Investigating the role of chain and linker length on the catalytic activity of an H2 production catalyst containing a ?-hairpin peptide

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dc.contributor.author Reback, Matthew L.
dc.contributor.author Ginovska, Bojana
dc.contributor.author Buchko, Garry W.
dc.contributor.author Dutta, Arnab
dc.contributor.author Priyadarshani, Nilusha
dc.contributor.author Kier, Brandon L.
dc.contributor.author Helm, Monte L.
dc.contributor.author Raugei, Simone
dc.contributor.author Shaw, Wendy J.
dc.date.accessioned 2016-06-09T12:59:43Z
dc.date.available 2016-06-09T12:59:43Z
dc.date.issued 2016-07
dc.identifier.citation Reback, Matthew L.; Ginovska, Bojana; Buchko, Garry W.; Dutta, Arnab; Priyadarshani, Nilusha; Kier, Brandon L.; Helm, Monte L.; Raugei, Simone and Shaw, Wendy J., “Investigating the role of chain and linker length on the catalytic activity of an H2 production catalyst containing a β-hairpin peptide”, Journal of Coordination Chemistry, DOI: 10.1080/00958972.2016.1188924, vol. 69, no. 11-13, pp. 1730-1747, Jul. 2016.
dc.identifier.issn 0095-8972
dc.identifier.uri https://repository.iitgn.ac.in/handle/123456789/2313
dc.identifier.uri http://dx.doi.org/10.1080/00958972.2016.1188924
dc.description.abstract Building on our recent report of an active H2 production catalyst [Ni(PPh2NProp–peptide)2]2+ (Prop = para-phenylpropionic acid, peptide (R10) = WIpPRWTGPR-NH2, p = D-proline and P2N = 1-aza-3,6-diphosphacycloheptane) that contains structured β-hairpin peptides, here we investigate how H2 production is effected by: (1) the length of the hairpin (8 or 10 residues) and (2) limiting the flexibility between the peptide and the core complex by altering the length of the linker: para-phenylpropionic acid (three carbons) or para-benzoic acid (one carbon). Reduction of the peptide chain length from 10 to 8 residues increases or maintains the catalytic current for H2 production for all complexes, suggesting a non-productive steric interaction at longer peptide lengths. While the structure of the hairpin appears largely intact for the complexes, NMR data are consistent with differences in dynamic behavior which may contribute to the observed differences in catalytic activity. Molecular dynamics simulations demonstrate that complexes with a one-carbon linker have the desired effect of restricting the motion of the hairpin relative to the complex; however, the catalytic currents are significantly reduced compared to complexes containing a three-carbon linker as a result of the electron withdrawing nature of the –COOH group. These results demonstrate the complexity and interrelated nature of the outer coordination sphere on catalysis. en_US
dc.description.statementofresponsibility by Matthew L. Reback, Bojana Ginovska, Garry W. Buchko, Arnab Dutta, Nilusha Priyadarshani, Brandon L. Kier, Monte L. Helm, Simone Raugei and Wendy J. Shaw
dc.format.extent Vol. 69, no. 11-13, pp. 1730-1747
dc.language.iso en_US en_US
dc.publisher Taylor & Francis en_US
dc.subject Hydrogen production en_US
dc.subject Electrocatalysis en_US
dc.subject Peptide Catalyst en_US
dc.subject Outer Coordination Sphere en_US
dc.subject Renewable Energy en_US
dc.subject Enzyme Mimic en_US
dc.title Investigating the role of chain and linker length on the catalytic activity of an H2 production catalyst containing a ?-hairpin peptide en_US
dc.type Article en_US
dc.relation.journal Journal of Coordination Chemistry


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