期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 125, 期 42, 页码 23226-23230出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.1c08197
关键词
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资金
- JST, CREST [JPMJCR20B2]
- Elements Strategy Initiative for Catalysts & Batteries (ESICB) of MEXT [JPMXP0112101003]
- JSPS KAKENHI [JP19K15499, JP20H00370]
The effects of alkynyl and thiolate ligands on the catalytic activities of Au-25 and PtAu24 nanoparticles for the hydrogen evolution reaction were studied. It was found that alkynyl ligands significantly enhanced the HER activity of Au-25, while the effect on PtAu24 was negligible.
We studied the effects of the alkynyl and thiolate ligands (L) on the catalytic activities of Au-25(L)(18) and PtAu24(L)(18) for the hydrogen evolution reaction (HER): the ligands used were C CArF (Ar-F = 3,5-bis(trifluoromethyl)-phenyl) and SC2H4Ph. The onset potential for Au-25(C CArF)(18) was shifted to the positive side by similar to 70 mV with respect to that for Au-25(SC2H4Ph)(18), indicating that the HER activity of the pure Au-13 core was significantly enhanced when protected by alkynyl ligands. This remarkable ligand effect was explained by the acceleration of the protonation step to the more negatively charged Au-25(C CArF)(18) than the less negatively charged Au-25(SC2H4Ph)(18). In contrast, the HER activities of the doped PtAu24(C CArF)(18) and PtAu24(SC2H4Ph)(18) were comparable. The negligible ligand effect on the activity of the Pt@Au-12 core was ascribed to the change in the rate-determining step from the protonation step to the reductive regeneration step of the catalysts.
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