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Photocatalytic Aqueous Reforming of Methyl Formate

DOI zum Zitieren der Version auf EPub Bayreuth: https://doi.org/10.15495/EPub_UBT_00009028
URN to cite this document: urn:nbn:de:bvb:703-epub-9028-1

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Zuo, Dongxu ; Pradhan, Suman ; Banerjee, Manami ; Rockstroh, Nils ; Bartling, Stephan ; Rabee, Abdallah I. M. ; Tian, Xinxin ; Skorynina, Alina ; Jaworski, Aleksander ; Simonelli, Laura ; Rabeah, Jabor ; Jiao, Haijun ; Beller, Matthias ; Das, Shoubhik:
Photocatalytic Aqueous Reforming of Methyl Formate.
In: Advanced Materials. Vol. 37 (2025) Issue 39 . - 2509890.
ISSN 1521-4095
DOI der Verlagsversion: https://doi.org/10.1002/adma.202509890

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Abstract

Green hydrogen is critical to establish a sustainable energy future as it offers a clean, renewable, and a versatile alternative for decarbonizing industries, transportation, and power generation. However, the limitations of current methods significantly restrict the scope and hinder many of the envisioned applications. This study aims to report on the first example of a 3d-metal-based (Cu) heterogeneous photocatalytic system to produce green hydrogen via dehydrogenation of methyl formate (MF), a reaction previously known to require 4d/5d transition metals. Employing a Cu-based atomically dispersed heterogeneous photocatalyst supported on aryl-amino-substituted graphitic carbon nitride (d-gC3N4), the protocol offers numerous key advantages, including the recyclability of the photocatalyst for >10 cycles without significant activity loss, sustained hydrogen production (>15 days!) with high hydrogen yield (19.8 mmol gcat−1) and negligible CO emission, following an operationally simple, sustainable, and efficient catalytic pathway. Furthermore, the photocatalyst is characterized (using HAADF-STEM, SS-NMR, XAS, EPR, and XPS), all of which clearly demonstrated the presence of single atomic Cu-site. Additionally, comprehensive mechanistic investigations together with DFT calculations allow for a thorough mechanistic rationale for this reaction. It is strongly believed that this atomically dispersed heterogeneous photocatalytic approach will open new avenues for establishing liquid organic hydrogen career (LOHC) technologies.

Further data

Item Type: Article in a journal
Keywords: DFT calculations; LOHC; atomically dispersed photocatalyst; green hydrogen; photocatalysis
DDC Subjects: 500 Science > 540 Chemistry
Institutions of the University: Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Chair Organic Chemistry I - Photo- und Elektrokatalyse für Nachhaltigkeit > Chair Organic Chemistry I - Photo- und Elektrokatalyse für Nachhaltigkeit - Univ.-Prof. Dr. Shoubhik Das
Faculties
Faculties > Faculty of Biology, Chemistry and Earth Sciences
Faculties > Faculty of Biology, Chemistry and Earth Sciences > Department of Chemistry > Chair Organic Chemistry I - Photo- und Elektrokatalyse für Nachhaltigkeit
Language: English
Originates at UBT: Yes
URN: urn:nbn:de:bvb:703-epub-9028-1
Date Deposited: 27 Mar 2026 08:41
Last Modified: 27 Mar 2026 08:42
URI: https://epub.uni-bayreuth.de/id/eprint/9028

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