Understanding alkali contamination in colloidal nanomaterials to unlock grain boundary impurity engineering
Author(s)
Type
Journal Article
Abstract
Metal nanogels combine a large surface area, a high structural stability, and a high catalytic activity toward a variety of chemical reactions. Their performance is underpinned by the atomic-level distribution of their constituents, yet analyzing their subnanoscale structure and composition to guide property optimization remains extremely challenging. Here, we synthesized Pd nanogels using a conventional wet chemistry route, and a near-atomic-scale analysis reveals that impurities from the reactants (Na and K) are integrated into the grain boundaries of the poly crystalline gel, typically loci of high catalytic activity. We demonstrate that the level of impurities is controlled by the reaction condition. Based on ab initio calculations, we provide a detailed mechanism to explain how surface-bound impurities become trapped at grain boundaries that form as the particles coalesce during synthesis, possibly facilitating their decohesion. If controlled, impurity integration into grain boundaries may offer opportunities for designing new nanogels.
Date Issued
2022-01-19
Date Acceptance
2022-01-01
Citation
Journal of the American Chemical Society, 2022, 144 (2), pp.987-994
ISSN
0002-7863
Publisher
American Chemical Society
Start Page
987
End Page
994
Journal / Book Title
Journal of the American Chemical Society
Volume
144
Issue
2
Copyright Statement
© 2022 The Authors. Published by American Chemical Society
License URL
Identifier
https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000741117600001&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=a2bf6146997ec60c407a63945d4e92bb
Subjects
AEROGELS
ATOM-PROBE TOMOGRAPHY
Chemistry
CHEMISTRY
Chemistry, Multidisciplinary
ELECTROCATALYSTS
GROWTH
HIGH-PERFORMANCE
NANOPARTICLES
PD
Physical Sciences
REDUCTION
Science & Technology
SEGREGATION
Publication Status
Published
Date Publish Online
2022-01-04