利用极性 MnNiO 和铠装碳对 RuOx 纳米粒子进行双重限制,以促进水的电解

Ning Wen, Xiaoxiao Duan, Ruiying Chai, Xiuling Jiao, Yuguo Xia, Dairong Chen
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引用次数: 0

摘要

具有催化活性的纳米粒子催化剂稳定性差,是其工业应用的一大障碍。建立合理的纳米粒子结构,阐明催化剂结构与其催化活性和稳定性之间的关系,对于构建高活性和高稳定性的纳米粒子催化剂至关重要。我们提出了一种构建纳米粒子双重约束效应的策略,特别是通过调节 MnNiO 支承的极化来增强强氧化物-支承相互作用(SOSI),并用碳壳包裹纳米粒子外层,这已被证明能有效提高基于纳米粒子的氧进化反应(OER)电催化剂的活性和稳定性。在 100 mA cm 的电流密度下,铠装 C@RuO@MnNiO 催化剂的 OER 过电位为 260 mV。经过 100 h 的 OER 测试后,C@RuO@MnNiO 的电流密度没有明显衰减,而 RuO@MnNiO 和 RuO@MnO 的电流密度则迅速下降,这表明催化剂具有显著的催化活性和稳定性。组装好的 C@RuO@MnNiO||Pt/C 电极在 MEA 电解槽中表现出优异的碱性水电解性能,只需要 1.76 V 的低电池电压就能达到 1 A cm 的安培级电流密度。原位电化学拉曼光谱揭示了纳米颗粒与极性支持物之间的显著相互作用。密度泛函理论计算表明,吉布斯自由能的降低是由 RuO@MnNiO 中极性锰掺杂引起的电荷再分布和配位结构的改变造成的,而吉布斯自由能的降低确立了 OER 的速率决定步骤 (RDS)。这项工作为通过 SOSI 诱导的强相互作用和铠装碳层的双重约束效应设计高效稳定的纳米粒子电催化剂提供了一种方法。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Dual confinement of RuOx nanoparticle using polar MnNiO and armored carbon for boosting water electrolysis
The poor stability of nanoparticle catalysts with catalytic activity is a significant obstacle to their industrial application. The establishment of rational nanoparticle structures to elucidate the relationship between catalyst structure and its catalytic activity and stability is crucial for constructing nanoparticle catalysts that are both highly active and stable. We propose a strategy to construct a dual-confinement effect of the nanoparticle, specifically by regulating the polarization of the MnNiO support to enhance strong oxide-support interactions (SOSI) and encapsulating the outer layer of nanoparticles with a carbon shell, which has been proven effective in improving the activity and stability of nanoparticle-based oxygen evolution reaction (OER) electrocatalysts. At a current density of 100 mA cm, the armor C@RuO@MnNiO catalyst displays an overpotential of 260 mV for the OER. After the OER test for 100 h, the current density of C@RuO@MnNiO shows no significant decay, whereas that of RuO@MnNiO and RuO@MnO rapidly decreases, indicating significant catalytic activity and stability of the catalyst. The assembled C@RuO@MnNiO||Pt/C electrode demonstrates excellent alkaline water electrolysis performance in an MEA electrolyzer, requiring only a low cell voltage of 1.76 V to achieve an ampere-level current density of 1 A cm. In-situ electrochemical Raman spectroscopy reveals the significant interaction between nanoparticles and the polar support. The reduction in Gibbs free energy, which establishes the rate-determining step (RDS) of OER, is caused by the charge redistribution caused by polar Mn doping in RuO@MnNiO and the coordination structure modifications, as shown by density functional theory calculations. This work provides an approach to designing efficient and stable nanoparticle electrocatalysts through the dual-confinement effect of SOSI-induced strong interactions and armor carbon layers.
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