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Dive into the research topics where Matthias Zeller is active.

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Featured researches published by Matthias Zeller.


Chemical Communications | 2009

Near-infrared emitting ytterbium metal–organic frameworks with tunable excitation properties

Kiley A. White; Demetra A. Chengelis; Matthias Zeller; Steven J. Geib; Jessica Szakos; Stéphane Petoud; Nathaniel L. Rosi

The design of metal-organic frameworks (MOFs) incorporating near-infrared emitting ytterbium cations and organic sensitizers allows for the preparation of new materials with tunable and enhanced photophysical properties.


Chemical Communications | 2009

In situ tetrazole ligand synthesis leading to a microporous cadmium–organic framework for selective ion sensing

Yongcai Qiu; Hong Deng; Jixia Mou; Shihe Yang; Matthias Zeller; Stuart R. Batten; Haohan Wu; Jing Li

In situ tetrazole ligand synthesis leads to a luminescent microporous cadmium-organic framework {[Cd(mu2-Cl)(mu4-5MT)]n (5MT = 5-methyl-1H-tetrazole)} that exhibits a high-sensitivity sensing function with respect to nitrite in both DMF and water.


Nature | 2016

Machine-learning-assisted materials discovery using failed experiments

Paul Raccuglia; Katherine C. Elbert; Philip Adler; Casey Falk; Malia B. Wenny; Aurelio Mollo; Matthias Zeller; Sorelle A. Friedler; Joshua Schrier; Alexander J. Norquist

Inorganic–organic hybrid materials such as organically templated metal oxides, metal–organic frameworks (MOFs) and organohalide perovskites have been studied for decades, and hydrothermal and (non-aqueous) solvothermal syntheses have produced thousands of new materials that collectively contain nearly all the metals in the periodic table. Nevertheless, the formation of these compounds is not fully understood, and development of new compounds relies primarily on exploratory syntheses. Simulation- and data-driven approaches (promoted by efforts such as the Materials Genome Initiative) provide an alternative to experimental trial-and-error. Three major strategies are: simulation-based predictions of physical properties (for example, charge mobility, photovoltaic properties, gas adsorption capacity or lithium-ion intercalation) to identify promising target candidates for synthetic efforts; determination of the structure–property relationship from large bodies of experimental data, enabled by integration with high-throughput synthesis and measurement tools; and clustering on the basis of similar crystallographic structure (for example, zeolite structure classification or gas adsorption properties). Here we demonstrate an alternative approach that uses machine-learning algorithms trained on reaction data to predict reaction outcomes for the crystallization of templated vanadium selenites. We used information on ‘dark’ reactions—failed or unsuccessful hydrothermal syntheses—collected from archived laboratory notebooks from our laboratory, and added physicochemical property descriptions to the raw notebook information using cheminformatics techniques. We used the resulting data to train a machine-learning model to predict reaction success. When carrying out hydrothermal synthesis experiments using previously untested, commercially available organic building blocks, our machine-learning model outperformed traditional human strategies, and successfully predicted conditions for new organically templated inorganic product formation with a success rate of 89 per cent. Inverting the machine-learning model reveals new hypotheses regarding the conditions for successful product formation.


Journal of the American Chemical Society | 2012

White Light Emission and Second Harmonic Generation from Secondary Group Participation (SGP) in a Coordination Network

Jun He; Matthias Zeller; Allen D. Hunter; Zhengtao Xu

We describe a white emitting coordination network solid that can be conveniently applied as a thin film onto a commercial UV-LED lamp for practical white lighting applications. The solid state material was discovered in an exercise of exploring molecular building blocks equipped with secondary groups for fine-tuning the structures and properties of coordination nets. Specifically, CH(3)SCH(2)CH(2)S- and (S)-CH(3)(OH)CHCH(2)S- (2-hydroxylpropyl) were each attached as secondary groups to the 2,5- positions of 1,4-benzenedicarboxylic acid (bdc), and the resultant molecules (L1 and L2, respectively) were crystallized with Pb(II) into the topologically similar 3D nets of PbL1 and PbL2, both consisting of interlinked Pb-carboxyl chains. While the CH(3)S- groups in PbL1 are not bonded to the Pb(II) centers, the hydroxy groups in PbL2 participate in coordinating to Pb(II) and thus modify the bonding features around the Pb(II), but only to a slight and subtle degree (e.g., Pb-O distances 2.941-3.116 Å). Interestingly, the subtle change in structure significantly impacts the properties, i.e., while the photoluminescence of PbL1 is yellowish green, PbL2 features bright white emission. Also, the homochiral side group in PbL2 imparts significant second harmonic generation, in spite of its seemingly weak association with the main framework (the NLO-phore). In a broad perspective, this work showcases the idea of secondary group participation (SGP) in the construction of coordination networks, an idea that parallels that of hemilabile ligands in organometallics and points to an effective strategy in developing advanced functions in solid state framework materials.


