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Title: Acid-Compatible Halide Perovskite Photocathodes Utilizing Atomic Layer Deposited TiO 2 for Solar-Driven Hydrogen Evolution

Abstract

Although solution-processable halide perovskite semiconductors exhibit optoelectronic performance comparable to the best photoabsorbers for solar fuel production, halide perovskites rapidly decompose in the presence of water or even humid air. We show that a hybrid electron transport layer, a PC 61BM + TiO 2 film (18-40 nm thickness) grown over the sensitive absorber by atomic layer deposition, enables photoassisted proton reduction without further encapsulation. These semitransparent photocathodes, when paired with a Pt catalyst, display continuous reduction of H + to H 2 for hours under illumination, even while in direct contact with a strongly acidic aqueous electrolyte (0.5 M H 2SO 4). Under 0.5 Sun illumination, a photocurrent density of >10 mA cm -2 is observed, and a photovoltage of 0.68 V assists proton reduction, consistent with a structurally related photovoltaic (PV) device. Submersible halide perovskite photoelectrodes point the way to more efficient photoassisted overall water splitting and other solar fuel generation using solution-processed semiconductors with tunable band gaps.

Authors:
 [1];  [1]; ORCiD logo [1]
  1. Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States; Argonne−Northwestern Solar Energy Research (ANSER) Center, Evanston, Illinois 60208, United States
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division
OSTI Identifier:
1489420
Alternate Identifier(s):
OSTI ID: 1493729; OSTI ID: 1508836
Grant/Contract Number:  
AC02-06CH11357; SC0001059
Resource Type:
Journal Article: Published Article
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Kim, In Soo, Pellin, Michael J., and Martinson, Alex B. F. Acid-Compatible Halide Perovskite Photocathodes Utilizing Atomic Layer Deposited TiO2 for Solar-Driven Hydrogen Evolution. United States: N. p., 2019. Web. doi:10.1021/acsenergylett.8b01661.
Kim, In Soo, Pellin, Michael J., & Martinson, Alex B. F. Acid-Compatible Halide Perovskite Photocathodes Utilizing Atomic Layer Deposited TiO2 for Solar-Driven Hydrogen Evolution. United States. doi:10.1021/acsenergylett.8b01661.
Kim, In Soo, Pellin, Michael J., and Martinson, Alex B. F. Thu . "Acid-Compatible Halide Perovskite Photocathodes Utilizing Atomic Layer Deposited TiO2 for Solar-Driven Hydrogen Evolution". United States. doi:10.1021/acsenergylett.8b01661.
@article{osti_1489420,
title = {Acid-Compatible Halide Perovskite Photocathodes Utilizing Atomic Layer Deposited TiO2 for Solar-Driven Hydrogen Evolution},
author = {Kim, In Soo and Pellin, Michael J. and Martinson, Alex B. F.},
abstractNote = {Although solution-processable halide perovskite semiconductors exhibit optoelectronic performance comparable to the best photoabsorbers for solar fuel production, halide perovskites rapidly decompose in the presence of water or even humid air. We show that a hybrid electron transport layer, a PC61BM + TiO2 film (18-40 nm thickness) grown over the sensitive absorber by atomic layer deposition, enables photoassisted proton reduction without further encapsulation. These semitransparent photocathodes, when paired with a Pt catalyst, display continuous reduction of H+ to H2 for hours under illumination, even while in direct contact with a strongly acidic aqueous electrolyte (0.5 M H2SO4). Under 0.5 Sun illumination, a photocurrent density of >10 mA cm-2 is observed, and a photovoltage of 0.68 V assists proton reduction, consistent with a structurally related photovoltaic (PV) device. Submersible halide perovskite photoelectrodes point the way to more efficient photoassisted overall water splitting and other solar fuel generation using solution-processed semiconductors with tunable band gaps.},
doi = {10.1021/acsenergylett.8b01661},
journal = {ACS Energy Letters},
issn = {2380-8195},
number = 1,
volume = 4,
place = {United States},
year = {2019},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1021/acsenergylett.8b01661

Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

Figures / Tables:

Figure 1 Figure 1: Photoassisted proton reduction with halide perovskite photocathodes. (a) Cross-sectional schematic of a photocathode stabilized against corrosion in 0.5 M H2SO4(aq) via a hybrid ETL comprising PC61BM with TiO2 deposited by ALD. Photogenerated electrons are conducted through the TiO2 to the Pt catalysts, where electrons are used to reducemore » protons to hydrogen. (b) Photoelectrochemical behavior of ITO/PEDOT:PSS/halide perovskite/PC61BM/TiO2/Pt photocathode tested under 0.5 Sun. The dark response of a ITO/TiO2/Pt electrode reveals the shift in the proton reduction onset potential for the photoelectrode (0.68 V). (c) Photoelectrochemical behavior of the photocathode in the dark and under continuous and chopped illumination reveals the time scale (ms) and magnitude (>10 mA cm−2) of the photocurrent response.« less

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