纳米材料的性能在很大程度上取决于界面微环境,其中表面活性剂作为吸附剂起着至关重要的作用,但它在界面反应中的参与往往被忽视。
该文中,研究人员发现柠檬酸盐和抗坏血酸这两种主要用于胶体金纳米粒子(Au NPs)的表面活性剂,可以在环境下与痕量含氮残留物自发发生催化反应,形成肟,随后肟被裂解产生CN或含有-CN基团的化合物。
这种催化反应在反应物(包括各种碳质和含氮源)和金属催化剂(包括Au、Ag、Fe、Cu、Ni、Pt和Pd NP)中显示出广泛的普遍性。此外,随着该反应的去除,在没有施加电势的环境条件下,通过表面增强拉曼光谱,观察到具有不同吸附构型的吸附CO。
该工作强调了表面活性剂在界面微环境中不可忽视的重要性,并为界面化学反应的基本理解提供了至关重要的见解。
附:英文原文
Title: Spontaneous Catalytic Reaction of a Surfactant in the Interfacial Microenvironment of Colloidal Gold Nanoparticles
Author: Si-Qi Pan, Ping Luo, Qiuting Huang, Jinjuan Xue, Xiang-Dong Tian, Bin Xu, Jianfeng Wu, Jia Chen, Jianwei Xie, Na Yang, Xia-Guang Zhang, Zhong-Qun Tian, Guo-Kun Liu
Issue&Volume: January 7, 2025
Abstract: The performance of nanomaterials is significantly determined by the interfacial microenvironment, in which a surfactant plays an essential role as the adsorbent, but its involvement in the interfacial reaction is often overlooked. Here, it was discovered that citrate and ascorbic acid, the two primarily used surfactants for colloidal gold nanoparticles (Au NPs), can spontaneously undergo catalytic reaction with trace-level nitrogenous residue under ambient environment to form oxime, which is subsequently cleaved to generate CN– or a compound containing the –CN group. Such a catalytic reaction shows wide universality in both reactants, including various carbonaceous and nitrogenous sources, and metal catalysts, including Au, Ag, Fe, Cu, Ni, Pt, and Pd NPs. Furthermore, with the removal of this reaction, adsorbed CO with diverse adsorption configurations was observed via surface-enhanced Raman spectroscopy under ambient conditions without an applied potential. Our work highlights the non-negligible significance of surfactants in interfacial microenvironments and provides crucial insights into the fundamental understanding of interfacial chemical reactions.
DOI: 10.1021/jacs.4c16796
Source: https://pubs.acs.org/doi/abs/10.1021/jacs.4c16796
JACS:《美国化学会志》,创刊于1879年。隶属于美国化学会,最新IF:16.383
官方网址:https://pubs.acs.org/journal/jacsat
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