High-Density Iridium Single Atoms on Vanadium-Doped TiO2 for Electrochemical Water Oxidation Catalysis

IF 13.6 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2026-10-16 DOI:10.1021/acscatal.6c04537

Chang Hyun Lee,Nodo Lee,Seungwoo Choi,Jun Ho Jang,Kyung Tae Kim,Ji Hoon Chung,Donghyeon Oh,Jung Sug Hong,Byung Soo Oh,Choul Kim,Young Hwan Min,Hui-Youn Shin,Myeong-Soo Chang,Zhipeng Wang,Sang Ho Oh,Hyacinthe Randriamahazaka,Ki Tae Nam

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引用次数: 0

Abstract

Abstract Water oxidation in proton exchange membrane water electrolysis (PEMWE) uses IrO2 nanoparticles supported on corrosion-resistant TiO2. However, the low conductivity of TiO2 imposes electronic transport limitations that necessitate high Ir loadings for effective catalysis. Here, we present a catalyst design strategy that couples a heavily V-doped TiO2 support with high-density Ir single atoms, enabling water oxidation at minimal Ir loading. In this design, Ti-site-substituted V provides n-type doping, and selective V leaching creates cation vacancies that anchor Ir as isolated atoms. TEM with convolutional neural network (CNN)-based analysis shows Ir single-atom density increases with V content, accompanied by lower charge-transfer resistance and higher Ir-specific activity. The density functional theory indicates that cation-site Ir introduces a midgap state below V 3d levels and shifts neighboring V 3d orbitals toward the Fermi level. Ir1/V-TiO2 achieves 1480 A gIr–1 at 1.55 V vs RHE (1.3 wt % Ir) and demonstrates device-level PEMWE operation at an Ir loading as low as 0.027 mgIr cm–2.

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钒掺杂TiO2上高密度铱单原子的电化学水氧化催化

摘要质子交换膜水电解（PEMWE）中的水氧化使用耐腐蚀TiO2负载的IrO2纳米颗粒。然而，TiO2的低导电性施加了电子传输限制，需要高Ir负载才能有效催化。在这里，我们提出了一种催化剂设计策略，将重v掺杂的TiO2载体与高密度Ir单原子偶联，使水在最小的Ir负载下氧化。在该设计中，钛位取代的V提供n型掺杂，选择性V浸出产生阳离子空位，将Ir固定为孤立原子。基于卷积神经网络（CNN）的TEM分析表明，随着V含量的增加，Ir单原子密度增加，伴随着更低的电荷转移电阻和更高的Ir特异性活性。密度泛函理论表明，阳离子位Ir引入了一个低于v3d能级的中隙态，并使邻近的v3d轨道向费米能级移动。Ir1/V- tio2在1.55 V vs RHE （1.3 wt % Ir）下达到1480 A gIr-1，并在低至0.027 mgIr cm-2的Ir负载下演示器件级PEMWE操作。

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来源期刊

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.