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Interfacial Water Coordination on Ruthenium Oxide Nanoparticles Confined Within Covalent Organic Framework and Its
Yun Li1, Xin Zhao1,2, Arsenii S Portniagin1
1Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, Hong Kong SAR, P. R. China.
Abstract:
Electrochemical nitrate reduction reaction (NO3RR) enables sustainable and decentralized ammonia production. Here, we demonstrate how oxygen-deficient ruthenium oxide (RuOx) nanoparticles confined within the imine-based covalent organic framework (COF) produced from 1,3,5-tris(4-aminophenyl)benzene (TAPB) achieve highly efficient nitrate-to-ammonia conversion, delivering a high Faradaic efficiency of 99.2% at -1.1 V vs Ag/AgCl in a neutral electrolyte. Crystal structure, optical spectra, and electronic state analysis reveal the strong interaction between RuOx nanoparticles and TAPB-COF. The confined nanoparticles change the interlayer spacing of TAPB-COF, which in turn results in the high oxygen-deficiency of RuOx. Investigations by in situ optical spectroscopies and ab initio molecular dynamics simulations reveal the occurrence of a repelling effect on water molecules at the surface of hydrophobic TAPB-COF framework, which contributes to the prevalence of 2-coordinated water at the surface of RuOx nanoparticles. This ensures a slow-down proton transfer kinetics, leading to suppression of the hydrogen generation as an undesired competing process. The upshift of d-band center and bridge-site adsorption due to the high oxygen-deficiency and the shortened Ru-Ru distance of the confined RuOx nanoparticles contribute to the strengthened bonding of *NO2 and *NOH intermediates, which alleviates the nitrite production and accelerates the NO3RR process.
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