Published: Jan. 1, 2025
Language: Английский
ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(3), P. 1942 - 1951
Published: Jan. 17, 2025
Iridium-based electrocatalysts are the most promising candidates for acidic oxygen evolution reaction (OER). Considering their high cost and scarcity, it is imperative to maximize atom utilization enhance intrinsic activity of iridium. In this work, IrOx sub-2 nm clusters stabilized on TiO2 supports via metal support interaction (MSI) induced by vacancy defects in TiO2. The strength MSI readily tuned type vacancies: vacancies (VO-TiO2) induce adsorbed with relatively weak strength, while titanium (VTi-TiO2) lead strong embedded MSI. tunable further modulates electronic structure clusters. IrOx/VO-TiO2 exhibits an optimized a downshifted d-band center IrOx, resulting reduced binding energy low barrier rate-determining step OER. Consequently, delivers twice that commercial IrO2 good stability 120 h practical proton exchange membrane water electrolyzer. Our study provides guideline rational design OER catalysts based modulating
Language: Английский
Citations
1
The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 924 - 931
Published: Jan. 20, 2025
Understanding the mechanism of nitrogen reduction reaction (NRR) is essential for designing highly efficient catalysts. In this study, we investigated effects metal–support interaction (MSI) on NRR using density functional theory. The simulations revealed that MSI weak in Au13/BiOCl system, with charge accumulation and depletion primarily occurring within Au13 cluster. By replacement one Au atom either a Ag or Pt atom, becomes stronger compared to system. because doping breaks symmetry cluster, leading at interface. Specifically, enhanced reduces energy barriers rate-determining step from 1.07 eV system 0.91 Au12Ag/BiOCl 0.87 Au12Pt/BiOCl, respectively. Our study uncovers critical role activity NRR, providing theoretical insights development
Language: Английский
Citations
0
ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 13, 2025
Metal–support interactions (MSI) play a crucial role in enhancing the catalytic activity and stability of metal catalysts by establishing stable metal-oxide interface. However, precisely controlling MSI at atomic scale remains significant challenge, as how to construct an optimal is still not fully understood: Both insufficient excessive showed inferior performance. In this study, we propose finely tuning using temporal-precise transient high-temperature pulse heating. Using Pt/CeO2 model system, systematically investigate variations duration atmosphere influence reconstruction metal–support interface MSIs. This leads formation two distinct types MSI: (1) strong (SMSI, Pt@CeO2) (2) reactive (RMSI, Pt5Ce@CeO2), each with unique compositions, structures, electrochemical behaviors. Notably, Pt5Ce@CeO2 RMSI exhibits remarkable performance alkaline hydrogen evolution, showing overpotential −29 mV operation for over 300 h −10 mA·cm–2. Theoretical studies reveal that alloying Pt Ce form Pt5Ce modifies electronic structure Pt, shifting d-band center optimize adsorption dissociation intermediates, thereby reducing reaction energy barrier. Moreover, intimate interaction CeO2 further improves stability. Our strategy enables precise, stepwise, controllable regulation MSIs, providing insights development highly efficient durable heterostructured wide range applications.
Language: Английский
Citations
0
Published: Jan. 1, 2025
Language: Английский
Citations
0