Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 61, Issue 47, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202212196
Keywords
Electrocatalyst; Hydrogen Evolution Reaction; Hydrogen Spillover; Oxygen Vacancy; Support-Structure Engineering
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Funding
- Taishan Scholar Program of Shandong Province, China [ts201712045]
- National Natural Science Foundation of China [22102079]
- Natural Science Foundation of Shandong Province of China [ZR2021YQ10]
- Talent Foundation - Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering [STHGYX2207]
- Ulsan National Institute of Science and Technology (UNIST) [1.190002.01]
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In this study, a Ru cluster anchored on a trace P-doped defective TiO2 substrate (Ru/P-TiO2) was synthesized as an electrocatalyst for the hydrogen evolution reaction (HER) in alkaline media. The Ru/P-TiO2 exhibited superior activity compared to commercial Pt/C and Ru/TiO2 materials. Experimental and theoretical studies revealed that the rutile-TiO2 crystal phase substrate with rich surface oxygen vacancies facilitated water adsorption and dissociation, while P substitution enhanced hydrogen generation by promoting hydrogen spillover, synergistically enhancing the HER activity.
Synergistic optimization of the elementary steps of water dissociation and hydrogen desorption for the hydrogen evolution reaction (HER) in alkaline media is a challenge. Herein, the Ru cluster anchored on a trace P-doped defective TiO2 substrate (Ru/P-TiO2) was synthesized as an electrocatalyst for the HER; it exhibited a commercial Pt/C-like geometric activity and an excellent mass activity of 9984.3 mA mg(Ru)(-1) at -0.05 V vs. RHE, which is 34.3 and 18.7 times higher than that of Pt/C and Ru/TiO2, respectively. Experimental and theoretical studies indicated that using a rutile-TiO2-crystal-phase substrate enhanced the HER activity more than the anatase phase. Rich surface oxygen vacancies on rutile-TiO2 facilitated the adsorption and dissociation of water, while the partial substitution of Ti4+ with P5+ enhanced H-2 generation by facilitating hydrogen spillover from the Ru site to the surface P site, synergistically enhancing the HER activity.
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