Journal
ACS NANO
Volume 14, Issue 7, Pages 8689-8696Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.0c03050
Keywords
nanogap; colloidal gold; gold atom movement; capping agent; ligand; SERS reproducibility; citrate binding
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Funding
- EPSRC [EP/L027151/1, EP/R020965/1, EP/P029426/1, EP/L015889/1]
- Leverhulme Trust
- Isaac Newton Trust
- Winton Foundation for the Physics of Sustainability
- EPSRC [EP/P029426/1, EP/H007024/1, EP/R020965/1, EP/L027151/1] Funding Source: UKRI
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Gold nanoparticles used in many types of nanostructure are mostly stabilized by citrate ligands. Fully understanding their dynamic surface chemistry is thus essential for applications, particularly since aging is frequently a problem. Using surface-enhanced Raman spectroscopy in conjunction with density functional theory calculations, we are able to determine Au-citrate coordination in liquid with minimal invasiveness. We show that citrate coordination is mostly bidentate and simply controlled by its protonation state. More complex binding motifs are caused by interfering chloride ions and gold adatoms. With increasing age of stored gold nanoparticle suspensions, gold adatoms are found to move atop the Au facets and bind to an additional terminal carboxylate of the citrate. Aged nanoparticles are fully refreshed by removing these adatoms, using etching and subsequent boiling of the gold nanoparticles.
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