scholarly journals Wafer-scale synthesis of monolayer two-dimensional porphyrin polymers for hybrid superlattices

Science ◽  
2019 ◽  
Vol 366 (6471) ◽  
pp. 1379-1384 ◽  
Author(s):  
Yu Zhong ◽  
Baorui Cheng ◽  
Chibeom Park ◽  
Ariana Ray ◽  
Sarah Brown ◽  
...  
Keyword(s):  
Large Scale ◽  
Building Blocks ◽  
Two Dimensional ◽  
Wafer Scale ◽  
Molecular Building Blocks ◽  
2D Polymers ◽  
Metal Organic ◽  
Artificial Solids ◽  
Ultimate Limit ◽  
Porphyrin Polymers

The large-scale synthesis of high-quality thin films with extensive tunability derived from molecular building blocks will advance the development of artificial solids with designed functionalities. We report the synthesis of two-dimensional (2D) porphyrin polymer films with wafer-scale homogeneity in the ultimate limit of monolayer thickness by growing films at a sharp pentane/water interface, which allows the fabrication of their hybrid superlattices. Laminar assembly polymerization of porphyrin monomers could form monolayers of metal-organic frameworks with Cu2+ linkers or covalent organic frameworks with terephthalaldehyde linkers. Both the lattice structures and optical properties of these 2D films were directly controlled by the molecular monomers and polymerization chemistries. The 2D polymers were used to fabricate arrays of hybrid superlattices with molybdenum disulfide that could be used in electrical capacitors.

scholarly journals Chemical engineering of quasicrystal approximants in lanthanide-based coordination solids

2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Laura Voigt ◽  
Mariusz Kubus ◽  
Kasper S. Pedersen
Keyword(s):  
Chemical Engineering ◽  
Organic Materials ◽  
Building Blocks ◽  
Lanthanide Ions ◽  
Two Dimensional ◽  
Ionic Radii ◽  
Coordination Solids ◽  
Self Assembling ◽  
Molecular Building Blocks ◽  
Metal Organic

Abstract Tessellation of self-assembling molecular building blocks is a promising strategy to design metal-organic materials exhibiting geometrical frustration and ensuing frustrated physical properties. Appearing in two-dimensional quasiperiodic phases, tilings consisting of five-vertex nodes are regarded as approximants for quasicrystals. Unfortunately, these structural motifs are exceedingly rare due to the complications of acquiring five-fold coordination confined to the plane. Lanthanide ions display the sufficient coordinative plasticity, and large ionic radii, to allow their incorporation into irregular molecule-based arrays. We herein present the use of ytterbium(II) as a five-vertex node in a two-dimensional coordination solid, YbI2(4,4′-bipyridine)2.5. The semi-regular Archimedean tessellation structure verges on quasicrystallinity and paves the way for lanthanide-based metal-organic materials with interesting photonic and magnetic properties.

A Molecular Artisans Guide to Supramolecular Coordination Complexes and Metal Organic Frameworks

2015 ◽  
Vol 03 (01n02) ◽  
pp. 1540004 ◽  
Author(s):  
Xialu Wu ◽  
David J. Young ◽  
T. S. Andy Hor
Keyword(s):  
Chemical Reactivity ◽  
Metal Organic Frameworks ◽  
Building Blocks ◽  
Coordination Complexes ◽  
Large Molecules ◽  
Molecular Building Blocks ◽  
Supramolecular Coordination ◽  
Metal Organic ◽  
Molecular Synthesis ◽  
And Function

As molecular synthesis advances, we are beginning to learn control of not only the chemical reactivity (and function) of molecules, but also of their interactions with other molecules. It is this basic idea that has led to the current explosion of supramolecular science and engineering. Parallel to this development, chemists have been actively pursuing the design of very large molecules using basic molecular building blocks. Herein, we review the general development of supramolecular chemistry and particularly of two new branches: supramolecular coordination complexes (SCCs) and metal organic frameworks (MOFs). These two fields are discussed in detail with typical examples to illustrate what is now possible and what challenges lie ahead for tomorrow's molecular artisans.

scholarly journals Inverse Design of Nanoporous Crystalline Reticular Materials with Deep Generative Models

2020 ◽  
Author(s):  
Zhenpeng Yao ◽  
Benjamin Sanchez-Lengeling ◽  
N. Scott Bobbitt ◽  
Benjamin J. Bucior ◽  
Sai Govind Hari Kumar ◽  
...  
Keyword(s):  
Self Assembly ◽  
Metal Organic Framework ◽  
Internal Surface ◽  
Building Blocks ◽  
Structural Features ◽  
Generative Models ◽  
Combinatorial Design ◽  
Surface Areas ◽  
Molecular Building Blocks ◽  
Metal Organic

Reticular frameworks are crystalline porous materials that form <i>via</i> the self-assembly of molecular building blocks (<i>i.e.</i>, nodes and linkers) in different topologies. Many of them have high internal surface areas and other desirable properties for gas storage, separation, and other applications. The notable variety of the possible building blocks and the diverse ways they can be assembled endow reticular frameworks with a near-infinite combinatorial design space, making reticular chemistry both promising and challenging for prospective materials design. Here, we propose an automated nanoporous materials discovery platform powered by a supramolecular variational autoencoder (SmVAE) for the generative design of reticular materials with desired functions. We demonstrate the automated design process with a class of metal-organic framework (MOF) structures and the goal of separating CO<sub>2</sub> from natural gas or flue gas. Our model exhibits high fidelity in capturing structural features and reconstructing MOF structures. We show that the autoencoder has a promising optimization capability when jointly trained with multiple top adsorbent candidates identified for superior gas separation. MOFs discovered here are strongly competitive against some of the best-performing MOFs/zeolites ever reported. This platform lays the groundwork for the design of reticular frameworks for desired applications.

