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Synergistic tailoring of band structure and charge carrier extraction in "€œgreen"€ core/shell quantum dots for highly efficient solar energy conversion
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, P. R. China.
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, P. R. China; Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313001, P. R. China.
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, P. R. China.
Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, P. R. China.
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2022 (English)In: Chemical Engineering Journal, ISSN 1385-8947, E-ISSN 1873-3212, Vol. 442, no 2, article id 136214Article in journal (Refereed) Published
Abstract [en]

Environment-friendly colloidal core/shell quantum dots (QDs) with controllable optoelectronic characteristics are promising building blocks for future commercial solar technologies. Herein, we synergistically tailor the electronic band structure and charge carrier extraction of eco-friendly AgInS2 (AIS)/ZnS core/shell QDs via Mn-alloying and Cu-doping in the core and shell, respectively. It is demonstrated that the Mn-alloying in AIS core can broaden the band gap to facilitate delocalization of photogenerated electrons into the shell and further incorporation of Cu in the ZnS shell enables the creation of Cu-related states that capture the photogenerated holes from core, thus leading to charge carrier recombination and accelerated transfer of photogenerated electrons in the core/shell QDs. As-prepared Mn-AIS/ZnS@Cu QDs were assembled as light harvesters in a photoelectrochemical (PEC) device for light-driven hydrogen evolution, delivering a maximum photocurrent density of ∼6.4 mA cm-2 with superior device stability under standard one sun irradiation (AM 1.5G, 100 mW cm-2). Our findings highlight that simultaneously engineering the band alignment and charge carrier dynamics of “green” core/shell QDs endow the feasibility to design future high-efficiency and durable solar hydrogen production systems.

Place, publisher, year, edition, pages
Elsevier, 2022. Vol. 442, no 2, article id 136214
Keywords [en]
Colloidal quantum dots, Environment-friendly, Core/shell system, Synergistic optoelectronic engineering, Solar hydrogen evolution
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Other Physics Topics
Research subject
Experimental Physics
Identifiers
URN: urn:nbn:se:ltu:diva-90119DOI: 10.1016/j.cej.2022.136214ISI: 000799812700004Scopus ID: 2-s2.0-85127750575OAI: oai:DiVA.org:ltu-90119DiVA, id: diva2:1650606
Funder
The Kempe FoundationsKnut and Alice Wallenberg Foundation
Note

Validerad;2022;Nivå 2;2022-04-13 (joosat);

Funder: National Key Research and Development Programof China (2019YFE0121600); National Natural Science Foundation of China (22105031, 62011530131); Sichuan Science and Technology Program (2021YFH0054); Innovation Group Project of Sichuan Province (20CXTD0090); “111 Project” (B20030)

Available from: 2022-04-07 Created: 2022-04-07 Last updated: 2022-06-10Bibliographically approved

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Vomiero, Alberto

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