在锂-S 电池中通过筛选描述符定制过渡金属双原子催化剂

IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
ACS Nano Pub Date : 2024-12-11 DOI:10.1021/acsnano.4c12536
Yifei Wang, Conglei Xu, Beibei Li, Meng Tian, Mu Liu, Daming Zhu, Shixue Dou, Qiang Zhang, Jingyu Sun
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引用次数: 0

摘要

硫还原反应(SRR)中多硫化物的吸附-转化模式对解决Li-S电池中的穿梭效应很有吸引力,特别是基于原子分散的电催化剂。然而,对这种催化系统的机理见解仍然不明确,限制了对硫电化学的理解,并阻碍了现有催化剂的合理设计。在此,我们通过双原子模型系统地探索了多硫化物吸附转化的本质,以了解催化剂对加速SRR的作用。考虑到Fe/M (M: 3d嵌段过渡金属)原子系综的几何和电子口述,提出了一个包含电子结构指数(IES)和电子亲和指数(IEA)的描述符。在理论计算的帮助下,我们成功地确定了Fe/M部分的SRR热力学/动力学趋势。在这些发现的指导下,我们设计了一种Fe/V-NC双原子催化剂,该催化剂可以获得最小的IES和最大的IEA,从而增强了多硫化物的吸附-转化,提高了全电池性能。计算描述和实验证据之间的这种一致性突出了原子催化剂筛选和锂硫电池选择的重要性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Tailoring a Transition Metal Dual-Atom Catalyst via a Screening Descriptor in Li-S Batteries

Tailoring a Transition Metal Dual-Atom Catalyst via a Screening Descriptor in Li-S Batteries
The adsorption-conversion paradigm of polysulfides during the sulfur reduction reaction (SRR) is appealing to tackle the shuttle effect in Li-S batteries, especially based upon atomically dispersed electrocatalysts. However, mechanistic insights into such catalytic systems remain ambiguous, limiting the understanding of sulfur electrochemistry and retarding the rational design of available catalysts. Herein, we systematically explore the polysulfide adsorption-conversion essence via a geminal-atom model system to understand the catalyst roles toward an expedited SRR. A descriptor involving an electronic structure index (IES) and electron affinity index (IEA) is proposed, considering the geometric and electronic dictation within a Fe/M (M: 3d-block transition metal) atomic ensemble. With the aid of theoretical computation, we managed to identify the SRR thermodynamic/kinetic trends of Fe/M moieties. Guided by these findings, we in target design a Fe/V-NC dual-atom catalyst, which harvests a minimum IES and maximum IEA, accordingly demonstrating enhanced polysulfide adsorption-conversion and improved full-cell performances. Such a consistency between a computational descriptor and experimental evidence highlights the importance of an atomic catalyst screen and selection for Li-S batteries.
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来源期刊
ACS Nano
ACS Nano 工程技术-材料科学:综合
CiteScore
26.00
自引率
4.10%
发文量
1627
审稿时长
1.7 months
期刊介绍: ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.
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