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Solar-assisted photocatalytic water splitting using defective UiO-66 solids from modulated synthesis

Nano Research 2024年第5期17卷 4134-4150页

作者： Celia M.Rueda-Navarro María Cabrero-Antonino Paula Escamilla Valentín Díez-Cabanes Dong Fan Pedro Atienzar Belén Ferrer Ignacio Vayá guillaume maurin.herme g.baldov. Sergio Navalón Departamento de Química Universitat Politècnica de ValènciaCamino de Vera s/nValencia 46022Spain Instituto de Ciencia Molecular(ICMOL) Universitat de ValènciaPaterna 46980Spain ICgM Univ.MontpellierCNRSENSCMMontpellier34095France Instituto de Tecnología Química(UPV-CSIC) Universitat Politècnica de ValènciaAvenida de los Naranjos s/nValencia 46022Spain

Metal-organic frameworks(MOFs)are attracting increasing interests as photocatalysts for solar-driven hydrogen production from *** paper reports on a comparative study of using either acetic acid(AA)or trifluoroacetic acid(TFA)as the representative UiO-66 organic modulators for synthesizing visible light responsive UiO-66(Zr)-X(X:NH_(2) or NO_(2))photocatalysts for water *** results show that photocatalytic hydrogen generation from a water/methanol mixture can be improved by varying the nature and amount of the modulator employed to prepare the different UiO-66(Zr)-X(X:NH_(2) or NO_(2))solid ***-66(Zr)-NH_(2) was the most active photocatalyst,followed by UiO-66(Zr)-NO_(2),both prepared with 12 equivalents of AA with respect to the organic *** UiO-66(Zr)-NH_(2) solid was more active than the parent MOF in photocatalytic overall water splitting(OWS)(H_(2) and O_(2) production of 450 and 160μmol·g^(-1),respectively,in 5 h;apparent quantum yield(AQY)at 400 nm of 0.06%)in the absence of methanol and compares favourably with analogous *** on the photocatalytic activity of the most active solids of both series was obtained by means of a series of techniques,including ultraviolet-visible(UV-vis)diffuse reflectance,X-ray photoelectron spectroscopy(XPS),laser flash photolysis(LFP),electron spin resonance(ESR),photoluminescence and photoelectrochemical measurements together with density functional theory(DFT)*** results showed that organic acid modulators can be used to enhance the photocatalytic activity of missing linker UiO-66 defective materials in solar-powered water splitting.

关键词： heterogeneous photocatalysis metal-organic frameworks(MOFs) UiO-66 materials carboxylic acid modulators water splitting solar light

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Acidic open-cage solution containing basic cage-confined nanospaces for multipurpose catalysis

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National Science Review 2022年第5期9卷 99-107页

作者： Kang Li Kai Wu Yan-Zhong Fan Jing guo Yu-Lin Lu Yuan-Fan Wang guillaume maurin Cheng-Yong Su MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-sen University School of Chemistry South China Normal University Institute Charles gerhardt Montpellier Centre National de la Recherche Scientifiqueécole Nationale Supérieure de Chimie de MontpellierUniversité de Montpellier

The nanoscale chemical spaces inherent in porous organic/coordination cages or solid/liquid materials have been continuously explored for their nanoconfinement effect on selective adsorption and reaction of small gas or organic ***,we aim to rationalize the unconventional chemical reactivities motivated by the cage-confined nanospaces in aqueous solutions,where the robust yet permeable nanospaces defined by the open cages facilitate dynamic guest exchange and unusual chemical *** high positive charges on [(Pd/Pt)6(RuL3)8]28+nanocages drive imidazole-proton equilibrium to display a significantly perturbed pKashift,creating cage-defined nanospaces in solution with distinct intrinsic basicity and extrinsic *** supramolecular cage effect plays pivotal roles in elaborating robust solution nanospaces,controlling ingress-and-egress molecular processes through open-cage portals and endowing nanocages with transition-state stabilization,amphoteric reactivities and the phase transfer of insoluble molecules,thus promoting chemical transformations in unconventional ***,a wide range of application of cage-confined catalysis with anomalous reactivities maybe expected based on this kind of open-cage solution medium,which combines cage nanocavity,solution heterogeneity and liquid-phase fluidity to benefit various potential mass transfer and molecular process options.

关键词： open-cage solution supramolecular cage effect supramolecular catalysis cage-confined catalysis cage-confined nanospaces in solution

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