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Antimony Complexes for Electrocatalysis: Activity of a Main-Group Element in Proton Reduction

Journal Article · · Angewandte Chemie (International Edition)
 [1];  [2];  [2];  [2];  [2];  [2];  [2]
  1. Yale Univ., New Haven, CT (United States); DOE/OSTI
  2. Yale Univ., New Haven, CT (United States)
+ Show Author Affiliations
Main-group complexes are shown to be viable electrocatalysts for the H2-evolution reaction (HER) from acid. A series of antimony porphyrins with varying axial ligands were synthesized for electrocatalysis applications. The proton-reduction catalytic properties of TPSb(OH)2 (TP=5,10,15,20-tetra(p-tolyl)porphyrin) with two axial hydroxy ligands were studied in detail, demonstrating catalytic H2 production. Experiments, in conjunction with quantum chemistry calculations, demonstrate that the catalytic cycle is driven via the redox activity of both the porphyrin ligand and the Sb center. This study brings insight into main group catalysis and the role of redox-active ligands during catalysis.
Research Organization:
Yale Univ., New Haven, CT (United States)
Sponsoring Organization:
TomKat Foundation; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
FG02-07ER15909
OSTI ID:
1533110
Alternate ID(s):
OSTI ID: 1374916
Journal Information:
Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 31 Vol. 56; ISSN 1433-7851
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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A squaraine-linked metalloporphyrin two-dimensional polymer photocatalyst for hydrogen and oxygen evolution reactions journal January 2019
Remote ion-pair interactions in Fe-porphyrin-based molecular catalysts for the hydrogen evolution reaction journal January 2019
Electrocatalytic hydrogen evolution with gallium hydride and ligand-centered reduction journal January 2019
A Recycling Hydrogen Supply System of NaBH4 Based on a Facile Regeneration Process: A Review journal January 2018

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
antimony
chemistry
electrocatalysis
main-group elements
porphyrins
proton reduction