Journal of the American Chemical Society | 2013

Convenient Detection of Pd(II) by a Metal–Organic Framework with Sulfur and Olefin Functions

Jun He; Meiqin Zha; Jieshun Cui; Matthias Zeller; Allen D. Hunter; Shek-Man Yiu; Shuit-Tong Lee; Zhengtao Xu

A highly specific, distinct color change in the crystals of a metal-organic framework with pendant allyl thioether units in response to Pd species was discovered. The color change (from light yellow to orange/brick red) can be triggered by Pd species at concentrations of a few parts per million and points to the potential use of these crystals in colorimetric detection and quantification of Pd(II) ions. The swift color change is likely due to the combined effects of the multiple functions built into the porous framework: the carboxyl groups for bonding with Zn(II) ions to assemble the host network and the thioether and alkene functions for effective uptake of the Pd(II) analytes (e.g., via the alkene-Pd interaction). The resultant loading of Pd (and other noble metal) species into the porous solid also offers rich potential for catalysis applications, and the alkene side chains are amenable to wide-ranging chemical transformations (e.g., bromination and polymerization), enabling further functionalization of the porous networks.


CrystEngComm | 2010

Rationally designed and controlled syntheses of different series of 4d–4f heterometallic coordination frameworks based on lanthanide carboxylate and Ag(IN)2 substructures

Yongcai Qiu; Zhi-Hui Liu; Jixia Mou; Hong Deng; Matthias Zeller

Different series of Ln(III)–Ag(I) heterometallic coordination frameworks, namely LnAg(OAc)(IN)2(H2O)·(ClO4) [Ln = Tb (1a); Ho (1b), HOAc = acetic acid, HIN = isonicotinic acid], LnAg2(OX)0.5(IN)3(H2O)1.5·(ClO4) [Ln = Nd (2a); Eu (2b) Tb (2c), OX = oxalate], Eu2Ag3(OX)0.5(IN)6(NO3)(ClO4)(H2O)3·2(H2O) (3), LnAg(OX) (IN)2(H2O) [Ln = Ce (4a); Sm (4b)], LnAg(Mal)(IN)2(H2O) [Ln = La (5a); Nd (5b), H2Mal = malonic acid], Ln3Ag4(Lac)2(IN)8(H2O)5·2(ClO4)·2.5(H2O) [Ln = La (6a); Lu (6b), HLac = lactic acid], Sm3Ag4(Lac)2(IN)8(H2O)4·2(ClO4)·2.5(H2O) (7), and Eu2Ag3(S-Lac)(IN)6(H2O)4·2(ClO4)·4(H2O) (8) were successfully synthesized by systematic variation of reaction parameters such as initial reactants, reaction time, pH, temperature, etc. Compounds 1a and 1b represent 3D coordination frameworks that are constructed from adjacent lanthanide carboxylate layers and pillared Ag(IN)2 units. Compounds 2a, 2b and 2c comprise of 2D Ln-carboxylate-Ag layered networks and pillared Ag(IN)2 units. Compound 3 exhibits 3D coordination frameworks that are built up from the assembly of europium-carboxylate layers and pillared Ag(IN)2 units. 3D coordination networks of compounds 4a and 4b containing tetranuclear Ln2Ag2 cores are constructed from 2D cerium oxalate layers and tilted pillared Ag(IN)2 subunits. Compounds 5a and 5b display attractive 3D coordination frameworks constructed of 2D lanthanum malonate chains and pillared Ag(IN)2 units. Compounds 6a and 6b are 2D coordination frameworks comprised of 1D racemic lanthanum carboxylate chains and pillared Ag(IN)2 units. The crystal structure of 7 is almost the same as that of 6a and 6b, only one less coordination water molecule is coordinated to its metal centre. Compound 8, which spontaneously resolved upon crystallization, represents the first example of a 3D Ln–Ag coordination framework built up from 1D europium-carboxylate chains containing chiral molecules and pillared Ag(IN)2 units.


CrystEngComm | 2007

Mercury(II) coordination polymers generated from 1,4-bis(2 or 3 or 4-pyridyl)-2,3-diaza-1,3-butadiene ligands

Ghodrat Mahmoudi; Ali Morsali; Allen D. Hunter; Matthias Zeller

A series of new polymeric mercury(II) complexes, [Hg(4-bpdb)(SCN)2]n (1), [Hg(3-bpdb)(SCN)2]n (2), [Hg(4-bpdb)Br2]n (3), [Hg(3-bpdb)Br2]n (4) and [Hg2(2-bpdb)Br4]n (5) {4-bpdb = 1,4-bis(4-pyridyl)-2,3-diaza-1,3-butadiene, 3-bpdb = 1,4-bis(3-pyridyl)-2,3-diaza-1,3-butadiene and 2-bpdb = 1,4-bis(2-pyridyl)-2,3-diaza-1,3-butadiene} was prepared from reactions of mercury(II) thiocyanate or bromide with three organic nitrogen donor-based ligands under thermal gradient conditions using the branched tube method. All these compounds were structurally characterized by single-crystal X-ray diffraction. The thermal stabilities of compounds 1–5 were studied by thermal gravimetric (TG) and differential thermal analyses (DTA).


