has a high impact on society-relevant technological advances. The scope of the journal is intentionally broad, recognizing the complexity of issues and challenges related to energy and environmental materials. Therefore, interdisciplinary work across basic science and engineering disciplines is particularly encouraged. The areas covered by the journal include, but are not limited to, materials and composites for photovoltaics and photoelectrochemistry, bioprocessing, batteries, fuel cells, supercapacitors, clean air, and devices with multifunctionality. The readership of the journal includes chemical, physical, biological, materials, and environmental scientists and engineers from academia, industry, and policy-making.
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