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Title: Theoretical limits of multiple exciton generation and singlet fission tandem devices for solar water splitting

Abstract

Photoelectrochemical (PEC) water splitting is one of the most important approaches being investigated for solar fuel generation. In this study, we determine the maximum thermodynamic power conversion efficiencies (PCEs) of PEC water splitting two-bandgap tandem devices that produce multiple carriers per photon absorbed via Multiple Exciton Generation (MEG) or Singlet Fission (SF) and in the presence of solar concentration. Here, we employ a detailed balance thermodynamic analysis to determine the effects of top cell thickness, solar concentration, carrier multiplication, electrode overvoltage (VO), and water absorption on PEC power conversion efficiency for water splitting cells. We have found a maximum PEC power conversion efficiency of 62.9% in cells using two ideal tandem MEG absorbers with bandgaps of 0.3 and 1.2 eV at 1000-suns solar concentration and 0 overvoltage; the maximum PCE for two tandem SF absorbers under the same conditions is nearly the same at 59% with the same values for the absorption thresholds. A very interesting and important result was that, upon thinning the top cell, the range of viable bandgaps for both the top and bottom cells is extended by as much as 0.5-1 eV while still maintaining high maximum conversion efficiency (60-63%). The effects of imposing different solarmore » concentrations from 1X to 1000X and having different tandem configurations of SF and MEG layers were also studied.« less

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States); 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:
1569450
Report Number(s):
NREL/JA-5900-73808
Journal ID: ISSN 0021-9606; TRN: US2001249
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 151; Journal Issue: 11; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; multiple exciton generation; solar water splitting; quantum dots; singlet fission

Citation Formats

Martinez, Marissa, Nozik, Arthur J., and Beard, Matthew C. Theoretical limits of multiple exciton generation and singlet fission tandem devices for solar water splitting. United States: N. p., 2019. Web. doi:10.1063/1.5102095.
Martinez, Marissa, Nozik, Arthur J., & Beard, Matthew C. Theoretical limits of multiple exciton generation and singlet fission tandem devices for solar water splitting. United States. doi:10.1063/1.5102095.
Martinez, Marissa, Nozik, Arthur J., and Beard, Matthew C. Thu . "Theoretical limits of multiple exciton generation and singlet fission tandem devices for solar water splitting". United States. doi:10.1063/1.5102095. https://www.osti.gov/servlets/purl/1569450.
@article{osti_1569450,
title = {Theoretical limits of multiple exciton generation and singlet fission tandem devices for solar water splitting},
author = {Martinez, Marissa and Nozik, Arthur J. and Beard, Matthew C.},
abstractNote = {Photoelectrochemical (PEC) water splitting is one of the most important approaches being investigated for solar fuel generation. In this study, we determine the maximum thermodynamic power conversion efficiencies (PCEs) of PEC water splitting two-bandgap tandem devices that produce multiple carriers per photon absorbed via Multiple Exciton Generation (MEG) or Singlet Fission (SF) and in the presence of solar concentration. Here, we employ a detailed balance thermodynamic analysis to determine the effects of top cell thickness, solar concentration, carrier multiplication, electrode overvoltage (VO), and water absorption on PEC power conversion efficiency for water splitting cells. We have found a maximum PEC power conversion efficiency of 62.9% in cells using two ideal tandem MEG absorbers with bandgaps of 0.3 and 1.2 eV at 1000-suns solar concentration and 0 overvoltage; the maximum PCE for two tandem SF absorbers under the same conditions is nearly the same at 59% with the same values for the absorption thresholds. A very interesting and important result was that, upon thinning the top cell, the range of viable bandgaps for both the top and bottom cells is extended by as much as 0.5-1 eV while still maintaining high maximum conversion efficiency (60-63%). The effects of imposing different solar concentrations from 1X to 1000X and having different tandem configurations of SF and MEG layers were also studied.},
doi = {10.1063/1.5102095},
journal = {Journal of Chemical Physics},
number = 11,
volume = 151,
place = {United States},
year = {2019},
month = {9}
}

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