Cited by 177Advanced Photocatalysis TechniquesPerovskite Materials and ApplicationsTiO2 Photocatalysis and Solar Cells

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Integrated halide perovskite photoelectrochemical cells with solar-driven water-splitting efficiency of 20.8%

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Abstract

Achieving high solar-to-hydrogen (STH) efficiency concomitant with long-term durability using low-cost, scalable photo-absorbers is a long-standing challenge. Here we report the design and fabrication of a conductive adhesive-barrier (CAB) that translates >99% of photoelectric power to chemical reactions. The CAB enables halide perovskite-based photoelectrochemical cells with two different architectures that exhibit record STH efficiencies. The first, a co-planar photocathode-photoanode architecture, achieved an STH efficiency of 13.4% and 16.3 h to t 60, solely limited by the hygroscopic hole transport layer in the n-i-p device. The second was formed using a monolithic stacked silicon-perovskite tandem, with a peak STH efficiency of 20.8% and 102 h of continuous operation before t 60 under AM 1.5G illumination. These advances will lead to efficient, durable, and low-cost solar-driven water-splitting technology with multifunctional barriers.

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Crossref · 10.1038/s41467-023-39290-y

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Figures

Fig. 1 Photovoltaic performance and stability of perovskite solar cells. a Current-voltage curve for p-i-n (inverted) architecture PSC. b J-V curve for n-i-p (regular) PSC. c External quantum efficiency and integrated photocurrent of p-i-n (red) and n-i-p (blue) PSCs. d Stability of p-i-n (red) and n-i-p (blue) PVs over time with traditional epoxy encapsulation.
Fig. 1 Photovoltaic performance and stability of perovskite solar cells. a Current-voltage curve for p-i-n (inverted) architecture PSC. b J-V curve for n-i-p (regular) PSC. c External quantum efficiency and integrated photocurrent of p-i-n (red) and n-i-p (blue) PSCs. d Stability of p-i-n (red) and n-i-p (blue) PVs over time with traditional epoxy encapsulation.CC BY · PubMed Central
Fig. 2 CAB (conductive adhesive-barrier) design for near-perfect preservation of photovoltaic efficiency. a Schematic design of a p-i-n perovskite solar cell transformed into a photocathode, with the circled region highlighted to depict the CAB|catalyst layers. The CAB|catalyst is attached to the top electrode of the PSC. b SEM image of CAB with graphite and C-based PSA. c Solar cell J-V measurements for devices with various methods of encapsulation, including glass-epoxy (control) and various commercial conductive adhesive inks capped with graphite. Lighter lines and smaller markers denote reverse sweeps. d Stability measurements of representative devices encapsulated with epoxy-glass (control), commercial C paste, and graphite barrier, and conducting C-filled PSA with graphite barrier (CAB). e Photocathode and f photoanode J-V measurements with electrocatalyst versus corresponding dark electrocatalyst-only in 0.5 M H2SO4 at 10 mV/s.
Fig. 2 CAB (conductive adhesive-barrier) design for near-perfect preservation of photovoltaic efficiency. a Schematic design of a p-i-n perovskite solar cell transformed into a photocathode, with the circled region highlighted to depict the CAB|catalyst layers. The CAB|catalyst is attached to the top electrode of the PSC. b SEM image of CAB with graphite and C-based PSA. c Solar cell J-V measurements for devices with various methods of encapsulation, including glass-epoxy (control) and various commercial conductive adhesive inks capped with graphite. Lighter lines and smaller markers denote reverse sweeps. d Stability measurements of representative devices encapsulated with epoxy-glass (control), commercial C paste, and graphite barrier, and conducting C-filled PSA with graphite barrier (CAB). e Photocathode and f photoanode J-V measurements with electrocatalyst versus corresponding dark electrocatalyst-only in 0.5 M H2SO4 at 10 mV/s.CC BY · PubMed Central
Fig. 3 Series photocathode-photoanode unassisted water-splitting performance. a Schematic representation of the unassisted PEC water-splitting system using halide perovskite PECs. b Co-plotted photocathode and photoanode polarization curves from most efficient devices showing a maximum theoretical operating current density of 22.7 mA/cm2. c 2-electrode unassisted water-splitting stability test showing degradation after 5 h. d Electrocatalyst-only electrolyzer stability at 20 mA/cm2. e Distribution of STH efficiency across five devices, with an average STH of 12.4 ± 0.7%.
Fig. 3 Series photocathode-photoanode unassisted water-splitting performance. a Schematic representation of the unassisted PEC water-splitting system using halide perovskite PECs. b Co-plotted photocathode and photoanode polarization curves from most efficient devices showing a maximum theoretical operating current density of 22.7 mA/cm2. c 2-electrode unassisted water-splitting stability test showing degradation after 5 h. d Electrocatalyst-only electrolyzer stability at 20 mA/cm2. e Distribution of STH efficiency across five devices, with an average STH of 12.4 ± 0.7%.CC BY · PubMed Central
Fig. 4 Tandem silicon-perovskite photoanode unassisted water-splitting performance. a Schematic representation of the unassisted PEC water-splitting system using HaP/Si tandem. b Optical images of absorber (top) and catalytic (bottom) faces of transformed silicon-perovskite photoanode. c HaP/Si tandem photovoltaic J-V curve. Scale bars are 1 cm. d 2-electrode J-V curve of photoanode from champion device showing a theoretical operating current density of 16.9 mA/cm2. e 2-electrode unassisted water-splitting over time. f IrOx nanoparticulate and Pt foil electrocatalyst 2-electrode time-dependent voltage at 15 mA/cm2. g Comparison among other integrated PEC-type devices with respect to STH and lifetime at t60. Demonstrations not reaching t60 are shown with full reported lifetime.
Fig. 4 Tandem silicon-perovskite photoanode unassisted water-splitting performance. a Schematic representation of the unassisted PEC water-splitting system using HaP/Si tandem. b Optical images of absorber (top) and catalytic (bottom) faces of transformed silicon-perovskite photoanode. c HaP/Si tandem photovoltaic J-V curve. Scale bars are 1 cm. d 2-electrode J-V curve of photoanode from champion device showing a theoretical operating current density of 16.9 mA/cm2. e 2-electrode unassisted water-splitting over time. f IrOx nanoparticulate and Pt foil electrocatalyst 2-electrode time-dependent voltage at 15 mA/cm2. g Comparison among other integrated PEC-type devices with respect to STH and lifetime at t60. Demonstrations not reaching t60 are shown with full reported lifetime.CC BY · PubMed Central

