Computationally Assisted Identification of Functional Inorganic Materials

Dyer, Matthew S.; Collins, Christopher M.; Hodgeman, Darren; Chater, Philip A.; Demont, Antoine; Romani, S.; Sayers, Ruth; Thomas, Michael F.; Claridge, John B.; Darling, George R.; Rosseinsky, Matthew J.

doi:10.1126/science.1226558

Cited by 65 publications

(66 citation statements)

References 44 publications

(7 reference statements)

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“…Moreover, the recent huge progress in computer science has made it possible to use computational calculations and simulations as powerful research tools in chemistry and materials science areas including materials discovery, mechanistic studies, etc. Particular attention should be paid to crystal structure prediction techniques, which will be of great benefit for the discovery of new COMs based on old macrocycles. In addition, molecular simulations may also be helpful to better understand the structure–function relationships in macrocycle‐based COMs and give inspirations about structural design toward task‐specific applications .…”

Section: Resultsmentioning

confidence: 99%

Supramolecular‐Macrocycle‐Based Crystalline Organic Materials

et al. 2019

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macrocycles. They have been also employed to modify the surface properties of metal nanoparticles via noncovalent host−guest interactions, [31] covering their applications in drug delivery, [32] highly sensitive sensors, [33] selective catalysis, [34] and so on.In addition to their intensive applications based on their host−guest chemistry, macrocycles have also been used as building blocks to construct solid materials including porous organic polymers (POPs), [35,36] metal-organic frameworks (MOFs), [37][38][39][40][41][42][43] and crystalline organic materials (COMs). [44][45][46][47][48][49][50][51][52][53][54][55][56][57] Particular attention should be paid to COMs, a class of organic materials featuring facile preparation, high crystallinity, structural diversity, chemical stability, solution-processability, etc. [58][59][60][61][62][63][64][65][66][67][68][69][70] Different from MOFs that are composed of both inorganic (metal ions) and organic species (organic ligands) through coordination, COMs refer to a kind of crystalline materials composed of pure organics connected by either covalent or noncovalent bonds. [71][72][73] For COMs connected by noncovalent bonds, the typical materials are organic molecular crystals with intriguing properties such as semiconductor, [53] porosity, [68] etc. Owing to the inefficient packing of organic building blocks in the crystal state, some molecular crystals display extrinsic porosity, which are often termed as hydrogen-bonded organic frameworks (HOFs) [74,75] or supramolecular organic frameworks (SOFs). [76][77][78][79][80] For COMs connected by covalent bonds, typical materials are crystalline covalent organic frameworks (COFs), which were firstly reported in 2005 by Yaghi and co-workers [44] Benefitting from rigid chemical bonds and building blocks, COFs show permanent and well-ordered porosity. [45][46][47][48] Supramolecular-macrocycle-based COMs, a class of COMs with macrocycles as the main building blocks, have drawn particular attention in recent years. According to their components, supramolecular-macrocycle-based COMs can be classified into two main categories, the ones composed of pure macrocycles and the others consisting of macrocycles and other simple organic building blocks. Owing to their prefabricated cavities of a certain type, some of macrocycle-based COMs exhibit intrinsic microporosity for guest adsorption in the solid state. On the other hand, the extrinsic porosity of some macrocyclebased COMs may form due to the inefficient packing of these rigid macrocyclic molecules in the crystalline state. In certain circumstances, both intrinsic and extrinsic microporosity can be created in a single lattice of a certain COM, thus leading to Supramolecular macrocycles are well known as guest receptors in supramolecular chemistry, especially host−guest chemistry. In addition to their wide applications in host−guest chemistry and related areas, macrocycles have also been employed to construct crystalline organic materials (COMs) owing to their particular structur...

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Section: Resultsmentioning

confidence: 99%

Supramolecular‐Macrocycle‐Based Crystalline Organic Materials

et al. 2019

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“…By contrast, most MOFs, COFs, and polymers are prepared from smaller building blocks, which increases computational expense for unconstrained structure-composition searches. It is possible that a strategy of "extended modules," as used to predict function for inorganic oxides (126), might also be adapted to porous framework solids so that the structure and function of complex materials could be predicted in a more granular way.…”

Section: De Novo Computational Designmentioning

confidence: 99%

Function-led design of new porous materials

Slater

Cooper

2015

Science

1,378

918

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Porous solids are important as membranes, adsorbents, catalysts, and in other chemical applications. But for these materials to find greater use at an industrial scale, it is necessary to optimize multiple functions in addition to pore structure and surface area, such as stability, sorption kinetics, processability, mechanical properties, and thermal properties. Several different classes of porous solids exist, and there is no one-size-fits-all solution; it can therefore be challenging to choose the right type of porous material for a given job. Computational prediction of structure and properties has growing potential to complement experiment to identify the best porous materials for specific applications.

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“…Solid-state synthesis is slow, resulting from relatively long diffusion distances (typically on the order of the particle size of the raw materials) and often suffers from the formation of recalcitrant intermediate phases which are difficult to eliminate in a single or two-step heat treatment. 10 This diffusionlimited compositional heterogeneity can also lead to local variations in functional properties 11 and in many cases the formation of core-shell structures 12 which may or may not be desirable, depending on the target application. Solid-state synthesis also offers little in the way of size or morphological control in the final product.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of Barium Titanate Using Deep Eutectic Solvents

et al. 2016

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Novel synthetic routes to prepare functional oxides at lower temperatures are an increasingly important area of research. Many of these synthetic routes, however, use water as the solvent and rely on dissolution of the precursors, precluding their use with, for example, titanates. Here we present a low cost solvent system as a means to rapidly create phase-pure ferroelectric barium titanate using a choline chloride-malonic acid deep eutectic solvent. This solvent is compatible with alkoxide precursors and allows for the rapid synthesis of nanoscale barium titanate powders at 950 °C. The phase and morphology were determined, along with investigation of the synthetic pathway, with the reaction proceeding via BaCl2 and TiO2 intermediates. The powders were also used to create sintered ceramics, which exhibit a permittivity maximum corresponding to a tetragonal-cubic transition at 112 °C, as opposed to the more conventional temperature of ~ 120 °C. The lower-thanexpected value for the ferro-to para-electric phase transition is likely due to undetectable levels of contaminants.

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Computationally Assisted Identification of Functional Inorganic Materials

Cited by 65 publications

References 44 publications

Supramolecular‐Macrocycle‐Based Crystalline Organic Materials

Supramolecular‐Macrocycle‐Based Crystalline Organic Materials

Function-led design of new porous materials

Synthesis of Barium Titanate Using Deep Eutectic Solvents

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