Catalytic Metallopolymers from [2Fe-2S] Clusters: Artificial Metalloenzymes for Hydrogen Production

Metin Karayilan, William P. Brezinski, Kayla E. Clary, Dennis L. Lichtenberger, Richard S. Glass, Jeffrey Pyun

Research output: Contribution to journalReview articlepeer-review

35 Scopus citations


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.

Original languageEnglish (US)
Pages (from-to)7537-7550
Number of pages14
JournalAngewandte Chemie - International Edition
Issue number23
StatePublished - Jun 3 2019


  • energy conversion
  • enzymes
  • hydrogen
  • metallopolymers
  • water splitting

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)


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