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Interfacial Chemical Bond‐Modulated Z‐Scheme Charge Transfer for Efficient Photoelectrochemical Water Splitting
Author(s) -
Xu Weiwei,
Tian Wei,
Meng Linxing,
Cao Fengren,
Li Liang
Publication year - 2021
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.202003500
Subject(s) - heterojunction , overlayer , materials science , photocurrent , band bending , water splitting , redox , reversible hydrogen electrode , fermi level , charge carrier , chemical physics , photocatalysis , electrochemistry , electrode , nanotechnology , optoelectronics , chemistry , catalysis , working electrode , physics , biochemistry , quantum mechanics , electron , metallurgy
The Z‐scheme heterojunction has great potential in photoelectrochemical (PEC) water splitting due to its unique charge‐carrier migration pathway, superior carrier separation efficiency, and high redox capacity, but how to regulate the Z‐scheme charge transfer at the nanometric interface of heterostructures still remains a big challenge. Herein, InOCd bond is rationally introduced at the interface between ZnIn 2 S 4 nanosheets and CdS nanoparticles through a facile cation exchange reaction, which successfully converts the previously reported type II band structure to a direct Z‐scheme heterojunction (ZnIn 2 S 4 /CdS) as confirmed by various characterizations. Density functional theory calculation reveals that the InOCd interfacial chemical bond significantly uplifts the Fermi level of ZnIn 2 S 4 and CdS, inverts the interfacial band bending direction, thus resulting in the formation of Z‐scheme heterojunction. Moreover, an amorphous ZnO overlayer is deposited to eliminate the surface defects and accelerate the surface reaction kinetics. Benefiting from the superior charge separation efficiency and high redox ability originating from the Z‐scheme structure, the optimum ZnIn 2 S 4 /CdS/ZnO photoanode exhibits a dramatically enhanced PEC performance with low onset potential (−0.03 V vs reversible hydrogen electrode, V RHE ) and large photocurrent of 3.48 mA cm −2 at 1.23 V RHE , which is about 21.75 times that of pristine ZnIn 2 S 4 .