Unveiling Formation Pathways of Ternary I–III–VI CuInS2 Quantum Dots and Their Effect on Photoelectrochemical Hydrogen Generation

Abstract Understanding the formation mechanisms of semiconductor nanocrystal quantum dots (QDs) is essential for fine‐tuning their optical and electrical properties. Despite their potential in solar energy conversion, the synthesis processes and resulting properties of ternary I–III–VI QDs remain un...

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Main Authors: Hyo Cheol Lee, Hwapyong Kim, Kiwook Kim, Kyunghoon Lee, Wookjin Chung, Seung Beom Ha, Minseo Kim, Eonhyoung Ahn, Shi Li, Seunghyun Ji, Gyudong Lee, Hyeonjong Ma, Sung Jun Lim, Hongsoo Choi, Jae‐Yup Kim, Hyungju Ahn, Su‐Il In, Jiwoong Yang
Format: Article
Language:English
Published: Wiley 2025-08-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202500829
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author Hyo Cheol Lee
Hwapyong Kim
Kiwook Kim
Kyunghoon Lee
Wookjin Chung
Seung Beom Ha
Minseo Kim
Eonhyoung Ahn
Shi Li
Seunghyun Ji
Gyudong Lee
Hyeonjong Ma
Sung Jun Lim
Hongsoo Choi
Jae‐Yup Kim
Hyungju Ahn
Su‐Il In
Jiwoong Yang
author_facet Hyo Cheol Lee
Hwapyong Kim
Kiwook Kim
Kyunghoon Lee
Wookjin Chung
Seung Beom Ha
Minseo Kim
Eonhyoung Ahn
Shi Li
Seunghyun Ji
Gyudong Lee
Hyeonjong Ma
Sung Jun Lim
Hongsoo Choi
Jae‐Yup Kim
Hyungju Ahn
Su‐Il In
Jiwoong Yang
author_sort Hyo Cheol Lee
collection DOAJ
description Abstract Understanding the formation mechanisms of semiconductor nanocrystal quantum dots (QDs) is essential for fine‐tuning their optical and electrical properties. Despite their potential in solar energy conversion, the synthesis processes and resulting properties of ternary I–III–VI QDs remain underexplored due to the complex interplay among their constituent elements. Herein, the formation mechanism of ternary I–III–VI CuInS2 QDs is investigated, and a direct correlation between their synthesis pathways and photoelectrochemical hydrogen generation performance is established. Two distinct formation pathways governed by the Lewis acid strength of the precursors are revealed. Precursors with weaker Lewis acid strength, such as indium acetate–alkylamine complexes, induce the nucleation of Cu x S phases, which subsequently transform into CuInS2 QDs. Conversely, exemplified by indium iodide–alkylamine complexes, precursors with stronger Lewis acid strength enable the simultaneous incorporation of all elements during nucleation, resulting in the direct formation of CuInS2 QDs. Notably, QDs synthesized through this direct pathway exhibit significantly improved electrical properties with lower electron trap densities, resulting in outstanding photoelectrochemical hydrogen production with an excellent photocurrent density of 11.3 mA cm−2 at 0.6 VRHE when used as sensitizers in photoanodes. These findings highlight the critical role of formation pathways in tailoring the properties of ternary I–III–VI QDs.
