克服结垢关系限制的动态镓单原子催化剂:二氧化碳还原和析氢反应的AIMD筛选。

IF 8.7 Q1 CHEMISTRY, MULTIDISCIPLINARY
JACS Au Pub Date : 2025-08-20 eCollection Date: 2025-09-22 DOI:10.1021/jacsau.5c00823
Mohsen Tamtaji, William A Goddard, Ziyang Hu, Shuguang Chen, GuanHua Chen
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引用次数: 0

摘要

单原子催化剂(SACs)在一系列电化学反应中的应用已经得到了广泛的研究。然而,静态sac受到扩展关系的限制,这阻碍了它们的进一步发展。在这项工作中,我们介绍了镓支持的动态sac用于析氢反应(HER)和二氧化碳还原反应(CO2RR)的思想。我们利用AIMD和DFT计算系统地对镓支持的s-, p-, d-和f-块元素进行高通量筛选,表示为M-SAC@Ga。我们发现,在所有的催化剂中,Re-、Pt-、Pd-、Rh-、Ir-、Au-、Ag-、Ru-、Tc-、Ni-、Cu-、Os-、Hg-和Ge-SAC@Ga都具有热力学和电化学稳定性。此外:Ni-SAC@Ga导致CO2RR过电位分别为0.28、0.28、0.69和0.92 V,有利于choh、CO、CH3OH和CH4的形成。通过DFT和AIMD计算,可以看到sac的原子智能(引导反应的能力)和动态配位变化,从而降低过电位和降低标度关系限制。分析声子诱导的总能量波动表明,计算出的过电位的标准偏差高达0.26 V。此外,这些动态体系的脱相时间小于5fs,这是影响催化行为建模的关键因素。特征重要性分析表明,d电子数可以作为这些催化剂的通用描述符。这项研究提供了一个全面的洞察前沿电催化剂的发现和超越应用动态sac的概念。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Dynamic Single-Atom Catalysts on Gallium To Overcome the Scaling Relationship Limit: AIMD Screening for CO2 Reduction and Hydrogen Evolution Reactions.

Extensive research has been conducted on single-atom catalysts (SACs) for a range of electrochemical reactions. However, static SACs suffer from scaling relationship limits, which hinder their further development. In this work, we introduce the idea of dynamic SACs supported on Gallium for the hydrogen evolution reaction (HER) and the CO2 reduction reaction (CO2RR). We utilized AIMD and DFT calculations to systematically conduct high-throughput screening on s-, p-, d-, and f-block elements supported by Gallium denoted as M-SAC@Ga. We found that among all the understudied catalysts, Re-, Pt-, Pd-, Rh-, Ir-, Au-, Ag-, Ru-, Tc-, Ni-, Cu-, Os-, Hg-, and Ge-SAC@Ga possess thermodynamic and electrochemical stabilities. In addition: Ni-SAC@Ga leads to CO2RR overpotentials of 0.28, 0.28, 0.69, and 0.92 V, respectively, toward CHOOH, CO, CH3OH, and CH4 formation. Low overpotentials and mitigation of scaling relationship limits are primarily due to the atomic intelligence (the ability to guide reactions) and dynamic coordination changes of SACs, seen through DFT and AIMD calculations. Analyzing the phonon-induced fluctuations in total energies suggests a standard deviation of up to 0.26 V in the calculated overpotentials. Additionally, the dephasing time for these dynamic systems is below 5 fs, a crucial factor affecting the modeling of catalytic behavior. Feature importance analysis suggests that the d-electron numbers serve as the universal descriptors for these catalysts. This study offers a comprehensive insight into the discovery of cutting-edge electrocatalysts and beyond by applying the concept of dynamic SACs.

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CiteScore
9.10
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