journal article·2026-05-22Open access

Fully Textured Monolithic Sb 2 S 3 /Silicon Tandem for Unbiased and Stable Solar‐Driven Water Splitting Paired with Iodide Oxidation Reaction

Jihong Min, Irene Dei Tos, Sepideh Rahimisheikh, Beatriz de la Fuente, Devika Rajagopal, Jan D'Haen, David Cornil, Tom Hauffman, Tom Aernouts, David Beljonne, Joke Hadermann, Byungha Shin, Bart Vermang, Sudhanshu Shukla

Abstract

ABSTRACT Solar‐driven photoelectrochemical (PEC) production of chemical fuels such as hydrogen is a viable solution to address climate neutrality objectives. Development of a monolithic tandem PEC device consisting of ideal bandgap absorbers is of paramount importance to realize efficient artificial photosynthesis systems. Herein, we report monolithic integration of Sb 2 S 3 on textured silicon to realize a completely inorganic and fully vacuum processed multilayer PEC device with Ag/Indium Tin Oxide (ITO)/Heterojunction with Intrinsic Thin layer (HIT) Si/ITO/Au/Sb 2 S 3 /NiO x architecture. Photoelectron spectroscopy and computational analysis show a staggered band alignment between Si and Sb 2 S 3 , emulating Z‐scheme charge transfer mechanism. We demonstrate a high performing and stable Sb 2 S 3 ‐Si monolithic tandem for PEC hydrogen evolution reaction (HER) coupled to iodide oxidation reaction (IOR). Under AM 1.5G illumination, the Sb 2 S 3 ‐Si monolithic tandem device achieves unassisted photocurrent density of 4.38 mA cm − 2 with faradaic efficiency of 97% for hydrogen, while maintaining ∼90% of its initial performance after 10 h of continuous operation. These results set a new benchmark for all inorganic monolithic tandems for efficient and sustainable solar‐to‐chemical conversion. This work unlocks the pathway for artificial photosynthesis systems comprising ideal bandgap photo absorbers.
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Research context

OpenAlex topics: Advanced Photocatalysis Techniques · Chalcogenide Semiconductor Thin Films · TiO2 Photocatalysis and Solar Cells

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Materials Science and Engineering Korea Advanced Institute of Science and Technology Daejeon Republic of Korea

imec IUMAT Genk Belgium

UHasselt Institute for Materials Research (IUMAT) Hasselt Belgium

EnergyVille Genk Belgium

Electron Microscopy for Materials Science (EMAT) University of Antwerp Antwerpen Belgium

Research Group Sustainable Materials Engineering (SUME) Lab of Electrochemical and Surface Engineering (SURF) Vrije Universiteit Brussel Brussels Belgium

UHasselt Institute for Materials Research (IUMAT) Analytical & Microscopical Services (AMS) Hasselt Belgium

imec IUMAT Diepenbeek Belgium

Laboratory for Chemistry of Novel Materials University of Mons (UMONS) Mons Belgium

Funding

Ministry of Strategy and Finance · Fonds De La Recherche Scientifique - FNRS

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