Interlayer pillaring influences the octahedral tilting and electrochemical capacity of tungsten oxides

Ding, Ran; Spencer, Michael A.; Holzapfel, Noah P.; Chagnot, Matthew; Augustyn, Veronica

doi:10.1039/D4TA08647C

Interlayer pillaring influences the octahedral tilting and electrochemical capacity of tungsten oxides

Journal Article · Wed Feb 26 00:00:00 EST 2025 · Journal of Materials Chemistry. A

DOI:https://doi.org/10.1039/D4TA08647C· OSTI ID:2524076

^[1]; Spencer, Michael A. ^[1]; ^[1]; Chagnot, Matthew ^[1]; ^[1]

North Carolina State University, Raleigh, NC (United States)

One strategy to tune the electrochemical properties of layered inorganic materials for energy storage and conversion is to introduce molecular organic pillars. We investigated how pillaring tungsten oxides with alkylammonium cations influences their physical and electrochemical properties relative to the non-pillared host. While the presence of alkylammonium increased the interlayer spacing, we found that the electrochemical capacity of the materials decreased in non-aqueous electrolytes. In aqueous acidic electrolytes, replacement of the interlayer alkylammonium pillars with water molecules led to the recovery of the electrochemical capacity. We rationalize these results based on the influence of interlayer pillars on the degree of octahedral tilting within the inorganic tungsten oxide layers. The presence of alkylammonium in the interlayer leads to an increase in octahedral tilting relative to interlayer water. In turn, this leads to an increase in the band gap and corresponding decrease in the electrochemical capacity. Our findings emphasize the correlation between the chemical nature of the interlayer molecular pillars and the electronic structure, which in turn affects the electrochemical capacity.

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Research Organization:: North Carolina State University, Raleigh, NC (United States); Stanford Univ., CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-76SF00515; SC0020234

OSTI ID:: 2524076

Alternate ID(s):: OSTI ID: 2571033

Journal Information:: Journal of Materials Chemistry. A, Journal Name: Journal of Materials Chemistry. A Journal Issue: 12 Vol. 13; ISSN 2050-7488; ISSN 2050-7496

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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