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Title: Role of Surface-Capping Ligands in Photoexcited Electron Transfer between CdS Nanorods and [FeFe] Hydrogenase and the Subsequent H 2 Generation

Abstract

Complexes of CdS nanorods and [FeFe] hydrogenase from Clostridium acetobutylicum have been shown to photochemically produce H2. This study examines the role of the ligands that passivate the nanocrystal surfaces in the electron transfer from photoexcited CdS to hydrogenase and the H2 generation that follows. We functionalized CdS nanorods with a series of mercaptocarboxylate surface-capping ligands of varying lengths and measured their photoexcited electron relaxation by transient absorption (TA) spectroscopy before and after hydrogenase adsorption. Rate constants for electron transfer from the nanocrystals to the enzyme, extracted by modeling of TA kinetics, decrease exponentially with ligand length, suggesting that the ligand layer acts as a barrier to charge transfer and controls the degree of electronic coupling. Relative light-driven H2 production efficiencies follow the relative quantum efficiencies of electron transfer, revealing the critical role of surface-capping ligands in determining the photochemical activity of these nanocrystal-enzyme complexes. Our results suggest that the H2 production in this system could be maximized with a choice of a surface-capping ligand that decreases the distance between the nanocrystal surface and the electron injection site of the enzyme.

Authors:
 [1]; ORCiD logo [1];  [1];  [2];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of Colorado, Boulder, CO (United States)
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1413443
Report Number(s):
NREL/JA-2700-68946
Journal ID: ISSN 1932-7447; TRN: US1800427
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 1; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
08 HYDROGEN; 09 BIOMASS FUELS; ligands; nanocrystals; hydrogenase

Citation Formats

Wilker, Molly B., Utterback, James K., Greene, Sophie, Brown, Katherine A., Mulder, David W., King, Paul W., and Dukovic, Gordana. Role of Surface-Capping Ligands in Photoexcited Electron Transfer between CdS Nanorods and [FeFe] Hydrogenase and the Subsequent H 2 Generation. United States: N. p., 2017. Web. https://doi.org/10.1021/acs.jpcc.7b07229.
Wilker, Molly B., Utterback, James K., Greene, Sophie, Brown, Katherine A., Mulder, David W., King, Paul W., & Dukovic, Gordana. Role of Surface-Capping Ligands in Photoexcited Electron Transfer between CdS Nanorods and [FeFe] Hydrogenase and the Subsequent H 2 Generation. United States. https://doi.org/10.1021/acs.jpcc.7b07229
Wilker, Molly B., Utterback, James K., Greene, Sophie, Brown, Katherine A., Mulder, David W., King, Paul W., and Dukovic, Gordana. Fri . "Role of Surface-Capping Ligands in Photoexcited Electron Transfer between CdS Nanorods and [FeFe] Hydrogenase and the Subsequent H 2 Generation". United States. https://doi.org/10.1021/acs.jpcc.7b07229. https://www.osti.gov/servlets/purl/1413443.
@article{osti_1413443,
title = {Role of Surface-Capping Ligands in Photoexcited Electron Transfer between CdS Nanorods and [FeFe] Hydrogenase and the Subsequent H 2 Generation},
author = {Wilker, Molly B. and Utterback, James K. and Greene, Sophie and Brown, Katherine A. and Mulder, David W. and King, Paul W. and Dukovic, Gordana},
abstractNote = {Complexes of CdS nanorods and [FeFe] hydrogenase from Clostridium acetobutylicum have been shown to photochemically produce H2. This study examines the role of the ligands that passivate the nanocrystal surfaces in the electron transfer from photoexcited CdS to hydrogenase and the H2 generation that follows. We functionalized CdS nanorods with a series of mercaptocarboxylate surface-capping ligands of varying lengths and measured their photoexcited electron relaxation by transient absorption (TA) spectroscopy before and after hydrogenase adsorption. Rate constants for electron transfer from the nanocrystals to the enzyme, extracted by modeling of TA kinetics, decrease exponentially with ligand length, suggesting that the ligand layer acts as a barrier to charge transfer and controls the degree of electronic coupling. Relative light-driven H2 production efficiencies follow the relative quantum efficiencies of electron transfer, revealing the critical role of surface-capping ligands in determining the photochemical activity of these nanocrystal-enzyme complexes. Our results suggest that the H2 production in this system could be maximized with a choice of a surface-capping ligand that decreases the distance between the nanocrystal surface and the electron injection site of the enzyme.},
doi = {10.1021/acs.jpcc.7b07229},
journal = {Journal of Physical Chemistry. C},
number = 1,
volume = 122,
place = {United States},
year = {2017},
month = {12}
}

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