Homonuclear/Heteronuclear Bimetallic Conjugated Coordination Polymers with Customized Oxygen Evolution Pathway

IF 14.4 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Journal of the American Chemical Society Pub Date : 2025-04-11 DOI:10.1021/jacs.5c02700

Yuhao Weng, Lizhi Sun, Hao Jia, Wenjuan Shang, Jie-Jie Chen, Barun Dhara, Yong Chen, Fei Huang, Shu Han, Hangjuan He, Baipeng Yin, Chuang Zhang, Ben Liu, Zhongxin Chen, Jingsong You, Daigo Miyajima, Cheng Zhang

{"title":"Homonuclear/Heteronuclear Bimetallic Conjugated Coordination Polymers with Customized Oxygen Evolution Pathway","authors":"Yuhao Weng, Lizhi Sun, Hao Jia, Wenjuan Shang, Jie-Jie Chen, Barun Dhara, Yong Chen, Fei Huang, Shu Han, Hangjuan He, Baipeng Yin, Chuang Zhang, Ben Liu, Zhongxin Chen, Jingsong You, Daigo Miyajima, Cheng Zhang","doi":"10.1021/jacs.5c02700","DOIUrl":null,"url":null,"abstract":"The reasons for the generally superior performance of synergistic effects in bimetallic catalysts in the oxygen evolution reaction (OER) are not fully understood, largely due to the complexity of catalyst structures and the challenges associated with synthesizing long-range atomic ordering catalysts. In this study, we present a series of two-dimensional (2D) conjugated bimetallic coordination polymers (c-CPs) involving Co or Ni with unambiguous and nearly identical geometry structures for the electrocatalysis of OER, which are highly suitable for discussions on structure–property correlations. The heteronuclear CoNi-PI unexpectedly alters the OER catalytic mechanisms from adsorbate evolution mechanism those observed in homonuclear CoCo-PI and NiNi-PI to the kinetically faster oxide path mechanism, exhibiting high stability and an ultralow overpotential of 282 mV even at 100 mA cm–2 with a Tafel slope of approximately 42 mV dec–1. This study presents an extremely rare crystalline heteronuclear bimetallic catalyst with excellent catalytic properties, promising significant influences in catalyst development research.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"108 1","pages":""},"PeriodicalIF":14.4000,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/jacs.5c02700","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

The reasons for the generally superior performance of synergistic effects in bimetallic catalysts in the oxygen evolution reaction (OER) are not fully understood, largely due to the complexity of catalyst structures and the challenges associated with synthesizing long-range atomic ordering catalysts. In this study, we present a series of two-dimensional (2D) conjugated bimetallic coordination polymers (c-CPs) involving Co or Ni with unambiguous and nearly identical geometry structures for the electrocatalysis of OER, which are highly suitable for discussions on structure–property correlations. The heteronuclear CoNi-PI unexpectedly alters the OER catalytic mechanisms from adsorbate evolution mechanism those observed in homonuclear CoCo-PI and NiNi-PI to the kinetically faster oxide path mechanism, exhibiting high stability and an ultralow overpotential of 282 mV even at 100 mA cm^–2 with a Tafel slope of approximately 42 mV dec^–1. This study presents an extremely rare crystalline heteronuclear bimetallic catalyst with excellent catalytic properties, promising significant influences in catalyst development research.

Abstract Image

查看原文本刊更多论文

自定义析氧途径的同核/异核双金属共轭配位聚合物

在析氧反应（OER）中，双金属催化剂的协同效应普遍表现优异，其原因尚不完全清楚，很大程度上是由于催化剂结构的复杂性以及与合成远程原子有序催化剂相关的挑战。在这项研究中，我们提出了一系列二维（2D）共轭双金属配位聚合物（c-CPs），涉及Co或Ni，具有明确的和几乎相同的几何结构，用于OER的电催化，非常适合讨论结构-性能相关性。异核co - pi出人意料地改变了OER催化机制，从同核co - pi和ni - pi中观察到的吸附物演化机制转变为动力学上更快的氧化路径机制，表现出高稳定性和超低过电位，即使在100 mA cm-2下也能达到282 mV， Tafel斜率约为42 mV / dec1。本研究提出了一种极为罕见的晶体异核双金属催化剂，具有优异的催化性能，在催化剂开发研究中具有重要意义。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Journal of the American Chemical Society 化学-化学综合

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.