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Abstract:
Developing oxide supports for stabilizing single-atom catalysts enables more flexibility for tuning the electronic metal-support interactions (EMSIs) toward better catalytic activities. However, due to the electronegativity of oxygen anions, single-metal atoms often remain positively charged in these oxide supports and are poor at binding hydrogen species for the hydrogen evolution reaction (HER). Here, we report a ligand charge donation-acquisition balance strategy via an amorphous TiBxOy support to tune the EMSIs, which lead to the boosted HER mass activity of a single Pt atom catalyst. Based on spectroscopic characterizations, we found that Pt single atoms preferentially bonded with nearly neutral B atoms originating from TiB2-like species in the Ti-B-O framework rather than O anions. Density functional theory calculations reveal that due to the charge-transfer balance between B-O and B-Pt, the nucleophilicity of Pt was tuned to an optimum state, with an ideal hydrogen binding energy that benefits the HER. As a result, this Pt/TiBxOy catalyst achieves a high HER mass activity (37.8 A mg(-1) Pt) and a turnover frequency (33.2 H-2 s(-1) Pt site(-1)) at an overpotential of 50 mV in an acid medium, outperforming commercial Pt/C by a factor of 34 and 33, respectively.
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ACS CATALYSIS
ISSN: 2155-5435
Year: 2022
Issue: 10
Volume: 12
Page: 5970-5978
1 2 . 9
JCR@2022
1 2 . 9 0 0
JCR@2022
ESI Discipline: CHEMISTRY;
ESI HC Threshold:53
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 34
SCOPUS Cited Count: 32
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 0
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