CdSe quantum dots (QDs) combined with [FeFe] hydrogenase mimics as molecular catalytic reaction centers based on earth-abundant elements have demonstrated promising activity for photocatalytic hydrogen generation. Direct linking of the [FeFe] hydrogenase mimics to the QD surface is expected to establish a close contact between the [FeFe] hydrogenase mimics and the light-harvesting QDs, supporting the transfer and accumulation of several electrons needed to drive hydrogen evolution. In this work, we report on the functionalization of QDs immobilized in a thin-film architecture on a substrate with [FeFe] hydrogenase mimics by covalent linking via carboxylate groups as the anchoring functionality. The functionalization was monitored via UV/vis, photoluminescence, IR, and X-ray photoelectron spectroscopy and quantified via micro-X-ray fluorescence spectrometry. The activity of the functionalized thin film was demonstrated, and turn-over numbers in the range of 360-580 (short linkers) and 130-160 (long linkers) were achieved. This work presents a proof-of-concept study, showing the potential of thin-film architectures of immobilized QDs as a platform for light-driven hydrogen evolution without the need for intricate surface modifications to ensure colloidal stability in aqueous environments.
Download full-text PDF |
Source |
|---|---|
| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10120591 | PMC |
| http://dx.doi.org/10.1021/acsami.3c00184 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Light-Driven Hybrid Nanoreactor Harnessing the Synergy of Carboxysomes and Organic Frameworks for Efficient Hydrogen Production.
ACS Catal
December 2024
Institute of Systems, Molecular and Integrative Biology, University of Liverpool, Liverpool L69 7ZB, U.K.
Synthetic photobiocatalysts are promising catalysts for valuable chemical transformations by harnessing solar energy inspired by natural photosynthesis. However, the synergistic integration of all of the components for efficient light harvesting, cascade electron transfer, and efficient biocatalytic reactions presents a formidable challenge. In particular, replicating intricate multiscale hierarchical assembly and functional segregation involved in natural photosystems, such as photosystems I and II, remains particularly demanding within artificial structures.
View Article and Find Full Text PDFYour Invitation to contribute to Chem. Eur. J. Electrocatalytic HER Performance of [FeFe]-Hydrogenase Mimics Bearing M-salen Moieties (M = Zn, Ni, Fe, Mn).
Chemistry
December 2024
Universidad Complutense de Madrid, Organic Chemistry, SPAIN.
The synthesis and characterization of novel compounds (5-8) as mimetics of [FeFe]-hydrogenase, combining two distinct systems capable of participating in hydrogen evolution reactions (HER): the [(μ-adt)Fe2(CO)6] fragment and M-salen complexes (salen = N,N'-bis(salicylidene)ethylenediamine) (M = Zn, Ni, Fe, Mn), is reported. These complexes were synthesized in high yields via a three-step procedure from N,N'-bis(4-R-salicylidene)ethanediamine) 4 [R = Fe2(CO)6(μ-SCH2)2COCH2O)]. Structural analysis through spectroscopic, spectrometric, and computational (DFT) methods confirmed distorted tetrahedral and square-planar geometries for Zn-salen and Ni-salen complexes (5 and 6) respectively, while complexes Fe-salen 7 and Mn-salen 8 exhibit square-based pyramidal structures typical of Fe(III) and Mn(III) high-spin salen-complexes.
View Article and Find Full Text PDFMathematical modeling of biohydrogen production via dark fermentation of fruit peel wastes by Clostridium butyricum NE95.
BMC Biotechnol
December 2024
Department of Botany and Microbiology, Faculty of Science, Suez University, P.O. Box 43221, Suez, Egypt.
Background: Biohydrogen production from agro-industrial wastes through dark fermentation offers several advantages including eco-friendliness, sustainability, and the simplicity of the process. This study aimed to produce biohydrogen from fruit and vegetable peel wastes (FVPWs) by anaerobic fermentative bacteria isolated from domestic wastewater. Kinetic analysis of the produced biohydrogen by five isolates on a glucose medium was analyzed using a modified Gompertz model (MGM).
View Article and Find Full Text PDFSemiartificial Photosynthetic Nanoreactors for H Generation.
J Am Chem Soc
December 2024
Leiden Institute of Chemistry, Leiden University, PO box 9502, 2300 RA Leiden, The Netherlands.
A relatively unexplored energy source in synthetic cells is transmembrane electron transport, which like proton and ion transport can be light driven. Here, synthetic cells, called nanoreactors, are engineered for compartmentalized, semiartificial photosynthetic H production by a [FeFe]-hydrogenase (Hase). Transmembrane electron transfer into the nanoreactor was enabled by MtrCAB, a multiheme transmembrane protein from MR-1.
View Article and Find Full Text PDFMesoporous Electrodes Enhance the Electrocatalytic Performance of [FeFe]-Hydrogenase.
Angew Chem Int Ed Engl
November 2024
Department of Inorganic and Analytical Chemistry, University of Geneva, Faculty of Sciences, Quai Ernest-Ansermet 30, 1211, Geneva 4, Switzerland.
The metalloenzyme [FeFe]-hydrogenase is of interest to future biotechnologies targeting the production of "green" hydrogen (H). We recently developed a simple two-step functionalized procedure to immobilize the [FeFe]-hydrogenase from Clostridium pasteurianum ("CpI") on mesoporous indium tin oxide (ITO) electrodes to achieve elevated H production with high operational stability and current densities of 8 mA cm. Here, we use a combination of atomic force microscopy (AFM), scanning electron microscopy (SEM) and electrochemical quartz crystal microbalance (EQCM) to understand how mesoporous ITO stabilizes and activates CpI for electroenzymatic H production.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!