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

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

doi:10.1021/acsami.7b19229

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

Journal Article · 30 April 2018 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.7b19229 · OSTI ID:1436031

Li, Hui ^[1]; Wen, Peng ^[2]; Hoxie, Adam ^[1]; Dun, Chaochao ^[1];

^[3]; Li, Qi ^[4]; Lu, Chang ^[1]; Itanze, Dominique ^[1]; Jiang, Lin ^[5]; Carroll, David L. ^[1]; Lachgar, Abdou ^[1]; Qiu, Yejun ^[2]; Geyer, Scott ^[1]

Wake Forest Univ., Winston-Salem, NC (United States)
Harbin Institute of Technology, Shenzhen (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
IBM TJ Watson Research Center, Yorktown Heights, NY (United States)
Soochow Univ., Jiangsu (China)

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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1436031

Journal Information:: ACS Applied Materials and Interfaces, Vol. 10, Issue 20; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 10 works

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42 ENGINEERING
interface engineering
colloidal quantum dots
atomic layer deposition
photocathode
hydrogen evolution

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

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