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spelling doaj-art-9cfc0085b0a949dbad1f6397c211e2f42025-08-23T14:14:26ZengWileyAdvanced Science2198-38442025-08-011231n/an/a10.1002/advs.202500829Unveiling Formation Pathways of Ternary I–III–VI CuInS2 Quantum Dots and Their Effect on Photoelectrochemical Hydrogen GenerationHyo Cheol Lee0Hwapyong Kim1Kiwook Kim2Kyunghoon Lee3Wookjin Chung4Seung Beom Ha5Minseo Kim6Eonhyoung Ahn7Shi Li8Seunghyun Ji9Gyudong Lee10Hyeonjong Ma11Sung Jun Lim12Hongsoo Choi13Jae‐Yup Kim14Hyungju Ahn15Su‐Il In16Jiwoong Yang17Department of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Chemical Engineering Dankook University Yongin 16890 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDivision of Nanotechnology Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDivision of Nanotechnology Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDGIST‐ETH Microrobotics Research Center Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Chemical Engineering Konkuk University Seoul 05029 Republic of KoreaPohang Accelerator Laboratory Pohang University of Science and Technology (POSTECH) Pohang 37673 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaDepartment of Energy Science and Engineering Daegu Gyeongbuk Institute of Science and Technology (DGIST) Daegu 42988 Republic of KoreaAbstract Understanding the formation mechanisms of semiconductor nanocrystal quantum dots (QDs) is essential for fine‐tuning their optical and electrical properties. Despite their potential in solar energy conversion, the synthesis processes and resulting properties of ternary I–III–VI QDs remain underexplored due to the complex interplay among their constituent elements. Herein, the formation mechanism of ternary I–III–VI CuInS2 QDs is investigated, and a direct correlation between their synthesis pathways and photoelectrochemical hydrogen generation performance is established. Two distinct formation pathways governed by the Lewis acid strength of the precursors are revealed. Precursors with weaker Lewis acid strength, such as indium acetate–alkylamine complexes, induce the nucleation of Cu x S phases, which subsequently transform into CuInS2 QDs. Conversely, exemplified by indium iodide–alkylamine complexes, precursors with stronger Lewis acid strength enable the simultaneous incorporation of all elements during nucleation, resulting in the direct formation of CuInS2 QDs. Notably, QDs synthesized through this direct pathway exhibit significantly improved electrical properties with lower electron trap densities, resulting in outstanding photoelectrochemical hydrogen production with an excellent photocurrent density of 11.3 mA cm−2 at 0.6 VRHE when used as sensitizers in photoanodes. These findings highlight the critical role of formation pathways in tailoring the properties of ternary I–III–VI QDs.https://doi.org/10.1002/advs.202500829I–III–VIformation mechanismhydrogen productionphotoelectrochemical propertiesquantum dots
spellingShingle Hyo Cheol Lee
Hwapyong Kim
Kiwook Kim
Kyunghoon Lee
Wookjin Chung
Seung Beom Ha
Minseo Kim
Eonhyoung Ahn
Shi Li
Seunghyun Ji
Gyudong Lee
Hyeonjong Ma
Sung Jun Lim
Hongsoo Choi
Jae‐Yup Kim
Hyungju Ahn
Su‐Il In
Jiwoong Yang
Unveiling Formation Pathways of Ternary I–III–VI CuInS2 Quantum Dots and Their Effect on Photoelectrochemical Hydrogen Generation
Advanced Science
I–III–VI
formation mechanism
hydrogen production
photoelectrochemical properties
quantum dots
title Unveiling Formation Pathways of Ternary I–III–VI CuInS2 Quantum Dots and Their Effect on Photoelectrochemical Hydrogen Generation
title_full Unveiling Formation Pathways of Ternary I–III–VI CuInS2 Quantum Dots and Their Effect on Photoelectrochemical Hydrogen Generation
title_fullStr Unveiling Formation Pathways of Ternary I–III–VI CuInS2 Quantum Dots and Their Effect on Photoelectrochemical Hydrogen Generation
title_full_unstemmed Unveiling Formation Pathways of Ternary I–III–VI CuInS2 Quantum Dots and Their Effect on Photoelectrochemical Hydrogen Generation
title_short Unveiling Formation Pathways of Ternary I–III–VI CuInS2 Quantum Dots and Their Effect on Photoelectrochemical Hydrogen Generation
title_sort unveiling formation pathways of ternary i iii vi cuins2 quantum dots and their effect on photoelectrochemical hydrogen generation
topic I–III–VI
formation mechanism
hydrogen production
photoelectrochemical properties
quantum dots
url https://doi.org/10.1002/advs.202500829
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