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通过筛选效应实现电子/质子双导电磺化聚苯胺微孔包裹氧化铱电催化剂对海水电解析氧的高催化选择性

High Catalytic Selectivity of Electron/Proton Dual-Conductive Sulfonated Polyaniline Micropore Encased IrO Electrocatalyst by Screening Effect for Oxygen Evolution of Seawater Electrolysis.

作者信息

Shen Yuhan, Zhao Shengqiu, Wu Fanglin, Zhang Hao, Zhu Liyan, Wu Mingjuan, Tian Tian, Tang Haolin

机构信息

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, P. R. China.

National Energy Key Laboratory for New Hydrogen-Ammonia Energy Technologies, Foshan Xianhu Laboratory, Foshan, 528200, P. R. China.

出版信息

Adv Sci (Weinh). 2025 Jan;12(4):e2412862. doi: 10.1002/advs.202412862. Epub 2024 Dec 4.

Abstract

Acidic seawater electrolysis offers significant advantages in high efficiency and sustainable hydrogen production. However, in situ electrolysis of acidic seawater remains a challenge. Herein, a stable and efficient catalyst (SPTTPAB/IrO) is developed by coating iridium oxide (IrO) with a microporous conjugated organic framework functionalized with sulfonate groups (-SOH) to tackle these challenges. The SPTTPAB/IrO presents a -SOH concentration of 5.62 × 10 mol g and micropore below 2 nm numbering 1.026 × 10 g. Molecular dynamics simulations demonstrate that the conjugated organic framework blocked 98.62% of Cl in seawater from reaching the catalyst. This structure combines electron conductivity from the organic framework and proton conductivity from -SOH, weakens the Cl adsorption, and suppresses metal-chlorine coupling, thus enhancing the catalytic activity and selectivity. As a result, the overpotential for the oxygen evolution reaction (OER) is only 283 mV@10 mA cm, with a Tafel slope of 16.33 mV dec, which reduces 13.8% and 37.8% compared to commercial IrO, respectively. Impressively, SPTTPAB/IrO exhibits outstanding seawater electrolysis performance, with a 35.3% improvement over IrO to 69 mA cm@1.9 V, while the degradation rate (0.018 mA h) is only 24.6% of IrO. This study offers an innovative solution for designing high-performance seawater electrolysis electrocatalysts.

摘要

酸性海水电解在高效和可持续制氢方面具有显著优势。然而,酸性海水的原位电解仍然是一个挑战。在此,通过用磺酸基团(-SOH)功能化的微孔共轭有机框架包覆氧化铱(IrO)来开发一种稳定且高效的催化剂(SPTTPAB/IrO),以应对这些挑战。SPTTPAB/IrO的-SOH浓度为5.62×10⁻³mol g⁻¹,微孔尺寸低于2nm,数量为1.026×10¹⁷g⁻¹。分子动力学模拟表明,共轭有机框架阻止了海水中98.62%的Cl⁻到达催化剂。这种结构结合了有机框架的电子传导性和-SOH的质子传导性,减弱了Cl⁻的吸附,并抑制了金属-氯耦合,从而提高了催化活性和选择性。结果,析氧反应(OER)的过电位在10mA cm⁻²时仅为283mV,塔菲尔斜率为16.33mV dec⁻¹,与商业IrO相比分别降低了13.8%和37.8%。令人印象深刻的是,SPTTPAB/IrO表现出出色的海水电解性能,在1.9V时比IrO提高了35.3%,达到69mA cm⁻²,而降解速率(0.018mA h⁻¹)仅为IrO的24.6%。这项研究为设计高性能海水电解电催化剂提供了一种创新解决方案。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/58b3/11775546/b2a137c3d26a/ADVS-12-2412862-g002.jpg

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