Amino group promoted photocatalytic hydrogen evolution activity observed in two copper()-based layered complexes

Two copper( ii )-based layered complexes with or without the amino group, [Cu(HL) 2 (NH 2 -BDC)] n ( 1 ) and [Cu(HL) 2 (BDC)] n ( 2 ) (HL = 4′-(4-hydroxyphenyl)-4,2′:6′,4′′-terpyridine, NH 2 -H 2 BDC = 2-amino-1,4-benzenedicarboxylic acid and H 2 BDC = 1,4-benzenedicarboxylic acid), were solvotherma...

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Published in:Dalton transactions : an international journal of inorganic chemistry 2018, Vol.47 (36), p.12726-12733
Main Authors: Li, Lei, Zhu, Shuang, Hao, Rui, Wang, Jia-Jun, Yang, En-Cui, Zhao, Xiao-Jun
Format: Article
Language:English
Subjects:
Catalysis
Catalytic activity
Charge transfer
Conduction bands
Coordination compounds
Copper
Copper compounds
Crystallography
Density functional theory
Electrochemical impedance spectroscopy
Electron density
Fluorescence
Format
Hydrogen evolution
Hydrogen production
Light irradiation
Mathematical analysis
Photocatalysis
Photocatalysts
Photoelectric effect
Photoelectric emission
Spectrum analysis
Water chemistry
Water splitting
X ray photoelectron spectroscopy
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Summary:Two copper( ii )-based layered complexes with or without the amino group, [Cu(HL) 2 (NH 2 -BDC)] n ( 1 ) and [Cu(HL) 2 (BDC)] n ( 2 ) (HL = 4′-(4-hydroxyphenyl)-4,2′:6′,4′′-terpyridine, NH 2 -H 2 BDC = 2-amino-1,4-benzenedicarboxylic acid and H 2 BDC = 1,4-benzenedicarboxylic acid), were solvothermally synthesized and used as photocatalysts to accelerate hydrogen production from water splitting. The amino group modified 1 has exhibited greatly enhanced photocatalytic activity with a hydrogen production rate of 2.34 mmol g −1 h −1 under visible light irradiation, which is almost double that of 2 . Density functional theory calculations, electrochemical impedance spectroscopy and transient photocurrent tests demonstrate that the higher catalytic activity of 1 than 2 is a result of the enriched electron density around the Cu II center by the amino group, which facilitates the charge transfer from the conduction band to the water molecule. The amino group effect of the photocatalyst on the catalytic activity of water splitting was investigated under visible light irradiation. The hydrogen production rate of the amino group modified layered complex is almost double that without the amino group.
ISSN:1477-9226
1477-9234
DOI:10.1039/c8dt02803f