Insights into the Molecular Assembly of Zeolitic Imidazolate Frameworks by ESI-MS

ZIFs are an interesting class of MOFs with zeolite-like topologies, owing to their structural similarities. Rational design and synthesis of ZIFs are highly challenging due to limited understanding of their formation process from solution, as previous studies were largely on crystal growth and properties. In this contribution, we describe a systematic approach to synthesize well-defined ZIF-8 crystals at different rates of nucleation by adjusting zinc to 2-methylimidazole ratios. For the first time, we report discrete chemical species detected in ZIF-8 synthesis and trace their transition with time using ESI-MS. Cravillon et al. have previously described three essential steps in ZIF-8 nucleation: (i) complex formation, (ii) complex deprotonation, and (iii) ligand exchange and oligomerization. In our work, we were able to identify species undergoing the various steps and correlate their evolution to the different nucleation rates. Applying ESI-MS in both positive and negative modes, we identified two speci...

[1]  S. Kitagawa,et al.  Functional Hybrid Porous Coordination Polymers , 2014 .

[2]  Michael O’Keeffe,et al.  The Chemistry and Applications of Metal-Organic Frameworks , 2013, Science.

[3]  Z. Zhong,et al.  High-yield synthesis of zeolitic imidazolate frameworks from stoichiometric metal and ligand precursor aqueous solutions at room temperature , 2013 .

[4]  Koji Kida,et al.  Formation of high crystalline ZIF-8 in an aqueous solution , 2013 .

[5]  F. Schüth,et al.  The formation of zeolites from solution – Analysis by mass spectrometry , 2013 .

[6]  Cheng Guo,et al.  An experimental and theoretical study on fragmentation of protonated N-(2-pyridinylmethyl)indole in electrospray ionization mass spectrometry. , 2012, Rapid communications in mass spectrometry : RCM.

[7]  Koji Kida,et al.  Size-controlled Synthesis of Zeolitic Imidazolate Framework-8 (ZIF-8) Crystals in an Aqueous System at Room Temperature , 2012 .

[8]  Fu-an Sun,et al.  Hydrothermal synthesis of zeolitic imidazolate framework-67 (ZIF-67) nanocrystals , 2012 .

[9]  E. Sherman,et al.  Aqueous room temperature synthesis of cobalt and zinc sodalite zeolitic imidizolate frameworks. , 2012, Dalton transactions.

[10]  Yi Wang,et al.  Imparting functionality to a metal-organic framework material by controlled nanoparticle encapsulation. , 2012, Nature chemistry.

[11]  Shyam Biswas,et al.  Synthesis of metal-organic frameworks (MOFs): routes to various MOF topologies, morphologies, and composites. , 2012, Chemical reviews.

[12]  J. Caro,et al.  Formate modulated solvothermal synthesis of ZIF-8 investigated using time-resolved in situ X-ray diffraction and scanning electron microscopy , 2012 .

[13]  H. Su,et al.  Tuning the crystal morphology and size of zeolitic imidazolate framework-8 in aqueous solution by surfactants , 2011 .

[14]  J. Cravillon,et al.  Fast nucleation and growth of ZIF-8 nanocrystals monitored by time-resolved in situ small-angle and wide-angle X-ray scattering. , 2011, Angewandte Chemie.

[15]  Michael W Anderson,et al.  Revelation of the molecular assembly of the nanoporous metal organic framework ZIF-8. , 2011, Journal of the American Chemical Society.

[16]  J. Jasinski,et al.  Room-Temperature Synthesis of ZIF-8: The Coexistence of ZnO Nanoneedles , 2011 .

[17]  Klaus Huber,et al.  Controlling Zeolitic Imidazolate Framework Nano- and Microcrystal Formation: Insight into Crystal Growth by Time-Resolved In Situ Static Light Scattering , 2011 .

[18]  Z. Lai,et al.  Rapid synthesis of zeolitic imidazolate framework-8 (ZIF-8) nanocrystals in an aqueous system. , 2011, Chemical communications.

[19]  M. Allendorf,et al.  Metal‐Organic Frameworks: A Rapidly Growing Class of Versatile Nanoporous Materials , 2011, Advanced materials.

[20]  Graham N. Newton,et al.  Following the self assembly of supramolecular MOFs using X-ray crystallography and cryospray mass spectrometry , 2010 .

[21]  Michael O'Keeffe,et al.  High-Throughput Synthesis of Zeolitic Imidazolate Frameworks and Application to CO2 Capture , 2008, Science.

[22]  Gérard Férey,et al.  Hybrid porous solids: past, present, future. , 2008, Chemical Society reviews.

[23]  W. Boggess,et al.  Assembly of a homochiral, body-centered cubic network composed of vertex-shared Mg12 cages: use of electrospray ionization mass spectrometry to monitor metal carboxylate nucleation. , 2007, Journal of the American Chemical Society.

[24]  Michael O’Keeffe,et al.  Exceptional chemical and thermal stability of zeolitic imidazolate frameworks , 2006, Proceedings of the National Academy of Sciences.

[25]  Xiao-Ming Chen,et al.  Ligand-directed strategy for zeolite-type metal-organic frameworks: zinc(II) imidazolates with unusual zeolitic topologies. , 2006, Angewandte Chemie.

[26]  Bradley F. Chmelka,et al.  Nonionic Triblock and Star Diblock Copolymer and Oligomeric Surfactant Syntheses of Highly Ordered, Hydrothermally Stable, Mesoporous Silica Structures , 1998 .