文献类型：期刊文献

英文题名：Unveiling the Role of Interfacial Interactions in Governing Electrocatalytic Activity at the Single Nanoparticle Level

作者：Liu, Zhenhua[1,2];Sun, Zehui[1,2];Su, Lei[1,2];Ma, Wei[1,2]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Frontiers Sci Ctr Materiobiol & Dynam Chem, Joint Int Res Lab Precis Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2026

卷号：2

期号：8

起止页码：1787

外文期刊名：ACS ELECTROCHEMISTRY

收录：Scopus(收录号：2-s2.0-105047003528);WOS:【ESCI(收录号:WOS:001842400200001)】；

基金：This research was supported by the Major Research Project (92577125), the National Natural Science Foundation of China (22272052), and the Baima Lake Laboratory Joint Fund of Zhejiang Provincial Natural Science Foundation of China (LBMHZ26B030001).

语种：英文

外文关键词：electrocatalysis; interfacial interactions; single nanoparticle; SECCM

摘要：Single-nanoparticle electrochemistry can uncover structure-activity relationships beyond ensemble averaging, yet nanoparticle-support interfacial interactions (NSIIs) are often overlooked in such studies. Here, we develop an optically addressed scanning electrochemical cell microscopy platform integrated with dark-field microscopy to directly quantify how NSIIs govern electrocatalytic behavior at the single nanoparticle level. Optical pre-selection allows the interrogation of individual Au microplates with matched size and morphology, while NSIIs are systematically tuned by functionalizing indium tin oxide electrodes with self-assembled monolayers, imparting neutral, positive, or negative surface charge. By combining single-particle voltammetry with localized electrochemical impedance spectroscopy, we demonstrate that repulsive NSIIs weaken physical contact and electronic coupling, leading to increased ohmic and charge-transfer resistances and reduced apparent activity. In contrast, attractive NSIIs promote intimate electrical contact, lower interfacial resistances, and substantially enhance the measured activity. Our findings establish NSIIs as a essential descriptor that must be explicitly considered to achieve accurate structure-activity relationships in single-particle electrocatalysis.