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晶格掺杂的铱与表面锚定的氧化铱协同作用用于超低铱负载的酸性析氧反应

Lattice-Doped Ir Cooperating with Surface-Anchored IrO for Acidic Oxygen Evolution Reaction with Ultralow Ir Loading.

作者信息

Wang Qi, Zhang Kaini, Zhang Zhengqi, Chen Xin, Deng Hao, Hua Weibo, Wei Jinjia, Shen Shaohua, Chen Jie

机构信息

School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China.

International Research Center for Renewable Energy, State Key Laboratory of Multiphase Flow in Power Engineering, Xi'an Jiaotong University, Xi'an, Shaanxi 710049, China.

出版信息

ACS Appl Mater Interfaces. 2025 Feb 5;17(5):7929-7937. doi: 10.1021/acsami.4c21373. Epub 2025 Jan 26.

Abstract

Reducing iridium (Ir) loading while maintaining efficiency and stability is crucial for the acidic oxygen evolution reaction (OER). In this study, we develop a synthetic method of sequential electrochemical deposition and high-temperature thermal shock to produce an IrO/Ir-WO electrocatalyst with ∼1.75 nm IrO nanoparticles anchoring on Ir-doped WO nanosheets. The IrO/Ir-WO electrocatalyst with a low Ir loading of 0.035 mg cm demonstrates a low overpotential of 239 mV to achieve a current density of 10 mA cm and a mass activity of 6.6 × 10 A g @1.75 V vs RHE in 0.5 M HSO. IrO/Ir-WO on carbon paper as the anode and Pt/C as the cathode work stably for 40 h at 30 mA cm in a proton exchange membrane water electrolyzer. It is found that the cooperation of lattice-doped Ir and surface-anchored IrO enhances the activity and stability of IrO/Ir-WO for acidic OER. Specifically, the doped Ir reduces the electron density of the anchored IrO, thus optimizing the adsorption energy of oxygen-containing intermediates and the kinetic barrier of HO dissociation, leading to an enhanced activity of IrO/Ir-WO. Also, the Ir-WO support provides electrons to retard the overoxidation and dissolution of Ir atoms from the anchored IrO during acidic OER.

摘要

在保持效率和稳定性的同时降低铱(Ir)负载量对于酸性析氧反应(OER)至关重要。在本研究中,我们开发了一种顺序电化学沉积和高温热冲击的合成方法,以制备一种IrO/Ir-WO电催化剂,其中约1.75 nm的IrO纳米颗粒锚定在Ir掺杂的WO纳米片上。Ir负载量低至0.035 mg cm的IrO/Ir-WO电催化剂在0.5 M HSO中相对于可逆氢电极(RHE)在1.75 V时实现10 mA cm的电流密度具有239 mV的低过电位和6.6×10 A g的质量活性。在质子交换膜水电解槽中,以碳纸上的IrO/Ir-WO作为阳极,Pt/C作为阴极,在30 mA cm下稳定工作40 h。研究发现,晶格掺杂的Ir和表面锚定的IrO的协同作用增强了IrO/Ir-WO对酸性OER的活性和稳定性。具体而言,掺杂的Ir降低了锚定的IrO的电子密度,从而优化了含氧中间体的吸附能和HO解离的动力学势垒,导致IrO/Ir-WO的活性增强。此外,Ir-WO载体提供电子以抑制酸性OER过程中Ir原子从锚定的IrO上的过度氧化和溶解。

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