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Research works printed but not linked: 1

  1. US Department of Energy. Advanced Water Splitting Materials Workshop Report. 56 (2016).

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Metadata

Authors
Fehr, A. M. K., Agrawal, A., Mandani, F., Conrad, C. L., Jiang, Q., Park, S. Y., Alley, O., Li, B., Sidhik, S., Metcalf, I., Botello, C., Young, J. L., Even, J., Blancon, J. C., Deutsch, T. G., Zhu, K., Albrecht, S., Toma, F. M., Wong, M., & Mohite, A. D.
Affiliations
  • Rice University (US)
  • National Laboratory of the Rockies (US)
  • Lawrence Berkeley National Laboratory (US)
  • Helmholtz-Zentrum Berlin für Materialien und Energie (DE)
  • Centre National de la Recherche Scientifique (FR)
Corresponding author
  • Wong, Michael
  • Mohite, Aditya D.
Venue
Nature Communications
Published
2023-06-26
Volume
14
Issue
1
Pages
3797-3797
ISSN
2041-1723 (ISSN-L)
OpenAlex
W4382020723
Cited by
177
References
47
Citations by year
2026: 54 · 2025: 59 · 2024: 54 · 2023: 10
FWCI
8.46
Type
journal article
Language
en
Open access
Locations
  • Nature Communications (publishedVersion, cc-by)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • HAL (submittedVersion, cc-by)
  • eScholarship (California Digital Library) (submittedVersion, cc-by)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
  • HZB Repository (Helmholtz-Zentrum Berlin für Materialien und Energie GmbH (HZB)) (submittedVersion, other-oa)
  • OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
Funders
DOE | Office of Energy Efficiency and Renewable Energy (DE-EE0008843)
Topics
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Advanced Photocatalysis Techniques
  • Physical Sciences › Engineering › Electrical and Electronic Engineering › Perovskite Materials and Applications
  • Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › TiO2 Photocatalysis and Solar Cells
Keywords
solar water splitting, solar-to-hydrogen efficiency, device durability

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