Document Type

Article

Publication Date

2015

Abstract

This density functional theory (DFT) investigation examines the formation of nonradical Au(0) species from the reduction of Au(I) species. The Au(I) complexes of interest are AuCl2, AuBr2, AuI2, AuClPH3, and AuCl(H)SCH3(−), which are precursors for gold nanoparticle and cluster formation. Reaction of two of the Au(I) species with a hydride results in ejection of two of the ligands and formation of Au2 with two ligands still attached. AuX2 (where X = Cl, Br, or I) reactions eject two halides and form Au2X22–. AuClL(−) (where L = PH3, HSCH3, or SCH3) reactions can eject either chloride, HCl, PH3, HSCH3, or SCH3 and form Au(0)L2q or Au(0)ClLq (q = 0, 1, 2). The Au2Cl22– complex can further react with AuCl2, which forms Au3Cl32– and a chloride anion. The new Au3Cl32– species can then react with AuCl2 or Au2Cl22– or with another Au3Cl32–. Larger clusters can be formed from these precursors. In this work, reactions in both methanol and benzene solvents are considered as models for one-phase and two-phase gold nanoparticle growth processes. Overall, this investigation shows how Au(0)-containing species can be formed without assuming the formation of Au(0) atoms (radical species).

Comments

Barngrover, Brian M., Timothy J. Manges, and Christine M. Aikens. "Prediction of Nonradical Au (0)-Containing Precursors in Nanoparticle Growth Processes." The Journal of Physical Chemistry A 119, no. 5 (2015): 889-895.

Posted with permission from the American Chemical Society.


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