TY - JOUR
T1 - Catalytic Metallopolymers from [2Fe-2S] Clusters
T2 - Artificial Metalloenzymes for Hydrogen Production
AU - Karayilan, Metin
AU - Brezinski, William P.
AU - Clary, Kayla E.
AU - Lichtenberger, Dennis L.
AU - Glass, Richard S
AU - Pyun, Jeffrey
N1 - Funding Information:
DLL, RSG, and JP gratefully acknowledge support of this work by NSF (CHE-1664745).
Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
PY - 2019/6/3
Y1 - 2019/6/3
N2 - Reviewed herein is the development of novel polymer-supported [2Fe-2S] catalyst systems for electrocatalytic and photocatalytic hydrogen evolution reactions. [FeFe] hydrogenases are the best known naturally occurring metalloenzymes for hydrogen generation, and small-molecule, [2Fe-2S]-containing mimetics of the active site (H-cluster) of these metalloenzymes have been synthesized for years. These small [2Fe-2S] complexes have not yet reached the same capacity as that of enzymes for hydrogen production. Recently, modern polymer chemistry has been utilized to construct an outer coordination sphere around the [2Fe-2S] clusters to provide site isolation, water solubility, and improved catalytic activity. In this review, the various macromolecular motifs and the catalytic properties of these polymer-supported [2Fe-2S] materials are surveyed. The most recent catalysts that incorporate a single [2Fe-2S] complex, termed single-site [2Fe-2S] metallopolymers, exhibit superior activity for H2 production.
AB - Reviewed herein is the development of novel polymer-supported [2Fe-2S] catalyst systems for electrocatalytic and photocatalytic hydrogen evolution reactions. [FeFe] hydrogenases are the best known naturally occurring metalloenzymes for hydrogen generation, and small-molecule, [2Fe-2S]-containing mimetics of the active site (H-cluster) of these metalloenzymes have been synthesized for years. These small [2Fe-2S] complexes have not yet reached the same capacity as that of enzymes for hydrogen production. Recently, modern polymer chemistry has been utilized to construct an outer coordination sphere around the [2Fe-2S] clusters to provide site isolation, water solubility, and improved catalytic activity. In this review, the various macromolecular motifs and the catalytic properties of these polymer-supported [2Fe-2S] materials are surveyed. The most recent catalysts that incorporate a single [2Fe-2S] complex, termed single-site [2Fe-2S] metallopolymers, exhibit superior activity for H2 production.
KW - energy conversion
KW - enzymes
KW - hydrogen
KW - metallopolymers
KW - water splitting
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U2 - 10.1002/anie.201813776
DO - 10.1002/anie.201813776
M3 - Review article
C2 - 30628136
AN - SCOPUS:85062568025
SN - 1433-7851
VL - 58
SP - 7537
EP - 7550
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 23
ER -