Tandem Postsynthetic Modification of a Metal–Organic Framework by Thermal Elimination and Subsequent Bromination: Effects on Absorption Properties and Photoluminescence

Sun, Feng; Yin, Zheng; Wang, Que-Qiao; Sun, Di; Zeng, Ming‐Hua; Kurmoo, Mohamedally

doi:10.1002/anie.201300821

Cited by 135 publications

(67 citation statements)

References 41 publications

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“…For UV/Vis spectrophotometric monitoring of the reaction (Figure S8), we focused on the d–d transition of the nickel at around 650 nm and compared it to those of Ni(H 2 O) 6 (ClO 4 ) 2 in water and in CH 3 CN, in which the Ni 2+ ions are surrounded by six oxygen atoms (NiO 6 ) and six nitrogen atoms (NiN 6 ), respectively. The band energy for Ni 1 in CH 3 CN is centered between those of NiO 6 and NiN 6 , suggesting that the ligand L is not dissociated upon dissolution . Following the addition of Ni(H 2 O) 6 (ClO 4 ) 2 , the band moved closer to that of NiN 6 .…”

Section: Resultsmentioning

confidence: 99%

Stepwise Assembly of M^II₇ Clusters Revealed by Mass Spectrometry, EXAFS, and Crystallography

Yang

Yin

et al. 2016

Chemistry A European J

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The square-planar monomer NiL (Ni ), L=2-ethoxy-6-(N-methyl-iminomethyl)phenolate, reacts with M(H O) (ClO ) , M=Ni or Co, to form heptanuclear disks [Co Ni (OH) (L) ](ClO ) ⋅2 CH CN (Co Ni , x=0-7) and the co-crystal [Co Ni (OH) L ][NiL ](ClO ) ⋅2 CH CN (Co Ni -Ni ) under ambient conditions. It has proved possible to explore the bottom-up assembly process of Co Ni and Co Ni -Ni in real time. The final products have been characterized by thermogravimetric analysis, IR, elemental analysis, ICP-MS, and single-crystal X-ray diffraction. Time-dependent mass spectrometry (MS) revealed the following reaction steps: Ni →[M L ] →[M (OH) L ] →[M (OH) L ] . In contrast, the reaction of Ni with Zn only reaches halfway, and crystallographic evidence indicates a butterfly structure for [Zn Ni (OH) Cl ] (Zn Ni ), an intermediate that is difficult to isolate in the above Ni-Co series. A summation method has been used to analyze the MS of bimetallic clusters with very similar atomic masses, as is the case for Co and Ni. The results provide ample information on the distribution of Co and Ni within each cluster and their statistical distribution within selected crystals.

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Section: Resultsmentioning

confidence: 99%

Stepwise Assembly of M^II₇ Clusters Revealed by Mass Spectrometry, EXAFS, and Crystallography

Yang

Yin

et al. 2016

Chemistry A European J

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“…However, this PSM resulted in a loss of crystallinity and porosity of the framework. 29 The thermally-promoted elimination of water from a non-porous lithium-L-malate coordination polymer above 280 °C was demonstrated and quite remarkably the extent of elimination could be followed by single crystal diffraction. 30 Liberation of N 2 from azidefunctionalized MOFs at 150 °C to generate reactive nitrenes en route to isocyanates has also been reported.…”

Section: Introductionmentioning

confidence: 97%

High Temperature Postsynthetic Rearrangement of Dimethylthiocarbamate-Functionalized Metal–Organic Frameworks

