De Novo Prediction of Inorganic Structures Developed through Automated Assembly of Secondary Building Units (AASBU Method)

Draznieks, Caroline Mellot; Newsam, J. M.; Gorman, A. M.; Freeman, C. M.; Férey, Gérard

doi:10.1002/1521-3773(20000703)39:13<2270::aid-anie2270>3.0.co;2-a

Cited by 187 publications

(107 citation statements)

References 16 publications

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“…Existing prediction methods focus on simulation of the selfassembly process, placing known SBUs into candidate periodic networks. [14][15][16] A limitation of these methods is that only pre-existing linkers are considered, with little or no exploration of the space of possible organic linkers.…”

Section: Introductionmentioning

confidence: 99%

In Silico Discovery of High Deliverable Capacity Metal–Organic Frameworks

Bao¹,

Martin

Simon

et al. 2014

J. Phys. Chem. C

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Metal organic frameworks (MOFs) are actively being explored as potential adsorbed natural gas storage materials for small vehicles. Experimental exploration of potential materials is limited by the throughput of synthetic chemistry. We here describe a computational methodology to complement and guide these experimental efforts. The method uses known chemical transformations in silico to identify MOFs with high methane deliverable capacity. The procedure explicitly considers synthesizability with geometric requirements on organic linkers. We efficiently search the composition and conformation space of organic linkers for nine MOF networks, finding 48 materials with higher predicted deliverable capacity (at 65 bar storage, 5.8 bar depletion, and 298 K) than MOF-5 in four of the nine networks. The best material has a predicted deliverable capacity 8% higher than that of MOF-5.

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Section: Introductionmentioning

confidence: 99%

In Silico Discovery of High Deliverable Capacity Metal–Organic Frameworks

Bao¹,

Martin

Simon

et al. 2014

J. Phys. Chem. C

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“…Scientists have successfully synthesized many new materials and studied their properties, but the purely experimental approach is no longer the only route to discover new compounds. The theoretical prediction of new compounds and new (meta)-stable modifications of already existing solids followed by their synthesis is fast becoming an alternative [1][2][3][4][5][6][7][8][9][10].…”

Section: Introductionmentioning

confidence: 99%

Structure Prediction for PbS and ZnO at Different Pressures and Visualization of the Energy Landscapes

et al. 2011

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An important issue in modern solid state chemistry is the development of a general methodology to predict the possible (meta)-stable modifications of a solid. This requires the global exploration of the energy landscape of the chemical system, since each stable phase corresponds to a locally ergodic region of the landscape. The global search in the lead sulfide system has been performed with simulated annealing on the ab initio level, while zinc oxide was studied with an empirical potential using simulated annealing, both at standard and elevated pressure (up to 100 GPa). The local optimization of the modifications found in the PbS system was performed using various density functionals. Next, the energy E(V ) and enthalpy H(p) as function of volume and pressure, respectively, were computed for these modifications and their electronic structure was analyzed. The structures found for ZnO were locally optimized on ab initio level (DFT and Hartree-Fock). In both systems the structures found were in good agreement with the experiment. Furthermore, we employed the threshold algorithm to explore the barrier structure of the landscape of ZnO as function of the number of formula units in the simulation cell. Based on the barrier and minima information 2-D models of the energy landscape were constructed.

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“…Such an approach started with close-packed compounds [45]; the greatest progress may be registered among molecular crystals [46]. Learning from crystal structure prediction done, not by ab initio calculations, but by exploiting known topologies and known building units of related crystals, led to the greatest success among framework materials [47][48][49][50].…”

Section: Pattern Modelling Methods Assisted By Ab Initio Calculationsmentioning

confidence: 99%

Crystal Structures from Powder Diffraction: Principles, Difficulties and Progress

Černý

2017

Crystals

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Abstract:The structure solution from powder diffraction has undergone an intense evolution during the last 20 years, but is far from being routine. Current challenges of powder crystallography include ab initio crystal structure determination on real samples of new materials with specific microstructures, characterization of intermediate reaction products from in situ, in operando studies and novel phases from in situ studies of phase diagrams. The intense evolution of electron diffraction in recent years, providing an experimental (precession) and theoretical (still under intense development) solution to strong dynamic scattering of electrons, smears the traditional frontier between poly-and single-crystal diffraction. Novel techniques like serial snapshot X-ray crystallography point in the same direction. Finally, for the computational chemistry, theoreticians hand-in-hand with crystallographers develop tools where the theory meets experiment for crystal structure refinement, which becomes an unavoidable step in the validation of crystal structures obtained from powder diffraction.Keywords: powder diffraction; structure solution; X-ray diffraction; DFT calculations; electron diffraction The structure solution means in this article determination of the (average) 3D-periodic arrangement of the atoms in the crystal using mainly the information content of Bragg scattering in the diffraction pattern. The case of aperiodic crystals (modulated and quasicrystals), of short-range order (diffuse scattering), as well as of nano-crystals (crystals without measurable Bragg signals) will not be discussed here. The structure prediction, on the other hand, will be used in the sense of the determination of the 3D arrangement of the atoms in the crystal using mainly first-principle calculations, and any experimental observation, like the diffraction pattern, is used only for the validation of the predicted structural model. Indexing: Still a BottleneckDespite an intense development of indexing algorithms in the last 20 years, the detection of the correct lattice may still be a bottleneck of the structure solution in the case of low resolution powder patterns or in the case of monoclinic and triclinic symmetry. A review of known indexing algorithms may be found in Chapter 7 of [3], Chapter 5 of [6] and Chapter 7 of [7]. Each crystallographer and each crystal may work better with a particular algorithm, but as is said in another excellent indexing The advantage of the dichotomy algorithm is its speed (especially in Fox) and its robustness towards low data quality. Indexing is followed by space group determination, which is based on systematic extinction analysis supported by the knowledge of crystal physical properties, like piezoelectricity, the presence of which excludes centrosymmetric space groups. Fairly robust algorithms for space group determination are based on full pattern fitting (Le Bail or Pawley), available in most software packages. The indexing can be quite difficult for the crystals lying on opposite ends of the s...

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De Novo Prediction of Inorganic Structures Developed through Automated Assembly of Secondary Building Units (AASBU Method)

Cited by 187 publications

References 16 publications

In Silico Discovery of High Deliverable Capacity Metal–Organic Frameworks

In Silico Discovery of High Deliverable Capacity Metal–Organic Frameworks

Structure Prediction for PbS and ZnO at Different Pressures and Visualization of the Energy Landscapes

Crystal Structures from Powder Diffraction: Principles, Difficulties and Progress

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