Activation of H 2 O by ThO 2 – Experimental and Computational Studies

Tufekci, Burak A. [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000269646630); Chiba, Tatsuya [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000291891309); Xu, Jinheng [Johns Hopkins University, Baltimore, MD (United States)]; Cheng, Lan [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000311659559); Bowen, Kit H. [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000228586352)

doi:10.1021/acs.jpca.4c06238

DOE OSTI · 2499270

Activation of H 2 O by ThO 2 – Experimental and Computational Studies

Tufekci, Burak A. [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000269646630)·Chiba, Tatsuya [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000291891309)·Xu, Jinheng [Johns Hopkins University, Baltimore, MD (United States)]·Cheng, Lan [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000311659559)·Bowen, Kit H. [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000228586352)

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Abstract

Here, a synergetic study that utilized anion photoelectron spectroscopy and high-level abinitio calculations has explored the activation of H 2 O molecules by ThO 2 – molecular anions. Both experiment and theory found conclusive evidence for said activation. In the experiments, this appeared as a tell-tale directional shift in the spectral profile of the anionic complex that ruled out physisorption,i.e., ThO 2 – (H 2 O), and implied chemisorption. In the computations, good agreement was found between the calculated and measured vertical detachment energies, and the atomic connectivity (the structure) of the resulting anionic complex was found to be [OTh(OH) 2 ] – .

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Anions Binding energy Chemical calculations Electrical energy Quantum mechanics

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Tufekci, Burak A. [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000269646630), Chiba, Tatsuya [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000291891309), Xu, Jinheng [Johns Hopkins University, Baltimore, MD (United States)], Cheng, Lan [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000311659559), Bowen, Kit H. [Johns Hopkins University, Baltimore, MD (United States)] (ORCID:0000000228586352). 2024-12-30. Activation of H 2 O by ThO 2 – Experimental and Computational Studies. https://doi.org/10.1021/acs.jpca.4c06238

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