Modulating Built-In Electric Field Strength in Ru/RuO2 Interfaces through Ni Doping to Enhance Hydrogen Conversion at Ampere-level Current

IF 16.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Angewandte Chemie International Edition Pub Date : 2025-01-15 DOI:10.1002/anie.202421869

Tao Liu, Lianqin Wang, Bin Chen, Haotian Liu, Sipu Wang, Yingjie Feng, Junfeng Zhang, Yan Yin, Guiver Michael

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引用次数: 0

Abstract

Improving the alkaline hydrogen evolution reaction (HER) efficiency is essential for developing advanced anion exchange membrane water electrolyzers (AEMWEs) that operate at industrial ampere-level currents. Herein, we employ density functional theory (DFT) calculations to identify Ni-RuO2 as the leading candidate among various 3d transition metal-doped M-RuO2 (where metal M includes Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, and Zn). The incorporation of Ni atoms facilitates the partial reduction of RuO2, resulting in the formation of a Ni-Ru/RuO2 interface having a significant built-in electric field (BIEF) during electrochemical reactions. The resulted BIEF enhances electron transfer across the interface, which is critical in lowering energy barriers and accelerating the hydrogen evolution reaction (HER) kinetics. As a result, the Ni-RuO2 catalyst exhibits an overpotential of 134 mV at 1 A cm-2 and a low Tafel slope of 20.85 mV dec-1, with just 0.03 mg cm-2 of Ru loading. The highly effective BIEF, therefore, plays a pivotal role in the catalyst's remarkable performance, allowing the Ni-RuO2-based AEMWE to require only 1.71V to maintain stable operation at 1 A cm-2 over a 1000-hour period.

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提高碱性氢进化反应（HER）的效率对于开发可在工业安培级电流下运行的先进阴离子交换膜水电解槽（AEMWEs）至关重要。在此，我们利用密度泛函理论（DFT）计算，确定 Ni-RuO2 是各种掺杂 3d 过渡金属的 M-RuO2（其中金属 M 包括 Sc、Ti、V、Cr、Mn、Fe、Co、Ni、Cu 和 Zn）中的主要候选物质。镍原子的加入促进了 RuO2 的部分还原，从而在电化学反应过程中形成了具有显著内置电场（BIEF）的 Ni-Ru/RuO2 界面。由此产生的内置电场增强了跨界面的电子转移，这对于降低能量障碍和加速氢进化反应（HER）动力学至关重要。因此，Ni-RuO2 催化剂在 1 A cm-2 时的过电位为 134 mV，Tafel 斜坡低至 20.85 mV dec-1，而 Ru 的负载量仅为 0.03 mg cm-2。因此，高效的 BIEF 在催化剂的卓越性能中发挥了关键作用，使基于 Ni-RuO2 的 AEMWE 在 1 A cm-2 的条件下只需要 1.71V 的电压就能稳定运行 1000 小时。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Angewandte Chemie International Edition 化学-化学综合

CiteScore

26.60

自引率

6.60%

发文量

3549

审稿时长

1.5 months

期刊介绍： Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.