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DOE OSTI2022

Deciphering Photochemical Reaction Pathways of Aqueous Tetrachloroauric Acid by X-ray Transient Absorption Spectroscopy

Photolysis reaction pathways of [Au(III)Cl 4 ] - in aqueous solution have been investigated by time-resolved X-ray absorption spectroscopy. Ultraviolet excitation directly breaks the Au-Cl bond in [Au(III)Cl 4 ] - to form [Au(II)Cl 3 ] - that becomes highly reactive within 79 ps. Disproportionation of [Au(II)Cl 3 ] - generates [Au(I)Cl 2 ] - , which is stable for ≤ 10 mu s. In contrast, intense near-infrared lasers photolyze water to generate hydrated electrons, which then reduce [Au(III)Cl 4 ] - to [Au(II)Cl 3 ] - at 5 ns. Hydrated electrons further induce a chain reaction from [Au(II)Cl 3 ] - to [Au(0)Cl] - by successively removing one Cl - . The zero-valency Au anions quickly polymerize and condense to form Au nanoparticles, which become the dominating product after 400 s. Here our results reveal that the condensation of zero-valency Au starts with dimerization of gold clusters coordinated with chloride ions rather than direct condensation of pristine Au atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Materials Data on AuCl3 by Materials Project

AuCl3 is Protactinium structured and crystallizes in the monoclinic P2_1/c space group. The structure is zero-dimensional and consists of two trichlorogold molecules. Au3+ is bonded in a rectangular see-saw-like geometry to four Cl1- atoms. There are two shorter (2.28 Å) and two longer (2.38 Å) Au–Cl bond lengths. There are three inequivalent Cl1- sites. In the first Cl1- site, Cl1- is bonded in an L-shaped geometry to two equivalent Au3+ atoms. In the second Cl1- site, Cl1- is bonded in a single-bond geometry to one Au3+ atom. In the third Cl1- site, Cl1- is bonded in a single-bond geometry to one Au3+ atom.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on AuCl by Materials Project

AuCl crystallizes in the tetragonal I4_1/amd space group. The structure is one-dimensional and consists of four AuCl ribbons oriented in the (1, 0, 0) direction. Au1+ is bonded in a linear geometry to two equivalent Cl1- atoms. Both Au–Cl bond lengths are 2.33 Å. Cl1- is bonded in a water-like geometry to two equivalent Au1+ atoms.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Materials Data on AuCl2 by Materials Project

AuCl2 crystallizes in the triclinic P-1 space group. The structure is one-dimensional and consists of one AuCl2 ribbon oriented in the (-1, 0, 1) direction. there are two inequivalent Au2+ sites. In the first Au2+ site, Au2+ is bonded in a distorted T-shaped geometry to three Cl1- atoms. There are a spread of Au–Cl bond distances ranging from 2.31–3.15 Å. In the second Au2+ site, Au2+ is bonded in a rectangular see-saw-like geometry to four Cl1- atoms. There are a spread of Au–Cl bond distances ranging from 2.31–2.39 Å. There are four inequivalent Cl1- sites. In the first Cl1- site, Cl1- is bonded in a water-like geometry to two Au2+ atoms. In the second Cl1- site, Cl1- is bonded in a water-like geometry to two Au2+ atoms. In the third Cl1- site, Cl1- is bonded in a single-bond geometry to one Au2+ atom. In the fourth Cl1- site, Cl1- is bonded in a distorted bent 150 degrees geometry to two Au2+ atoms.

36 MATERIALS SCIENCE↗