2023
DOI: 10.1021/acs.jpcc.3c01057
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Choice of Electrolyte Impacts the Selectivity of Proton-Coupled Electrochemical Reactions on Hydrogen Titanate

Abstract: Proton-coupled electron transfer (PCET) reactions involving transition metal oxides are prevalent in aqueous electrochemical systems used for energy storage and conversion. Here, we elucidate the role of electrolyte on PCET mechanisms in transition metal oxides in aqueous acidic electrolytes using layered hydrogen titanate (H 2 Ti 3 O 7 ) as an example. We identify three processes by which electrolyte protons interact with hydrogen titanate at the electrochemical interface: (1) adsorption at the surface and/or… Show more

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Cited by 10 publications
(5 citation statements)
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“…This buffer independence is not a universal characteristic of binary materials. CVs of nickel and cobalt-layered double hydroxides (LDHs) have distinct E 1/2 values depending on the anions within the electrolyte ( e.g., phosphate, borate). , This has also been observed recently on layered hydrogen titanate (H 2 Ti 3 O 7 ) . When bunsenite nickel oxide is used as the electrode instead, its Faradaic features are independent of the buffers, supporting electrolytes, and even solvents. , In the latter system, the observed medium independence was ascribed, at least in part, to a small fraction of surface Ni sites solely being electrochemically active; this contrasts with LDHs that have up to near-unity addressability owing to their layered structure that allows diffusion of electrolytes throughout their lattice structures. , The low electrochemical addressability of Ce-MOF-808|FTO is ascribed to its low electrical conductivity; in other words, the observed electrochemical response must solely arise from the Ce 6 nodes near the underlying FTO surface.…”
Section: Discussionmentioning
confidence: 67%
“…This buffer independence is not a universal characteristic of binary materials. CVs of nickel and cobalt-layered double hydroxides (LDHs) have distinct E 1/2 values depending on the anions within the electrolyte ( e.g., phosphate, borate). , This has also been observed recently on layered hydrogen titanate (H 2 Ti 3 O 7 ) . When bunsenite nickel oxide is used as the electrode instead, its Faradaic features are independent of the buffers, supporting electrolytes, and even solvents. , In the latter system, the observed medium independence was ascribed, at least in part, to a small fraction of surface Ni sites solely being electrochemically active; this contrasts with LDHs that have up to near-unity addressability owing to their layered structure that allows diffusion of electrolytes throughout their lattice structures. , The low electrochemical addressability of Ce-MOF-808|FTO is ascribed to its low electrical conductivity; in other words, the observed electrochemical response must solely arise from the Ce 6 nodes near the underlying FTO surface.…”
Section: Discussionmentioning
confidence: 67%
“…Nonideal peak shapes have been previously reported for many TiO 2 -coated electrodes and shown to vary significantly with TiO 2 polymorph, electrolyte identity, , and other factors. TiO 2 reduction was traditionally attributed to occur at intraband electronic trap states but is now recognized as proton-coupled .…”
Section: Resultsmentioning
confidence: 99%
“…The ReaxFF-MD simulations are performed using the AMS2021 suite , and the CHONSMgPNaTiClFKLi.ff force field , suitable for describing these systems in a water environment . The CHONSMgPNaTiClFKLi.ff force field , is further validated with the estimation of p K a for benzenesulfonic acid in the water environment (see the Supporting Information, Section S1.1). Each starting system is built up from a 17.22 × 17.04 Å 2 graphene layer placed in a cell of 17.22 × 17.04 × 25.00 Å 3 dimensions (Figure a).…”
Section: Methodsmentioning
confidence: 99%