scholarly journals Inverse Design of Nanoporous Crystalline Reticular Materials with Deep Generative Models

2020 ◽  
Author(s):  
Zhenpeng Yao ◽  
Benjamin Sanchez-Lengeling ◽  
N. Scott Bobbitt ◽  
Benjamin J. Bucior ◽  
Sai Govind Hari Kumar ◽  
...  
Keyword(s):  
Self Assembly ◽  
Metal Organic Framework ◽  
Internal Surface ◽  
Building Blocks ◽  
Structural Features ◽  
Generative Models ◽  
Combinatorial Design ◽  
Surface Areas ◽  
Molecular Building Blocks ◽  
Metal Organic

Reticular frameworks are crystalline porous materials that form <i>via</i> the self-assembly of molecular building blocks (<i>i.e.</i>, nodes and linkers) in different topologies. Many of them have high internal surface areas and other desirable properties for gas storage, separation, and other applications. The notable variety of the possible building blocks and the diverse ways they can be assembled endow reticular frameworks with a near-infinite combinatorial design space, making reticular chemistry both promising and challenging for prospective materials design. Here, we propose an automated nanoporous materials discovery platform powered by a supramolecular variational autoencoder (SmVAE) for the generative design of reticular materials with desired functions. We demonstrate the automated design process with a class of metal-organic framework (MOF) structures and the goal of separating CO<sub>2</sub> from natural gas or flue gas. Our model exhibits high fidelity in capturing structural features and reconstructing MOF structures. We show that the autoencoder has a promising optimization capability when jointly trained with multiple top adsorbent candidates identified for superior gas separation. MOFs discovered here are strongly competitive against some of the best-performing MOFs/zeolites ever reported. This platform lays the groundwork for the design of reticular frameworks for desired applications.

Stepwise Transformation of the Molecular Building Blocks in a Porphyrin-Encapsulating Metal–Organic Material

2013 ◽  
Vol 135 (16) ◽  
pp. 5982-5985 ◽  
Author(s):  
Zhenjie Zhang ◽  
Lukasz Wojtas ◽  
Mohamed Eddaoudi ◽  
Michael J. Zaworotko
Keyword(s):  
Organic Material ◽  
Building Blocks ◽  
Molecular Building Blocks ◽  
Metal Organic

Reticular Chemistry and Metal-Organic Frameworks for Clean Energy

MRS Bulletin ◽  
2009 ◽  
Vol 34 (9) ◽  
pp. 682-690 ◽  
Author(s):  
Omar M. Yaghi ◽  
Qiaowei Li
Keyword(s):  
Carbon Dioxide ◽  
Metal Organic Frameworks ◽  
Clean Energy ◽  
Building Blocks ◽  
Zeolitic Imidazolate Frameworks ◽  
Design Concepts ◽  
Surface Areas ◽  
Molecular Building Blocks ◽  
Metal Organic ◽  
Molecular Aspects

AbstractReticular chemistry concerns the linking of molecular building blocks into predetermined structures using strong bonds. We have been working on creating and developing the conceptual and practical basis of this new area of research. As a result, new classes of crystalline porous materials have been designed and synthesized: metal-organic frameworks, zeolitic imidazolate frameworks, and covalent organic frameworks. Crystals of this type have exceptional surface areas (2,000−6,000 m2/g) and take up voluminous amounts of hydrogen (7.5 wt% at 77 K and 3−4 × 106 Pa), methane (50 wt% at 298 K and 2.5 × 106 Pa), and carbon dioxide (140 wt% at 298 K and 3 × 106 Pa). We have driven the basic science all the way to applications without losing sight of our quest for understanding the underlying molecular aspects of this chemistry. The presentation was focused on the design concepts, synthesis, and structure of these materials, with emphasis on their applications to onboard energy storage.

Remote Stabilization of Copper Paddlewheel Based Molecular Building Blocks in Metal–Organic Frameworks

2015 ◽  
Vol 27 (6) ◽  
pp. 2144-2151 ◽  
Author(s):  
Wen-Yang Gao ◽  
Rong Cai ◽  
Tony Pham ◽  
Katherine A. Forrest ◽  
Adam Hogan ◽  
...  
Keyword(s):  
Metal Organic Frameworks ◽  
Building Blocks ◽  
Molecular Building Blocks ◽  
Metal Organic

Single Metal Ion Based Molecular Building Blocks (MBBs): Approach to the Design and Synthesis of Metal-Organic Assemblies

ChemInform ◽  
2007 ◽  
Vol 38 (4) ◽  
Author(s):  
Jacilynn A. Brant ◽  
Yunling Liu ◽  
Dorina F. Sava ◽  
Derek Beauchamp ◽  
Mohamed Eddaoudi
Keyword(s):  
Metal Ion ◽  
Building Blocks ◽  
Design And Synthesis ◽  
Molecular Building Blocks ◽  
Metal Organic ◽  
Organic Assemblies
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