https://scholars.lib.ntu.edu.tw/handle/123456789/575723
Title: | Pt Single Atoms Supported on N-Doped Mesoporous Hollow Carbon Spheres with Enhanced Electrocatalytic H2-Evolution Activity | Authors: | Kuang P Wang Y Zhu B Xia F Tung C.-W Wu J HAO MING CHEN Yu J. |
Keywords: | Atoms; Carbon; Doping (additives); Durability; Electrocatalysis; Electrocatalysts; Electrolytes; Electron transport properties; Electronic states; Electronic structure; Hydrogen evolution reaction; Platinum; Platinum compounds; Acidic electrolytes; Coordination structures; Hollow carbon spheres; Intermediate specie; Spectroscopic characterization; Support interaction; Theoretical simulation; Turnover frequency; Phosphorus compounds | Issue Date: | 2021 | Journal Volume: | 33 | Journal Issue: | 18 | Source: | Advanced Materials | Abstract: | The electronic metal–support interaction (EMSI) plays a crucial role in catalysis as it can induce electron transfer between metal and support, modulate the electronic state of the supported metal, and optimize the reduction of intermediate species. In this work, the tailoring of electronic structure of Pt single atoms supported on N-doped mesoporous hollow carbon spheres (Pt1/NMHCS) via strong EMSI engineering is reported. The Pt1/NMHCS composite is much more active and stable than the nanoparticle (PtNP) counterpart and commercial 20?wt% Pt/C for catalyzing the electrocatalytic hydrogen evolution reaction (HER), exhibiting a low overpotential of 40?mV at a current density of 10?mA cm?2, a high mass activity of 2.07 A mg?1Pt at 50?mV overpotential, a large turnover frequency of 20.18 s?1 at 300?mV overpotential, and outstanding durability in acidic electrolyte. Detailed spectroscopic characterizations and theoretical simulations reveal that the strong EMSI effect in a unique N1?Pt1?C2 coordination structure significantly tailors the electronic structure of Pt 5d states, resulting in promoted reduction of adsorbed proton, facilitated H?H coupling, and thus Pt-like HER activity. This work provides a constructive route for precisely designing single-Pt-atom-based robust electrocatalysts with high HER activity and durability. ? 2021 Wiley-VCH GmbH |
URI: | https://www.scopus.com/inward/record.uri?eid=2-s2.0-85103955338&doi=10.1002%2fadma.202008599&partnerID=40&md5=4150f8332c6c200a191bff823db7111d https://scholars.lib.ntu.edu.tw/handle/123456789/575723 |
ISSN: | 9359648 | DOI: | 10.1002/adma.202008599 |
Appears in Collections: | 化學系 |
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