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Title: Interface engineering of colloidal CdSe quantum dots thin films as acid-stable photocathodes for solar-driven hydrogen evolution

Abstract

Colloidal semiconductor quantum dots-based (CQD) photocathodes for solar-driven hydrogen evolution have attracted significant attention due to their tunable size, nanostructured morphology, crystalline orientation, and band-gap. Here, we report a thin film heterojunction photocathode composed of organic PEDOT:PSS as a hole transport layer, CdSe CQDs as a semiconductor light absorber, and conformal Pt layer deposited by atomic layer deposition (ALD) serving as both a passivation layer and cocatalyst for hydrogen evolution. In neutral aqueous solution, a PEDOT:PSS/CdSe/Pt heterogeneous photocathode with 200 cycles of ALD Pt produces a photocurrent density of -1.08 mA/cm2 (AM1.5G, 100 mW/cm2) at a potential of 0 V vs. RHE (j0) in neutral aqueous solution, which is nearly 12 times that of the pristine CdSe photocathode. This composite photocathode shows an onset potential for water reduction at +0.46 V vs. RHE and long-term stability with negligible degradation. In acidic electrolyte (pH = 1), where the hydrogen evolution reaction is more favorable but stability is limited due to photocorrosion, a thicker Pt film (300 cycles) is shown to greatly improve the device stability and a j0 of -2.14 mA/cm2 is obtained with only 8.3% activity degradation after 6 h, compared to 80% degradation under the same conditions when themore » less conformal electrodeposition method is used to deposit the Pt layer. Electrochemical impedance spectroscopy and time-resolved photoluminescence results indicate that these enhancements stem from a lower bulk charge recombination rate, higher interfacial charge transfer rate, and faster reaction kinetics. In conclusion, we believe that these interface engineering strategies can be extended to other colloidal semiconductors to construct more efficient and stable heterogeneous photoelectrodes for solar fuel production.« less

Authors:
 [1];  [2];  [1];  [1]; ORCiD logo [3];  [4];  [1];  [1];  [5];  [1];  [1];  [2];  [1]
+ Show Author Affiliations
  1. Wake Forest Univ., Winston-Salem, NC (United States)
  2. Harbin Institute of Technology, Shenzhen (China)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. IBM TJ Watson Research Center, Yorktown Heights, NY (United States)
  5. Soochow Univ., Jiangsu (China)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1436031
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 20; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; interface engineering; colloidal quantum dots; atomic layer deposition; photocathode; hydrogen evolution

Citation Formats

Li, Hui, Wen, Peng, Hoxie, Adam, Dun, Chaochao, Adhikari, Shiba P., Li, Qi, Lu, Chang, Itanze, Dominique, Jiang, Lin, Carroll, David L., Lachgar, Abdou, Qiu, Yejun, and Geyer, Scott. Interface engineering of colloidal CdSe quantum dots thin films as acid-stable photocathodes for solar-driven hydrogen evolution. United States: N. p., 2018. Web. doi:10.1021/acsami.7b19229.
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Li, Hui, Wen, Peng, Hoxie, Adam, Dun, Chaochao, Adhikari, Shiba P., Li, Qi, Lu, Chang, Itanze, Dominique, Jiang, Lin, Carroll, David L., Lachgar, Abdou, Qiu, Yejun, & Geyer, Scott. Interface engineering of colloidal CdSe quantum dots thin films as acid-stable photocathodes for solar-driven hydrogen evolution. United States. https://doi.org/10.1021/acsami.7b19229
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Li, Hui, Wen, Peng, Hoxie, Adam, Dun, Chaochao, Adhikari, Shiba P., Li, Qi, Lu, Chang, Itanze, Dominique, Jiang, Lin, Carroll, David L., Lachgar, Abdou, Qiu, Yejun, and Geyer, Scott. Mon . "Interface engineering of colloidal CdSe quantum dots thin films as acid-stable photocathodes for solar-driven hydrogen evolution". United States. https://doi.org/10.1021/acsami.7b19229. https://www.osti.gov/servlets/purl/1436031.
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@article{osti_1436031,
title = {Interface engineering of colloidal CdSe quantum dots thin films as acid-stable photocathodes for solar-driven hydrogen evolution},
author = {Li, Hui and Wen, Peng and Hoxie, Adam and Dun, Chaochao and Adhikari, Shiba P. and Li, Qi and Lu, Chang and Itanze, Dominique and Jiang, Lin and Carroll, David L. and Lachgar, Abdou and Qiu, Yejun and Geyer, Scott},
abstractNote = {Colloidal semiconductor quantum dots-based (CQD) photocathodes for solar-driven hydrogen evolution have attracted significant attention due to their tunable size, nanostructured morphology, crystalline orientation, and band-gap. Here, we report a thin film heterojunction photocathode composed of organic PEDOT:PSS as a hole transport layer, CdSe CQDs as a semiconductor light absorber, and conformal Pt layer deposited by atomic layer deposition (ALD) serving as both a passivation layer and cocatalyst for hydrogen evolution. In neutral aqueous solution, a PEDOT:PSS/CdSe/Pt heterogeneous photocathode with 200 cycles of ALD Pt produces a photocurrent density of -1.08 mA/cm2 (AM1.5G, 100 mW/cm2) at a potential of 0 V vs. RHE (j0) in neutral aqueous solution, which is nearly 12 times that of the pristine CdSe photocathode. This composite photocathode shows an onset potential for water reduction at +0.46 V vs. RHE and long-term stability with negligible degradation. In acidic electrolyte (pH = 1), where the hydrogen evolution reaction is more favorable but stability is limited due to photocorrosion, a thicker Pt film (300 cycles) is shown to greatly improve the device stability and a j0 of -2.14 mA/cm2 is obtained with only 8.3% activity degradation after 6 h, compared to 80% degradation under the same conditions when the less conformal electrodeposition method is used to deposit the Pt layer. Electrochemical impedance spectroscopy and time-resolved photoluminescence results indicate that these enhancements stem from a lower bulk charge recombination rate, higher interfacial charge transfer rate, and faster reaction kinetics. In conclusion, we believe that these interface engineering strategies can be extended to other colloidal semiconductors to construct more efficient and stable heterogeneous photoelectrodes for solar fuel production.},
doi = {10.1021/acsami.7b19229},
journal = {ACS Applied Materials and Interfaces},
number = 20,
volume = 10,
place = {United States},
year = {2018},
month = {4}
}
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https://doi.org/10.1021/acsami.7b19229
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