Affiliation:
1. Chemistry Department Indian Institute of Technology 400076 Bombay Maharashtra India
2. National center of Excellence CCU Indian Institute of Technology 400076 Bombay Maharashtra India
3. Interdisciplinary Program Climate Studies Indian Institute of Technology 400076 Bombay Maharashtra India
Abstract
AbstractThe development of potent H2 production catalysts is a key aspect in our journey toward the establishment of a sustainable carbon‐neutral power infrastructure. Hydrogenase enzymes provide the blueprint for designing efficient catalysts by the rational combination of central metal core and protein scaffold‐based outer coordination sphere (OCS). Traditionally, a biomimetic catalyst is crafted by including natural amino acids as OCS features around a synthetic metal motif to functionally imitate the metalloenzyme activity. Here, we have pursued an unconventional approach and implanted two distinct drug molecules (isoniazid and nicotine hydrazide) at the axial position of a cobalt core to create a new genre of synthetic catalysts. The resultant cobalt complexes are active for both electrocatalytic and photocatalytic H2 production in near‐neutral water, where they significantly enhance the catalytic performance of the unfunctionalized parent cobalt complex. The drug molecules showcased a dual effect as they influence the catalytic HER by improving the surrounding proton relay along and exerting subtle electronic effects. The isoniazid‐ligated catalyst C1 outperformed the nicotine hydrazide‐bound complex C2, as it produced H2 from water (pH 6.0) at a rate of 3960 s−1 while exhibiting Faradaic efficiency of about 90 %. This strategy opens up newer avenues of bio‐inspired catalyst design beyond amino acid‐based OCS features.
Subject
General Chemistry,Catalysis,Organic Chemistry
Cited by
6 articles.
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