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Unveiling the Nature of Pt Single‐Atom Catalyst during Electrocatalytic Hydrogen Evolution and Oxygen Reduction Reactions
Author(s) -
Li Junjie,
Banis Mohammad Norouzi,
Ren Zhouhong,
Adair Keegan R.,
DoyleDavis Kieran,
Meira Debora Motta,
Finfrock Y. Zou,
Zhang Lei,
Kong Fanpeng,
Sham TsunKong,
Li Ruying,
Luo Jun,
Sun Xueliang
Publication year - 2021
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.202007245
Subject(s) - catalysis , x ray absorption spectroscopy , hydrogen , materials science , adsorption , carbon fibers , chemistry , absorption spectroscopy , inorganic chemistry , photochemistry , organic chemistry , physics , quantum mechanics , composite number , composite material
Single‐atom catalysts (SACs) have attracted significant attention due to their superior catalytic activity and selectivity. However, the nature of active sites of SACs under realistic reaction conditions is ambiguous. In this work, high loading Pt single atoms on graphitic carbon nitride (g‐C 3 N 4 )‐derived N‐doped carbon nanosheets (Pt 1 /NCNS) is achieved through atomic layer deposition. Operando X‐ray absorption spectroscopy (XAS) is performed on Pt single atoms and nanoparticles (NPs) in both the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). The operando results indicate that the total unoccupied density of states of Pt 5 d orbitals of Pt 1 atoms is higher than that of Pt NPs under HER condition, and that a stable Pt oxide is formed during ORR on Pt 1 /NCNS, which may suppress the adsorption and activation of O 2 . This work unveils the nature of Pt single atoms under realistic HER and ORR conditions, providing a deeper understanding for designing advanced SACs.