Synthesis, Molecular Structure, and Water Electrolysis Performance of TiO2-Supported Raney-IrOx Nanoparticles for the Acidic Oxygen Evolution Reaction

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-03-19 DOI:10.1021/acscatal.4c06385
Jiaqi Kang, Xingli Wang, Sebastian Möhle, Shima Farhoosh, Miklós Márton Kovács, Johannes Schmidt, Liang Liang, Matthias Kroschel, Sören Selve, Michael Haumann, Dominik Dworschak, Holger Dau, Peter Strasser
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Abstract

Developing low-cost, highly active, and stable catalysts for the acidic oxygen evolution reaction (OER) at the proton exchange membrane (PEM) water electrolyzer anodes remains a scientific priority. Reducing the iridium loading while increasing the intrinsic activity of the catalysts is essential for cost-effective hydrogen production. Here, we address a family of TiO2-supported Raney-IrOx catalysts with low iridium loading and high activity in single-cell PEM water electrolyzer anode environments. A controlled Raney-type Ni leaching process of pristine, supported IrNi alloy phases forms crystalline IrOx nanoparticles (NPs) featuring metallic Ir-rich cores surrounded by more amorphous IrOx surfaces. This structure is shown to be conducive to catalytic activity and the suppression of membrane poisoning due to Ni degradation. The trace amounts of Ni remaining after leaching in the IrOx NPs result in heterogeneous crystal structure and induce local lattice strain. Further, we synthetically strike a balance between conductivity and activity and succeed to narrow down the notorious large performance gap between liquid electrolyte rotating disk electrodes (RDEs) and single-cell membrane electrode assembly (MEA) electrolyzer measurements. OER stability numbers (S-numbers) of the identified Raney-IrOx anode catalysts surpass commercial IrO2 catalysts, confirming the stability of these catalysts. The PEM electrolyzer tests reveal that Raney-IrOx anodes achieve 3 A cm–2 at 1.8 V with a low geometric Ir loading of ca. 0.3 mgIr cm–2, meeting the technically important power specific Ir utilization target of 0.05 gIr/kW.

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用于酸性析氧反应的tio2负载Raney-IrOx纳米颗粒的合成、分子结构和水电解性能
开发低成本、高活性和稳定的催化剂用于质子交换膜(PEM)水电解槽阳极的酸性析氧反应(OER)仍然是科学研究的重点。在降低铱负载的同时提高催化剂的固有活性是经济高效制氢的必要条件。在这里,我们研究了一个家族的tio2负载的Raney-IrOx催化剂具有低铱负载和高活性的单电池PEM水电解阳极环境。原始的、负载的IrNi合金相的可控raney型Ni浸出过程形成结晶的IrOx纳米颗粒(NPs),其特征是金属富铁的核被更多的无定形IrOx表面包围。这种结构有利于催化活性和抑制镍降解引起的膜中毒。浸出后残留在IrOx NPs中的微量Ni导致了非均质晶体结构,并诱发了局部晶格应变。此外,我们在电导率和活性之间取得了综合平衡,并成功缩小了液体电解质旋转圆盘电极(RDEs)和单细胞膜电极组件(MEA)电解槽测量之间的巨大性能差距。所鉴定的Raney-IrOx阳极催化剂的OER稳定值(s -number)超过了商用IrO2催化剂,证实了这些催化剂的稳定性。PEM电解槽测试表明,Raney-IrOx阳极在1.8 V电压下达到3 A cm-2,几何Ir负载低至0.3 mgIr cm-2,达到了技术上重要的功率比Ir利用率目标0.05 gIr/kW。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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