电化学发光法测定析氧反应中电催化剂的局部pH梯度

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yu Wang, Sijia Zhou, Yongjun Zheng, Yongji Wang, Yuhua Hou, Kaiqing Wu, Chaofeng Huang, Songqin Liu, Yanfei Shen, Ran Chen* and Yuanjian Zhang*, 
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引用次数: 0

摘要

准确理解析氧反应的机理对氢能工业中催化剂的设计至关重要。尽管在微观pH检测方面取得了重大进展,但在OER过程中选择性、敏感、快速和可靠地检测催化剂附近的局部pH梯度仍然是难以捉摸的。在这里,我们开创了一种电化学发光(ECL)方法,用于OER期间的局部pH检测。为此,从理论上预测了一类基于ECL共振能量转移的新型ECL发射体,并通过在高贵的二维氮化碳上接枝功能荧光染料,方便地合成了一类新的ECL发射体。通过在OER催化剂附近放置一个具有pH责任的ECL发射器,可以以亚秒级的分辨率实时定量测量催化剂附近的局部pH梯度产生。详细介绍了OER的反应机理,揭示了质子积累引起的催化剂降解途径。此外,还可以从局部pH测量中提取催化剂上的平均质子生成速率,作为OER反应速率的定量描述符。由于该接枝方法具有较高的可设计性,为研究反应机理和检测中间体开辟了新的策略。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Measurements of Local pH Gradients for Electrocatalysts in the Oxygen Evolution Reaction by Electrochemiluminescence

Measurements of Local pH Gradients for Electrocatalysts in the Oxygen Evolution Reaction by Electrochemiluminescence

An accurate understanding of the mechanism of the oxygen evolution reaction (OER) is crucial for catalyst design in the hydrogen energy industry. Despite significant advancements in microscopic pH detection, selective, sensitive, speedy, and reliable detection of local pH gradients near the catalysts during the OER remains elusive. Here, we pioneer an electrochemiluminescence (ECL) method for local pH detection during the OER. For this purpose, a new class of ECL emitters based on ECL resonance energy transfer was theoretically predicted and facilely synthesized by grafting functional fluorescent dyes onto noble 2D carbon nitride. By positioning one of the as-prepared ECL emitters with pH-responsibility neighboring the OER catalysts, local pH gradient generation near the catalysts could be qualitatively measured in real-time with a subsecond resolution. It provided details of the reaction mechanism of the OER and unveiled the catalyst degrading pathway caused by proton accumulation. Besides, the average proton generation rate on the catalyst was also extractable from the local pH measurement as a quantitative descriptor of the OER reaction rate. Owing to the high designability of the grafting method, this study opens up new strategies for studying reaction mechanisms and detecting intermediates.

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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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