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Pt Single Atoms Supported on N‐Doped Mesoporous Hollow Carbon Spheres with Enhanced Electrocatalytic H 2 ‐Evolution Activity
Author(s) -
Kuang Panyong,
Wang Yaru,
Zhu Bicheng,
Xia Fanjie,
Tung ChingWei,
Wu Jinsong,
Chen Hao Ming,
Yu Jiaguo
Publication year - 2021
Publication title -
advanced materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.707
H-Index - 527
eISSN - 1521-4095
pISSN - 0935-9648
DOI - 10.1002/adma.202008599
Subject(s) - overpotential , materials science , mesoporous material , electrolyte , catalysis , electronic structure , electrocatalyst , carbon fibers , metal , chemical engineering , nanotechnology , chemistry , composite number , computational chemistry , electrode , electrochemistry , organic chemistry , composite material , engineering , metallurgy
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 (Pt 1 /NMHCS) via strong EMSI engineering is reported. The Pt 1 /NMHCS composite is much more active and stable than the nanoparticle (Pt NP ) 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 −1 Pt 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 N 1 −Pt 1 −C 2 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.