Single-phase perovskite oxide with super-exchange induced atomic-scale synergistic active centers enables ultrafast hydrogen evolution.

Autor: Dai J; State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, 210009, Nanjing, P.R. China., Zhu Y; Department of Chemical Engineering, Monash University, Clayton, VIC, 3800, Australia. yinlong.zhu@monash.edu., Tahini HA; Integrated Materials Design Laboratory, Department of Applied Mathematics, Research School of Physics and Engineering, Australian National University, Canberra, 2601, Australia., Lin Q; Department of Chemical Engineering, Monash University, Clayton, VIC, 3800, Australia., Chen Y; Monash Centre for Electron Microscopy, Monash University, Clayton, VIC, 3800, Australia., Guan D; State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, 210009, Nanjing, P.R. China., Zhou C; State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, 210009, Nanjing, P.R. China., Hu Z; Max Planck Institute for Chemical Physics of Solids, Nothnitzer Strasse 40, Dresden, 01187, Germany., Lin HJ; National Synchrotron Radiation Research Center, 101 Hsin-Ann Road, Hsinchu, 30076, Taiwan., Chan TS; National Synchrotron Radiation Research Center, 101 Hsin-Ann Road, Hsinchu, 30076, Taiwan., Chen CT; National Synchrotron Radiation Research Center, 101 Hsin-Ann Road, Hsinchu, 30076, Taiwan., Smith SC; Integrated Materials Design Laboratory, Department of Applied Mathematics, Research School of Physics and Engineering, Australian National University, Canberra, 2601, Australia., Wang H; Department of Chemical Engineering, Monash University, Clayton, VIC, 3800, Australia., Zhou W; State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, 210009, Nanjing, P.R. China., Shao Z; State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, 210009, Nanjing, P.R. China. shaozp@njtech.edu.cn.; Department of Chemical Engineering, Curtin University, Perth, WA, 6845, Australia. shaozp@njtech.edu.cn.
Jazyk: angličtina
Zdroj: Nature communications [Nat Commun] 2020 Nov 09; Vol. 11 (1), pp. 5657. Date of Electronic Publication: 2020 Nov 09.
DOI: 10.1038/s41467-020-19433-1
Abstrakt: The state-of-the-art active HER catalysts in acid media (e.g., Pt) generally lose considerable catalytic performance in alkaline media mainly due to the additional water dissociation step. To address this issue, synergistic hybrid catalysts are always designed by coupling them with metal (hydro)oxides. However, such hybrid systems usually suffer from long reaction path, high cost and complex preparation methods. Here, we discover a single-phase HER catalyst, SrTi 0.7 Ru 0.3 O 3-δ (STRO) perovskite oxide highlighted with an unusual super-exchange effect, which exhibits excellent HER performance in alkaline media via atomic-scale synergistic active centers. With insights from first-principles calculations, the intrinsically synergistic interplays between multiple active centers in STRO are uncovered to accurately catalyze different elementary steps of alkaline HER; namely, the Ti sites facilitates nearly-barrierless water dissociation, Ru sites function favorably for OH* desorption, and non-metal oxygen sites (i.e., oxygen vacancies/lattice oxygen) promotes optimal H* adsorption and H 2 desorption.
Databáze: MEDLINE
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