Utilizing a Siloxane-Modified Organic Semiconductor for Photoelectrochemical Water Splitting

Hyo Jin Ahn; Ki Yong Yoon; Mingi Sung; Hyeonjin Yoo; Hyungju Ahn; Byoung Hoon Lee; Junghoon Lee; Ji Hyun Jang

doi:10.1021/acsenergylett.3c00755

Utilizing a Siloxane-Modified Organic Semiconductor for Photoelectrochemical Water Splitting

Hyo Jin Ahn, Ki Yong Yoon, Mingi Sung, Hyeonjin Yoo, Hyungju Ahn, Byoung Hoon Lee, Junghoon Lee, Ji Hyun Jang

Department of Chemical Engineering & Materials Science

Research output: Contribution to journal › Article › peer-review

24 Scopus citations

Abstract

We explore the potential of employing diketopyrrolopyrrole (DPP) based π-conjugated OSs as a hole transport layer material in heteroatom-doped hematite (Ti-Fe₂O₃/Ge-Fe₂O₃) photoanodes for efficient photoelectrochemical water splitting. The siloxane-modified π-conjugated polymer (P_Si) with a high carrier mobility and crystallinity revealed great potential to extract holes by forming a built-in potential with hematite photoanodes while showing high stability in an alkaline electrolyte for photoelectrochemical water oxidation. Because of the easy hole extraction and subsequent fast hole transport property of the P_Si interlayer between NiFe(OH)_x and Ge-doped porous Fe₂O₃(Ge-PH), NiFe(OH)_x/P_Si/Ge-PH showed a 1.8-fold increase in photocurrent density (4.57 mA cm^-2 at 1.23 V_RHE) with a cathodic shift of the onset potential (0.735 V_RHE) and good stability for 65 h compared to Ge-PH. This study demonstrates the successful use of inherently unstable π-conjugated OSs as a hole extracting/transport medium in a photoanode, addressing the intrinsic recombination issues of hematite for efficient and stable water splitting.

Original language	English
Pages (from-to)	2595-2602
Number of pages	8
Journal	ACS Energy Letters
Volume	8
Issue number	6
DOIs	https://doi.org/10.1021/acsenergylett.3c00755
State	Published - 9 Jun 2023

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© 2023 American Chemical Society.

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title = "Utilizing a Siloxane-Modified Organic Semiconductor for Photoelectrochemical Water Splitting",

abstract = "We explore the potential of employing diketopyrrolopyrrole (DPP) based π-conjugated OSs as a hole transport layer material in heteroatom-doped hematite (Ti-Fe2O3/Ge-Fe2O3) photoanodes for efficient photoelectrochemical water splitting. The siloxane-modified π-conjugated polymer (PSi) with a high carrier mobility and crystallinity revealed great potential to extract holes by forming a built-in potential with hematite photoanodes while showing high stability in an alkaline electrolyte for photoelectrochemical water oxidation. Because of the easy hole extraction and subsequent fast hole transport property of the PSi interlayer between NiFe(OH)x and Ge-doped porous Fe2O3(Ge-PH), NiFe(OH)x/PSi/Ge-PH showed a 1.8-fold increase in photocurrent density (4.57 mA cm-2 at 1.23 VRHE) with a cathodic shift of the onset potential (0.735 VRHE) and good stability for 65 h compared to Ge-PH. This study demonstrates the successful use of inherently unstable π-conjugated OSs as a hole extracting/transport medium in a photoanode, addressing the intrinsic recombination issues of hematite for efficient and stable water splitting.",

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AU - Ahn, Hyungju

AU - Lee, Byoung Hoon

AU - Lee, Junghoon

AU - Jang, Ji Hyun

PY - 2023/6/9

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N2 - We explore the potential of employing diketopyrrolopyrrole (DPP) based π-conjugated OSs as a hole transport layer material in heteroatom-doped hematite (Ti-Fe2O3/Ge-Fe2O3) photoanodes for efficient photoelectrochemical water splitting. The siloxane-modified π-conjugated polymer (PSi) with a high carrier mobility and crystallinity revealed great potential to extract holes by forming a built-in potential with hematite photoanodes while showing high stability in an alkaline electrolyte for photoelectrochemical water oxidation. Because of the easy hole extraction and subsequent fast hole transport property of the PSi interlayer between NiFe(OH)x and Ge-doped porous Fe2O3(Ge-PH), NiFe(OH)x/PSi/Ge-PH showed a 1.8-fold increase in photocurrent density (4.57 mA cm-2 at 1.23 VRHE) with a cathodic shift of the onset potential (0.735 VRHE) and good stability for 65 h compared to Ge-PH. This study demonstrates the successful use of inherently unstable π-conjugated OSs as a hole extracting/transport medium in a photoanode, addressing the intrinsic recombination issues of hematite for efficient and stable water splitting.

AB - We explore the potential of employing diketopyrrolopyrrole (DPP) based π-conjugated OSs as a hole transport layer material in heteroatom-doped hematite (Ti-Fe2O3/Ge-Fe2O3) photoanodes for efficient photoelectrochemical water splitting. The siloxane-modified π-conjugated polymer (PSi) with a high carrier mobility and crystallinity revealed great potential to extract holes by forming a built-in potential with hematite photoanodes while showing high stability in an alkaline electrolyte for photoelectrochemical water oxidation. Because of the easy hole extraction and subsequent fast hole transport property of the PSi interlayer between NiFe(OH)x and Ge-doped porous Fe2O3(Ge-PH), NiFe(OH)x/PSi/Ge-PH showed a 1.8-fold increase in photocurrent density (4.57 mA cm-2 at 1.23 VRHE) with a cathodic shift of the onset potential (0.735 VRHE) and good stability for 65 h compared to Ge-PH. This study demonstrates the successful use of inherently unstable π-conjugated OSs as a hole extracting/transport medium in a photoanode, addressing the intrinsic recombination issues of hematite for efficient and stable water splitting.

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Utilizing a Siloxane-Modified Organic Semiconductor for Photoelectrochemical Water Splitting

Abstract

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