构建掺钯 RuO2 纳米片,实现高效稳定的酸性水氧化

IF 10.7 1区 工程技术 Q1 CHEMISTRY, PHYSICAL Green Energy & Environment Pub Date : 2023-12-13 DOI:10.1016/j.gee.2023.12.003
Yibo Liu, Xing Hu, Chenxi Liu, Shan Zhu, Kezhu Jiang, Feng Liu, Shijian Zheng
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摘要

在氧进化反应(OER)中,RuO2 因其卓越的内在活性而被认为是商用 IrO2 的潜在替代品。然而,其固有结构在酸性环境中的溶解限制了其商业应用。在本研究中,我们报告了一种新型 Pd 掺杂氧化钌(Pd-RuO2)纳米片催化剂,该催化剂通过 Pd 对 Ru 电子结构和二维结构调制的协同效应提高了活性和稳定性。该催化剂性能卓越,在电流密度为 10 mA cm-2 时,过电位仅为 204 mV。令人印象深刻的是,经过 8000 次循环伏安测试后,过电位仅下降了 5 mV。使用 Pd0.08Ru0.92O2 作为阳极催化剂的 PEM 电解槽在 200 mA cm-2 的电流密度下工作了近 130 小时。为了阐明催化剂稳定性增强的内在机理,我们进行了 X 射线光电子能谱(XPS)分析,结果表明从 Pd 到 Ru 的电子转移有效地规避了 Ru 的过氧化反应,从而在增强催化剂稳定性方面发挥了关键作用。此外,密度泛函理论(DFT)计算提供了令人信服的证据,证明在 RuO2 中引入 Pd 能有效调节电子相关性,促进电子从 Pd 转移到 Ru,从而防止 Ru 过度氧化。此外,二维结构的应用还有效抑制了纳米颗粒的聚集和生长,进一步增强了催化剂的结构完整性。
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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Construction of Pd-doped RuO2 nanosheets for efficient and stable acidic water oxidation

RuO2 has been considered a potential alternative to commercial IrO2 for the oxygen evolution reaction (OER) due to its superior intrinsic activity. However, its inherent structure dissolution in acidic environments restricts its commercial applications. In this study, we report a novel Pd-doped ruthenium oxide (Pd-RuO2) nanosheet catalyst that exhibits improved activity and stability through a synergistic effect of Pd modulation of Ru electronic structure and the two-dimensional structure. The catalyst exhibits excellent performance, achieving an overpotential of only 204 mV at a current density of 10 mA cm-2. Impressively, after undergoing 8000 cycles of cyclic voltammetry testing, the overpotential merely decreased by 5 mV. The PEM electrolyzer with Pd0.08Ru0.92O2 as an anode catalyst survived an almost 130 h operation at 200 mA cm-2. To elucidate the underlying mechanisms responsible for the enhanced stability, we conducted an X-ray photoelectron spectroscopy (XPS) analysis, which reveals that the electron transfer from Pd to Ru effectively circumvents the over-oxidation of Ru, thus playing a crucial role in enhancing the catalyst's stability. Furthermore, density functional theory (DFT) calculations provide compelling evidence that the introduction of Pd into RuO2 effectively modulates electron correlations and facilitates the electron transfer from Pd to Ru, thereby preventing the over-oxidation of Ru. Additionally, the application of the two-dimensional structure effectively inhibited the aggregation and growth of nanoparticles, further bolstering the structural integrity of the catalyst.

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来源期刊
Green Energy & Environment
Green Energy & Environment Energy-Renewable Energy, Sustainability and the Environment
CiteScore
16.80
自引率
3.80%
发文量
332
审稿时长
12 days
期刊介绍: Green Energy & Environment (GEE) is an internationally recognized journal that undergoes a rigorous peer-review process. It focuses on interdisciplinary research related to green energy and the environment, covering a wide range of topics including biofuel and bioenergy, energy storage and networks, catalysis for sustainable processes, and materials for energy and the environment. GEE has a broad scope and encourages the submission of original and innovative research in both fundamental and engineering fields. Additionally, GEE serves as a platform for discussions, summaries, reviews, and previews of the impact of green energy on the eco-environment.
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