Quantity effect of heteroatom incorporation on the oxygen evolution mechanism in ruthenium oxide

IF 19.1 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chem Pub Date : 2024-12-13 DOI:10.1016/j.chempr.2024.11.005

Hyunwoo Jun, Eunseo Kang, Jinuk Moon, Hoyoung Kim, Sunghoon Han, Seokhyun Choung, Seongbeen Kim, Seung Yeop Yi, Eunae Kang, Chang Hyuck Choi, Jeong Woo Han, Jinwoo Lee

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Abstract

Research on ruthenium oxide (RuO₂) catalysts as alternatives to Ir-based catalysts for the acidic oxygen evolution reaction (OER) has focused on enhancing activity and stability by incorporating heteroatoms. However, the relationship between the amount of incorporated heteroatom and the OER mechanism remains unclear. Herein, we synthesized rutile manganese-ruthenium solid-solution oxides (Mn_xRu_1-xO₂) with varying Mn/Ru ratios to identify factors affecting activity and stability with Mn content. Both experimental and computational results show that increasing Mn content raises the oxidation state of Ru and shifts the OER mechanism from the adsorbate evolution mechanism (AEM) to the lattice oxygen mechanism (LOM). Increased Mn concentration enhances Ru–O bond covalency, leading to lattice oxygen involvement in the OER. The Mn_0.2Ru_0.8O₂ catalyst, with an optimal Mn/Ru ratio, operated stably in a proton exchange membrane water electrolyzer (PEMWE) for 100 h and achieved 3.15 A cm⁻² at 1.8 V_cell, surpassing the 2026 Department of Energy activity goal.

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来源期刊

Chem Environmental Science-Environmental Chemistry

CiteScore

32.40

自引率

1.30%

发文量

281

期刊介绍： Chem, affiliated with Cell as its sister journal, serves as a platform for groundbreaking research and illustrates how fundamental inquiries in chemistry and its related fields can contribute to addressing future global challenges. It was established in 2016, and is currently edited by Robert Eagling.