Ablott

Turzer

Telfer

et al. 2016

Crystal Growth & Design

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. (2016). High temperature postsynthetic rearrangement of dimethylthiocarbamate-functionalized metal-organic frameworks. Crystal Growth and Design, 16 (12),[7067][7068][7069][7070][7071][7072][7073] High temperature postsynthetic rearrangement of dimethylthiocarbamatefunctionalized metal-organic frameworks AbstractA thermally promoted postsynthetic rearrangement has been performed on a zinc IRMOF-9-type framework bearing dimethylthiocarbamate tag groups. The rearrangement was accomplished via conventional heating at 285 °C. Crucially, despite the high temperature, the MOF maintains its high accessible surface area and pore space following thermal treatment. The structures and physical properties of the frameworks were characterized by a combination of single-crystal X-ray diffraction, powder X-ray diffraction, differential thermal-thermogravimetric analysis, and gas sorption analysis. The rearrangement results in a slightly higher level of CO 2 adsorption for the modified MOF but with equivalent heat of adsorption. This work offers new perspectives on postsynthetic rearrangements in MOFs and demonstrates that rearrangements that occur at relatively high temperatures are still compatible with the need to retain the structural integrity and porosity of the framework. A thermally-promoted post-synthetic rearrangement has been performed on a zinc IRMOF-9 type framework bearing dimethylthiocarbamate tag groups. The rearrangement was accomplished via conventional heating at 285 °C. Crucially, despite the high temperature, the MOF maintains its high accessible surface area and pore space following thermal treatment. The structures and physical properties of the frameworks were characterized by a combination of single X-ray diffraction (SCXRD), powder X-ray diffraction (PXRD), differential thermalthermogravimetric analysis (DT-TGA), and gas sorption analysis. The rearrangement results in a slightly higher level of CO 2 adsorption for the modified MOF but with equivalent heat of 2 adsorption. This work offers new perspectives on post-synthetic rearrangements in MOFs, and demonstrates that rearrangements that occur at relatively high temperatures are still compatible with the need to retain the structural integrity and porosity of the framework.

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“…In our previous work, we have been interested in designing different types of MOFs accurately, and finally realized their functional regulation through post-synthesis modification, such as catalysis, conduction and magnetism [29][30][31]. Furthermore, we have been engaged in the assembly process and mechanism of coordination molecular clusters and their post-synthesis modification or thermal transformation regulation [32][33][34].…”

Section: Introductionmentioning

confidence: 99%

Heptanuclear brucite disk with cyanide bridges in a cocrystal and tracking its pyrolysis to an efficient oxygen evolution electrode

et al. 2019

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Tandem Postsynthetic Modification of a Metal–Organic Framework by Thermal Elimination and Subsequent Bromination: Effects on Absorption Properties and Photoluminescence

Cited by 135 publications

References 41 publications

Stepwise Assembly of M^II₇ Clusters Revealed by Mass Spectrometry, EXAFS, and Crystallography

Stepwise Assembly of M^II₇ Clusters Revealed by Mass Spectrometry, EXAFS, and Crystallography

High Temperature Postsynthetic Rearrangement of Dimethylthiocarbamate-Functionalized Metal–Organic Frameworks

Heptanuclear brucite disk with cyanide bridges in a cocrystal and tracking its pyrolysis to an efficient oxygen evolution electrode

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Tandem Postsynthetic Modification of a Metal–Organic Framework by Thermal Elimination and Subsequent Bromination: Effects on Absorption Properties and Photoluminescence

Cited by 135 publications

References 41 publications

Stepwise Assembly of MII7 Clusters Revealed by Mass Spectrometry, EXAFS, and Crystallography

Stepwise Assembly of MII7 Clusters Revealed by Mass Spectrometry, EXAFS, and Crystallography

High Temperature Postsynthetic Rearrangement of Dimethylthiocarbamate-Functionalized Metal–Organic Frameworks

Heptanuclear brucite disk with cyanide bridges in a cocrystal and tracking its pyrolysis to an efficient oxygen evolution electrode

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Product

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Stepwise Assembly of M^II₇ Clusters Revealed by Mass Spectrometry, EXAFS, and Crystallography

Stepwise Assembly of M^II₇ Clusters Revealed by Mass Spectrometry, EXAFS, and Crystallography