Isopropanol Electro-Oxidation on PtCu Alloys for Aqueous Organic Redox Chemistry Toward Energy Storage.

IF 4.6 2区 化学 Q2 BIOCHEMISTRY & MOLECULAR BIOLOGY
Jinyao Tang, Xiaochen Shen, Laura Newsom, Rongxuan Xie, Parsa Pishva, Yanlin Zhu, Bin Liu, Zhenmeng Peng
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引用次数: 0

Abstract

Integration of renewable energy into modern power grids remains limited by intermittency and the need for reliable energy storage. Redox flow batteries (RFBs) are promising for large-scale energy storage, yet their widespread adoption is hindered by the high cost. In this study, we investigate isopropanol as a redox-active species with Pt-Cu alloy electrocatalysts for aqueous-organic RFBs. A series of PtxCu catalysts with varying Pt:Cu ratios were synthesized and studied for isopropanol electro-oxidation reaction (IPAOR) performance. Among them, PtCu demonstrated the best performance, achieving a low activation energy of 14.4 kJ/mol at 0.45 V vs. RHE and excellent stability at 1 M isopropanol (IPA) concentration. Kinetic analysis and in situ attenuated total reflectance-Fourier transform infrared (ATR-FTIR) spectroscopy revealed significantly reduced acetone accumulation on PtCu compared to pure Pt, indicating enhanced resistance to catalyst poisoning. Density functional theory (DFT) calculations further identified the first proton-coupled electron transfer (PCET) as the rate-determining step (RDS) with C-H bond scission as the preferred pathway on PtCu. A proof-of-concept PtCu-catalyzed H-cell demonstrated stable cycling over 200 cycles, validating the feasibility of IPA as a low-cost, regenerable redox couple. These findings highlight PtCu-catalyzed IPA/acetone(ACE) chemistry as a promising platform for next-generation aqueous-organic RFBs.

异丙醇电氧化PtCu合金在水相有机氧化还原化学中的应用。
可再生能源与现代电网的整合仍然受到间歇性和可靠储能需求的限制。氧化还原液流电池(rfb)有望用于大规模储能,但其广泛应用受到高成本的阻碍。在本研究中,我们用Pt-Cu合金电催化剂研究了异丙醇作为一种氧化还原活性物质在水性有机rbf中的作用。合成了一系列不同Pt:Cu比的PtxCu催化剂,研究了其异丙醇电氧化反应(IPAOR)性能。其中,PtCu表现出最好的性能,在0.45 V / RHE条件下具有14.4 kJ/mol的低活化能,在1 M异丙醇(IPA)浓度下具有优异的稳定性。动力学分析和原位衰减全反射-傅里叶变换红外(ATR-FTIR)光谱分析显示,与纯Pt相比,PtCu上的丙酮积累显著减少,表明对催化剂中毒的抵抗力增强。密度泛函理论(DFT)进一步确定了质子耦合电子转移(PCET)为速率决定步骤(RDS),而C-H键断裂是PtCu上的首选途径。ptcu催化的h电池在200次循环中稳定循环,验证了IPA作为低成本、可再生氧化还原对的可行性。这些发现强调了ptcu催化的IPA/丙酮(ACE)化学是下一代水性有机rfb的一个有前途的平台。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Molecules
Molecules 化学-有机化学
CiteScore
7.40
自引率
8.70%
发文量
7524
审稿时长
1.4 months
期刊介绍: Molecules (ISSN 1420-3049, CODEN: MOLEFW) is an open access journal of synthetic organic chemistry and natural product chemistry. All articles are peer-reviewed and published continously upon acceptance. Molecules is published by MDPI, Basel, Switzerland. Our aim is to encourage chemists to publish as much as possible their experimental detail, particularly synthetic procedures and characterization information. There is no restriction on the length of the experimental section. In addition, availability of compound samples is published and considered as important information. Authors are encouraged to register or deposit their chemical samples through the non-profit international organization Molecular Diversity Preservation International (MDPI). Molecules has been launched in 1996 to preserve and exploit molecular diversity of both, chemical information and chemical substances.
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