Utilizing mixed-linker zirconium based metal-organic frameworks to enhance the visible light photocatalytic oxidation of alcohol

Goh, Tian Wei; Xiao, Chaoxian; Maligal‐Ganesh, Raghu V.; Li, Xinle; Huang, Wenyu

doi:10.1016/j.ces.2014.08.052

Cited by 115 publications

(78 citation statements)

References 33 publications

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“…These studies reveal that the change of organic ligand is an effective method to regulate band gap of MOF. Although in recent years many efforts have been made to modify the organic ligands of MOFs, 5,9,11,20,21 the effects of ligand functionalization on the photocatalytic properties of MOFs are still unclear. It is obvious that a better understanding the mechanism of ligand modification is important to develop new MOF-based photocatalysts.…”

Section: Introductionmentioning

confidence: 99%

“…Especially, many investigations have demonstrated that MOF materials are promising catalysts in photocatalysis. 5,6,[9][10][11][12][13][14][15][16] As one of the most popular MOF, 1,[5][6][7] the titanium-based MIL-125 can catalyze the oxidation of alcohols to aldehydes under the UV irradiation, indicating that MIL-125 is an active photocatalyst. 10 However, because of the large optical band gap (3.6 eV), 10 MIL-125 is only active under UV irradiation.…”

Section: Introductionmentioning

confidence: 99%

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Effects of ligand functionalization on the photocatalytic properties of titanium-based MOF: A density functional theory study

et al. 2018

AIP Advances

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The first principle calculations have been performed to investigate the geometries, band structures and optical absorptions of a series of MIL-125 MOFs, in which the 1,4-benzenedicarboxylate (BDC) linkers are modified by different types and amounts of chemical groups, including NH2, OH, and NO2. Our results indicate that new energy bands will appear in the band gap of pristine MIL-125 after introducing new group into BDC linker, but the components of these band gap states and the valence band edge position are sensitive to the type of functional group as well as the corresponding amount. Especially, only the incorporation of amino group can obviously decrease the band gap of MIL-125, and the further reduction of the band gap can be observed if the amount of NH2 is increased. Although MIL-125 functionalized by NH2 group exhibits relatively weak or no activity for the photocatalytic O2 evolution by splitting water, such ligand modification can effectively improve the efficiency in H2 production because now the optical absorption in the visible light region is significantly enhanced. Furthermore, the adsorption of water molecule becomes more favorable after introducing of amino group, which is also beneficial for the water-splitting reaction. The present study can provide theoretical insights to design new photocatalysts based on MIL-125.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Effects of ligand functionalization on the photocatalytic properties of titanium-based MOF: A density functional theory study

et al. 2018

AIP Advances

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“…Fortunately, these alcohols are selectively oxidized to their respective aldehydes employing optimum conditions. It is clear that the catalytic system was found to be also effective for the selective oxidation of primary aromatic alcohols (Table 6, entries [10][11][12][13][14][15][16][17][18][19][20][21][22]. In addition, selectivity toward aldehydes is more than 99%, because there no over-oxidation to acids occurred, except that the aldehyde was observed.…”

Section: Reusability Of Catalystmentioning

confidence: 93%

Ag2O Nanoparticles-Doped Manganese Immobilized on Graphene Nanocomposites for Aerial Oxidation of Secondary Alcohols

Assal

Shaik

Kuniyil

et al. 2018

Metals

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Ag 2 O nanoparticles-doped MnO 2 decorated on different percentages of highly reduced graphene oxide (HRG) nanocomposites, i.e., (X%)HRG/MnO 2 -(1%)Ag 2 O (where X = 0-7), were fabricated through straight-forward precipitation procedure, and 400 • C calcination, while upon calcination at 300 • C and 500 These nanocomposites have been found to be efficient and very effective heterogeneous catalysts for selective oxidation of secondary alcohols into their respective ketones using O 2 as a sole oxidant without adding surfactants or nitrogenous bases. Moreover, a comparative catalytic study was carried out to investigate the catalytic efficiency of the synthesized nanocomposites for the aerobic oxidation of 1-phenylethanol to acetophenone as a substrate reaction. Effects of several factors were systematically studied. The as-prepared nanocomposites were characterized by TGA, XRD, SEM, EDX, HRTEM, BET, Raman, and FTIR. The catalyst with structure (5%)HRG/MnO 2 -(1%)Ag 2 O showed outstanding specific activity (16.0 mmol/g·h) with complete conversion of 1-phenylethanol and >99% acetophenone selectivity within short period (25 min). It is found that the effectiveness of the catalyst has been greatly improved after using graphene support. A broad range of alcohols have selectively transformed to desired products with 100% convertibility and no over-oxidation products have been detected. The recycling test of (5%)HRG/MnO 2 -(1%)Ag 2 O catalyst for oxidation of 1-phenylethanol suggested no obvious decrease in its performance and selectivity even after five subsequent runs.

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“…[98] It is proposed that the presenceo fh alogenated ligand stabilizes the active species CO 2 À on Zr 3 + ,i nhibiting the recombination of the charge carriers and thus facilitating the reaction. Huang and co-workers reported that the introduction of halogenated ligand into NH 2 -UiO-66(Zr) to form the mixed-ligand MOFs enhanced the photocatalytic activity for benzyl alcohol oxidation.…”

Section: Reactions Initiated By Photoactive Metal Nodesmentioning

confidence: 99%

Visible Light Induced Organic Transformations Using Metal‐Organic‐Frameworks (MOFs)

Deng

Garcı́a

2017

Chemistry A European J

180

111

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With the aim of developing renewable energy based processes, researchers are paying increasing interest to light induced organic transformations. Metal-organic frameworks (MOFs), a class of micro-/mesoporous hybrid materials, are recently emerging as a new type of photoactive materials for organic syntheses due to their unique structural characteristics. In this Review, we summarized the recent applications of MOFs as photocatalysts for light induced organic transformations, including (1) oxidation of alcohols, amines, alkene, alkanes and sulfides; (2) hydroxylation of aromatic compounds like benzene; (3) activation of the C-H bonds to construct new C-C or C-X bonds; (4) atom-transfer radical polymerization (ATRP). This Review starts with general background information of using MOFs in photocatalysis, followed by a description of light induced organic transformations promoted by photoactive inorganic nodes and photocatalytic active ligands in MOFs, respectively. Thereafter, the use of MOFs as multifunctional catalysts for light induced organic transformations via an efficient merge of the metal/ligand/guest based catalysis where the photocatalytic activity of MOFs plays a key role are discussed. Finally, the limitations, challenges and the future perspective of the application of MOFs for light induced organic transformations were addressed. The objective of this Review is to serve as a starting point for other researchers to get into this largely unexplored field. It is also our goal to stimulate intensive research in this field for rational designing of MOF materials to overcome their current limitations in photocatalysis, which can lead to more creative visible-light-induced organic transformations.

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Utilizing mixed-linker zirconium based metal-organic frameworks to enhance the visible light photocatalytic oxidation of alcohol

Cited by 115 publications

References 33 publications

Effects of ligand functionalization on the photocatalytic properties of titanium-based MOF: A density functional theory study

Effects of ligand functionalization on the photocatalytic properties of titanium-based MOF: A density functional theory study

Ag2O Nanoparticles-Doped Manganese Immobilized on Graphene Nanocomposites for Aerial Oxidation of Secondary Alcohols

Visible Light Induced Organic Transformations Using Metal‐Organic‐Frameworks (MOFs)

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