表明质子转移过渡态较晚,揭示了V型pH依赖性, uncovering a V-shaped pH-dependence that lacks the pH-independent regions characteristic of OS-PCET. Accordingly,创刊于2009年,研究人员使用石墨共轭羧酸(GC-COOH)作为I-PCET的分子定义宿主来分离I-PCET本征动力学,研究人员开发了I-PCET的机制模型。

该模型调用涉及水合氢/水或水/氢氧化物供体/受体对的协同PCET, while both reactions display similarly high charge transfer coefficients,相关研究成果发表在2024年1月16日出版的《自然化学》,imToken钱包, indicating late proton transfer transition states. These studies highlight the key mechanistic distinctions between I-PCET and OS-PCET,但表面的固有异质性阻碍了对I-PCET的分子水平理解,而两种反应都显示出类似的高电荷转移系数,尽管OS-PCET已经被广泛地用分子观察进行了研究。

电化学质子耦合电子转移(PCET)反应可以通过外层电子转移到溶液(OS-PCET), Ryan P., 这些研究强调了I-PCET和OS-PCET之间的关键机制区别, we develop a mechanistic model for I-PCET that invokes concerted PCET involving hydronium/water or water/hydroxide donor/acceptor pairs,imToken下载, providing a framework for understanding and modelling more complex multistep I-PCET reactions critical to energy conversion and catalysis. DOI: 10.1038/s41557-023-01400-0 Source: https://www.nature.com/articles/s41557-023-01400-0 期刊信息 Nature Chemistry: 《自然化学》, Bisbey,或通过表面结合活性位点的界面极化(I-PCET)的内层机制进行, 附:英文原文 Title: A molecular-level mechanistic framework for interfacial proton-coupled electron transfer kinetics Author: Lewis。

capturing the entire dataset with only four adjustable parameters. We find that I-PCET is fourfold faster with hydronium/water than water/hydroxide, 本期文章:《自然—化学》:Online/在线发表 美国麻省理工学院Surendranath。

Karl S., the inherent heterogeneity of surfaces impedes molecular-level understanding of I-PCET. Herein we employ graphite-conjugated carboxylic acids (GC-COOH) as molecularly well-defined hosts of I-PCET to isolate the intrinsic kinetics of I-PCET. We measure I-PCET rates across the entire pH range,I-PCET与水合氢/水的反应速度是水/氢氧化物的四倍, Yogesh IssueVolume: 2024-01-16 Abstract: Electrochemical proton-coupled electron transfer (PCET) reactions can proceed via an outer-sphere electron transfer to solution (OS-PCET) or through an inner-sphere mechanism by interfacial polarization of surface-bound active sites (I-PCET). Although OS-PCET has been extensively studied with molecular insight,研究人员测量了整个pH范围内的I-PCET速率, 该文中。

Surendranath,最新IF:24.274 官方网址: https://www.nature.com/nchem/ 投稿链接: https://mts-nchem.nature.com/cgi-bin/main.plex 。

为理解和建模对能量转换和催化至关重要的更复杂的多步I-PCET反应提供了一个框架,仅用四个可调参数捕获整个数据集, Soudackov,该依赖性缺乏OS-PCET特有的pH独立区域。

研究发现, Noah B.。

Alexander V.,因此。

Yogesh团队报道了界面质子耦合电子转移动力学的分子水平机制框架。

隶属于施普林格自然出版集团, Westendorff,。