Journal of the American Chemical Society | 2011

Helimeric Porphyrinoids: Stereostructure and Chiral Resolution of meso-Tetraarylmorpholinochlorins

Christian Brückner; Daniel C. G. Götz; Simon P. Fox; Claudia Ryppa; Jason R. McCarthy; Torsten Bruhn; Joshua Akhigbe; Subhadeep Banerjee; Pedro Daddario; Heather W. Daniell; Matthias Zeller; Ross W. Boyle; Gerhard Bringmann

The synthesis and chiral resolution of free-base and Ni(II) complexes of a number of derivatives of meso-tetraphenylmorpholinochlorins, with and without direct β-carbon-to-o-phenyl linkages to the flanking phenyl groups, is described. The morpholinochlorins, a class of stable chlorin analogues, were synthesized in two to three steps from meso-tetraphenylporphyrin. The conformations and the relative stereostructures of a variety of free-base and Ni(II) complexes of these morpholinochlorins were elucidated by X-ray diffractometry. Steric and stereoelectronic arguments explain the relative stereoarray of the morpholino-substituents, which differ in the free-base and Ni(II) complexes, and in the monoalkoxy, β-carbon-to-o-phenyl linked morpholinochlorins, and the dialkoxy derivatives. The Ni(II) complexes were all found to be severely ruffled whereas the free-base chromophores are more planar. As a result of the helimeric distortion of their porphyrinoid chromophores, the ruffled macrocycles possess a stable inherent element of chirality. Most significantly, resolution of the racemic mixtures was achieved, both by classical methods via diastereomers and by HPLC on a chiral phase. Full CD spectra were recorded and modeled using quantum-chemical computational methods, permitting, for the first time, an assignment of the absolute configurations of the chromophores. The report expands the range of known pyrrole-modified porphyrins. Beyond this, it introduces large chiral porphyrinoid π-systems that exist in the form of two enantiomeric, stereochemically stable helimers that can be resolved. This forms the basis for possible future applications, for example, in molecular-recognition systems or in materials with chiroptic properties.


Angewandte Chemie | 2014

Pd Uptake and H2S Sensing by an Amphoteric Metal–Organic Framework with a Soft Core and Rigid Side Arms†

Jieshun Cui; Yan-Lung Wong; Matthias Zeller; Allen D. Hunter; Zhengtao Xu

Molecular components of opposite character are often incorporated within a single system, with a rigid core and flexible side arms being a common design choice. Herein, molecule L has been designed and prepared featuring the reverse design, with rigid side arms (arylalkynyl) serving to calibrate the mobility of the flexible polyether links in the core. Crystallization of this molecule with Pb(II)  ions led to a dynamic metal-organic framework (MOF) system that not only exhibits dramatic, reversible single-crystal-to-single-crystal transformations, but combines distinct donor and acceptor characteristics, allowing for substantial uptake of PdCl2 and colorimetric sensing of H2 S in water.


Science Advances | 2016

Mechanized azobenzene-functionalized zirconium metal-organic framework for on-command cargo release.

Xiangshi Meng; Bo Gui; Daqiang Yuan; Matthias Zeller; Cheng Wang

A simple strategy to construct a stimuli-responsive mechanized zirconium metal-organic framework for on-command cargo release. Stimuli-responsive metal-organic frameworks (MOFs) have gained increasing attention recently for their potential applications in many areas. We report the design and synthesis of a water-stable zirconium MOF (Zr-MOF) that bears photoresponsive azobenzene groups. This particular MOF can be used as a reservoir for storage of cargo in water, and the cargo-loaded MOF can be further capped to construct a mechanized MOF through the binding of β-cyclodextrin with the azobenzene stalks on the MOF surface. The resulting mechanized MOF has shown on-command cargo release triggered by ultraviolet irradiation or addition of competitive agents without premature release. This study represents a simple approach to the construction of stimuli-responsive mechanized MOFs, and considering mechanized UiO-68-azo made from biocompatible components, this smart system may provide a unique MOF platform for on-command drug delivery in the future.

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Allen D. Hunter

Youngstown State University

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Zhengtao Xu

City University of Hong Kong

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Jun He

Guangdong University of Technology

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Mazhar Hamid

Quaid-i-Azam University

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