Details

Autor(en) / Beteiligte

• Wang, Dongdi
• Xue, Jiawei
• Ding, Xilan
• Wei, Jie
• Feng, Chen
• Wang, Ruyang
• Ma, Peiyu
• Wang, Sicong
• Cao, Heng
• Wang, Jingyan
• Zuo, Ming
• Zhou, Shiming
• Zhang, Zhirong
• Zeng, Jie
• Bao, Jun

Titel

Neighboring Cationic Vacancy Assisted Adsorption Optimization on Single-Atom Sites for Improved Oxygen Evolution

Ist Teil von

• ACS catalysis, 2022-10, Vol.12 (19), p.12458-12468

Ort / Verlag

American Chemical Society

Erscheinungsjahr

2022

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Single-atom catalysts with particular electronic and geometric microenvironments provide an atomic-scale perspective for research into the mechanism of catalysis. Designing the neighboring geometry of single-atom catalysts can tailor the adsorption configuration of reaction intermediates and enhance their activity in catalytic reactions. In this work, we proposed a neighboring cationic vacancy strategy in single-atom Ru catalysts to adjust the adsorption configuration of reaction intermediates for improved oxygen evolution performance. An Ru single-atom catalyst with neighboring Co2+ vacancies (Ru1/VCo-Co­(OH)2) showed better OER performance than a catalyst without Co2+ vacancies (Ru1/Co­(OH)2). The mass activity of Ru1/VCo-Co­(OH)2 was calculated to be 6688 A g–1 at 300 mV overpotential, which was 4.73 times higher than that of Ru1/Co­(OH)2. Particularly, the mass activity of Ru1/VCo-Co­(OH)2 was notably 481.15 times higher than that of commercial RuO2. Both in situ ATR-FTIR spectroscopy measurements and DFT calculations manifested that the existence of neighboring Co2+ vacancies modulated the adsorption configuration of *OOH intermediates on atomic Ru sites by hydrogen bonding, which reduced the energy barrier of rate-determining steps and improved the OER activity.