Orbital Coupling of Dual-Atom Sites Boosts Electrocatalytic NO Oxidation and Dynamic Intracellular Response

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Ruijin Zeng, Yanli Li, Qing Wan, Zheng Lin, Qian Gao, Minghao Qiu, Zhaoqi Dong, Limei Xiao, Chenglong Sun, Mengyao Leng, Yu Gu, Mingchuan Luo, Shaojun Guo
{"title":"Orbital Coupling of Dual-Atom Sites Boosts Electrocatalytic NO Oxidation and Dynamic Intracellular Response","authors":"Ruijin Zeng,&nbsp;Yanli Li,&nbsp;Qing Wan,&nbsp;Zheng Lin,&nbsp;Qian Gao,&nbsp;Minghao Qiu,&nbsp;Zhaoqi Dong,&nbsp;Limei Xiao,&nbsp;Chenglong Sun,&nbsp;Mengyao Leng,&nbsp;Yu Gu,&nbsp;Mingchuan Luo,&nbsp;Shaojun Guo","doi":"10.1002/adma.202416371","DOIUrl":null,"url":null,"abstract":"<p>In situ measurement of nitric oxide (NO) in living tissue and single cells is highly important for achieving a profound comprehension of cellular functionalities and facilitating the precise diagnosis of critical diseases; however, the progress is greatly hindered by the weak affinity of ultratrace concentration NO in cellular environment toward electrocatalysts. Herein, a new strategy is reported for precisely constructing orbital coupled dual-atomic sites to enhance the affinity between the metal atomic sites and NO on a class of N-doped hollow carbon matrix dual-atomic sites Co─Ni (Co<sub>1</sub>Ni<sub>1</sub>-NC) for greatly boosting electrocatalytic NO performance. The as-synthesized Co<sub>1</sub>Ni<sub>1</sub>-NC demonstrates a substantially higher current density than Ni<sub>1</sub>-NC and Co<sub>1</sub>-NC, coupled with exceptional stability with a negligible degradation rate of 0.6 µA·cm<sup>−2</sup>·h<sup>−1</sup>, which is the best among the state-of-the-art electrocatalysts for NO oxidation. Experimental and theoretical investigations collectively reveal that the pivotal role of d-d orbit coupling between Co and Ni sites enables Ni to acquire additional electrons, leading to the occupation of Ni's 3d<sub>xy/yz</sub> within the 2π orbitals of NO, thus weakening the N≡O triple bond and concurrently accelerating NO adsorption kinetics. It is demonstrated that Co<sub>1</sub>Ni<sub>1</sub>-NC-coated nanoelectrode can achieve the in situ sensing of NO in living organs and single cells.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"37 6","pages":""},"PeriodicalIF":27.4000,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/adma.202416371","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

Abstract

In situ measurement of nitric oxide (NO) in living tissue and single cells is highly important for achieving a profound comprehension of cellular functionalities and facilitating the precise diagnosis of critical diseases; however, the progress is greatly hindered by the weak affinity of ultratrace concentration NO in cellular environment toward electrocatalysts. Herein, a new strategy is reported for precisely constructing orbital coupled dual-atomic sites to enhance the affinity between the metal atomic sites and NO on a class of N-doped hollow carbon matrix dual-atomic sites Co─Ni (Co1Ni1-NC) for greatly boosting electrocatalytic NO performance. The as-synthesized Co1Ni1-NC demonstrates a substantially higher current density than Ni1-NC and Co1-NC, coupled with exceptional stability with a negligible degradation rate of 0.6 µA·cm−2·h−1, which is the best among the state-of-the-art electrocatalysts for NO oxidation. Experimental and theoretical investigations collectively reveal that the pivotal role of d-d orbit coupling between Co and Ni sites enables Ni to acquire additional electrons, leading to the occupation of Ni's 3dxy/yz within the 2π orbitals of NO, thus weakening the N≡O triple bond and concurrently accelerating NO adsorption kinetics. It is demonstrated that Co1Ni1-NC-coated nanoelectrode can achieve the in situ sensing of NO in living organs and single cells.

Abstract Image

Abstract Image

双原子位轨道耦合促进电催化NO氧化和细胞内动态响应
原位测量活组织和单细胞中的一氧化氮(NO)对于实现对细胞功能的深刻理解和促进危重疾病的精确诊断非常重要;然而,细胞环境中超痕量NO对电催化剂的亲和力较弱,极大地阻碍了这一进展。本文报道了在一类n掺杂空心碳基Co─Ni (Co1Ni1-NC)双原子位上精确构建轨道耦合双原子位的新策略,以增强金属原子位与NO之间的亲和力,从而大大提高电催化NO的性能。合成的Co1Ni1-NC具有比Ni1-NC和Co1-NC高得多的电流密度,并且具有优异的稳定性,降解率为0.6µa·cm−2·h−1,是目前最先进的NO氧化电催化剂。实验和理论研究共同表明,Co和Ni位点之间的d-d轨道耦合的关键作用使Ni获得额外的电子,导致Ni在NO的2π轨道内的3dxy/yz占据,从而削弱N≡O三键,同时加速NO的吸附动力学。结果表明,co1ni1 - nc包覆纳米电极可以实现活体器官和单细胞中NO的原位传感。
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
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信