Optimizing the Electronic Structure of Ruthenium Oxide by Neodymium Doping for Enhanced Acidic Oxygen Evolution Catalysis

IF 5.1 Q1 POLYMER SCIENCE ACS Macro Letters Pub Date : 2023-01-05 DOI:10.1002/adfm.202213304

Lu Li, Gengwei Zhang, Jingwen Xu, Huijie He, Bin Wang, Zhimao Yang, Shengchun Yang

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引用次数: 18

Abstract

It is a great challenge to design active and durable oxygen evolution reaction (OER) electrocatalysts for proton exchange membrane (PEM) electrolyzer due to the high dissolution of electrocatalysts in acidic solution. Herein, the Nd-doped RuO₂ (Nd_0.1RuO_x) is developed for enhanced oxygen evolution in 0.5 m H₂SO₄ solution with an overpotential of 211 mV to achieve 10 mA cm⁻². The theoretical calculation reveals that the improved activity of Nd_0.1RuO_x is due to the moderate decrease of d-band center energy, which balances the adsorption and desorption of oxygen intermediates. Moreover, the formation of more high valence state Ru⁴⁺ in Nd_0.1RuO_x is beneficial to the chemical stability of Ru species during the OER process, indicating that the introduction of Nd can effectively suppress the dissolution of Ru in acidic electrolytes. In addition, the PEM electrolyzer using Nd_0.1RuO_x/CC as the anode can be operated at 10 mA cm⁻² stably for 50 h. This study sheds new light on the design of the OER catalysts in acid by engineering the electronic structure of RuO₂.

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用钕掺杂优化氧化钌的电子结构以增强酸性析氧催化

摘要质子交换膜(PEM)电解槽的析氧反应(OER)电催化剂在酸性溶液中具有较高的溶解性，因此设计出高效耐用的析氧反应电催化剂是一个很大的挑战。本文研制了掺钕的RuO2 (Nd0.1RuOx)，用于在0.5 m H2SO4溶液中增强析氧，过电位为211 mV，达到10 mA cm−2。理论计算表明，Nd0.1RuOx活性的提高是由于d带中心能的适度降低，平衡了氧中间体的吸附和解吸。此外，在Nd0.1RuOx中形成更多的高价态Ru4+有利于OER过程中Ru物质的化学稳定性，说明Nd的引入可以有效抑制Ru在酸性电解质中的溶解。此外，以Nd0.1RuOx/CC为阳极的PEM电解槽可以在10 mA cm−2下稳定运行50 h。本研究通过对RuO2的电子结构进行工程设计，为酸性OER催化剂的设计提供了新的思路。

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来源期刊

ACS Macro Letters 化学-

CiteScore

10.40

自引率

3.40%

发文量

209

审稿时长

1 months

期刊介绍： ACS Macro Letters publishes research in all areas of contemporary soft matter science in which macromolecules play a key role, including nanotechnology, self-assembly, supramolecular chemistry, biomaterials, energy generation and storage, and renewable/sustainable materials. Submissions to ACS Macro Letters should justify clearly the rapid disclosure of the key elements of the study. The scope of the journal includes high-impact research of broad interest in all areas of polymer science and engineering, including cross-disciplinary research that interfaces with polymer science. With the launch of ACS Macro Letters, all Communications that were formerly published in Macromolecules and Biomacromolecules will be published as Letters in ACS Macro Letters.