Quantum dot gels as efficient and unique photocatalysts for organic synthesis

Liu, Daohua; Nyakuchena, James; Maity, Rajendra; Geng, Xin; Mahajan, Jyoti P.; Hewa-Rahinduwage, Chathuranga C.; Peng, Yi; Huang, Jier; Luo, Long

doi:10.1039/d2cc03872b

Cited by 12 publications

(13 citation statements)

References 38 publications

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“…For example, QD gels, once deprived of the surface ligands, exhibit superior photocatalytic activity due to more exposed active sites which improve the probability of reactant adsorption and promote charge transfer. 59 On one hand, constructing a great quantity of surface active sites is of great significance for greatly improving photocatalytic organic conversion, enabling effective reactants and adsorption rapid charge transfer. On the other hand, the application of selective organic conversion can be further expanded by surface structure reconstruction, such as changing the atomic composition and introducing defect vacancies or cocatalysts.…”

Section: Basic Principles Of Photocatalytic Organic Synthesis Of Qd-b...mentioning

confidence: 99%

Semiconductor quantum dots: a versatile platform for photoredox organic transformation

Tang

et al. 2023

J. Mater. Chem. A

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Section: Basic Principles Of Photocatalytic Organic Synthesis Of Qd-b...mentioning

confidence: 99%

Semiconductor quantum dots: a versatile platform for photoredox organic transformation

Tang

et al. 2023

J. Mater. Chem. A

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“… Quantum Dot Gels as Efficient and Unique Photocatalysts for Organic SynthesisChem. Commun.2022581126011263 …”

Section: Key Referencesmentioning

confidence: 99%

Section: Electrochemical Oxidative Gelation Of Qds (Covalent Assembly)mentioning

confidence: 99%

“…In this Account, we discuss our contribution to metal chalcogenide gel formation using electrochemical methods to drive covalent or non-covalent assembly, which enables direct writing on an active electrode surface or formation of free-standing monoliths, and the application of such materials in sensing and photocatalysis. − ,, Relative to conventional chemical approaches, electrochemical gelation of metal chalcogenide QDs enables the use of two additional levers for tuning the assembly process: electrode material and potential, allowing the controlled synthesis of complicated gel structures that are challenging to achieve using chemical means. The current challenges and prospects in this field are also briefly discussed.…”

Section: Introductionmentioning

confidence: 99%

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Electrochemical Gelation of Metal Chalcogenide Quantum Dots: Applications in Gas Sensing and Photocatalysis

et al. 2023

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Conspectus Metal chalcogenide quantum dots (QDs) are prized for their unique and functional properties, associated with both intrinsic (quantum confinement) and extrinsic (high surface area) effects, as dictated by their size, shape, and surface characteristics. Thus, they have considerable promise for diverse applications, including energy conversion (thermoelectrics and photovoltaics), photocatalysis, and sensing. QD gels are macroscopic porous structures consisting of interconnected QDs and pore networks in which the pores may be filled with solvent (i.e., wet gels) or air (i.e., aerogels). QD gels are unique because they can be prepared as macroscale objects while fully retaining the size-specific quantum-confined properties of the initial QD building blocks. The extensive porosity of the gels also ensures that each QD in the gel network is accessible to the ambient, leading to high performance in applications that require high surface areas, such as (photo)catalysis and sensing. Metal chalcogenide QD gels are conventionally prepared by chemical approaches. We recently expanded the toolbox for QD gel synthesis by developing electrochemical gelation methods. Relative to conventional chemical oxidation approaches, electrochemical assembly of QDs (1) enables the use of two additional levers for tuning the QD assembly process and gel structure: electrode material and potential, and (2) allows direct gel formation on device substrates to simplify device fabrication and improve reproducibility. We have discovered two distinct electrochemical gelation methods, each of which enables the direct writing of gels on an active electrode surface or the formation of free-standing monoliths. Oxidative electrogelation of QDs leads to assemblies bridged by dichalcogenide (covalent) linkers, whereas metal-mediated electrogelation proceeds via electrodissolution of active metal electrodes to produce free ions that link QDs by binding to pendant carboxylate functionalities on surface ligands (non-covalent linkers). We further demonstrated that the electrogel composition produced from the covalent assembly could be modified by controlled ion exchange to form single-ion decorated bimetallic QD gels, a new category of materials. The QD gels exhibit unprecedented performance for NO2 gas sensing and unique photocatalytic reactivities (e.g., the “cyano dance” isomerization and the reductive ring-opening arylation). The chemistry unveiled during the development of electrochemical gelation pathways for QDs and their post-modification has broad implications for guiding the design of new nanoparticle assembly strategies and QD gel-based gas sensors and catalysts.

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“…Developing new types of metallogels and tuning them have been attracting considerable attention since the last two decades owing to their fascinating structural aspects and significant molecular interactions. 1 Also, these have become useful in various disciplines of contemporary research and applications by means of significant catalysts, 2 light harvesting materials, 3,4 sensors, 5,6 conductors, 7 magnetic and nano soft-materials, 8 carbon dots actuators, 9 quantum dots, 10 biomedical devices, 11 and therapeutic agents. 12 Their syntheses and properties pertaining to sophisticated supramolecular interactions may be significantly tuned employing several external stimuli such as sonication, photochemical, pH, temperature, redox stimulators, or other additives on suitable molecules called gelators.…”

Section: Introductionmentioning

confidence: 99%

Acquiring preferred mode of aggregation through positional antagonism for saponification triggered gelation

Chand

Kumar

2023

New J. Chem.

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Quantum dot gels as efficient and unique photocatalysts for organic synthesis

Abstract: Here we report CdS quantum dot (QD) gels as highly efficient and unique photocatalysts for organic synthesis. We found that the photocatalytic activity of CdS QD gel was superior to...

Cited by 12 publications

References 38 publications

Semiconductor quantum dots: a versatile platform for photoredox organic transformation

Semiconductor quantum dots: a versatile platform for photoredox organic transformation

Electrochemical Gelation of Metal Chalcogenide Quantum Dots: Applications in Gas Sensing and Photocatalysis

Acquiring preferred mode of aggregation through positional antagonism for saponification triggered gelation

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