Michael E. Briggs

Bio: Michael E. Briggs is an academic researcher from University of Liverpool. The author has contributed to research in topics: Crystal structure prediction & Microporous material. The author has an hindex of 25, co-authored 50 publications receiving 2346 citations. Previous affiliations of Michael E. Briggs include École Polytechnique & Centre national de la recherche scientifique.

Separation of rare gases and chiral molecules by selective binding in porous organic cages

Abstract: The separation of molecules with similar size and shape is an important technological challenge. For example, rare gases can pose either an economic opportunity or an environmental hazard and there is a need to separate these spherical molecules selectively at low concentrations in air. Likewise, chiral molecules are important building blocks for pharmaceuticals, but chiral enantiomers, by definition, have identical size and shape, and their separation can be challenging. Here we show that a porous organic cage molecule has unprecedented performance in the solid state for the separation of rare gases, such as krypton and xenon. The selectivity arises from a precise size match between the rare gas and the organic cage cavity, as predicted by molecular simulations. Breakthrough experiments demonstrate real practical potential for the separation of krypton, xenon and radon from air at concentrations of only a few parts per million. We also demonstrate selective binding of chiral organic molecules such as 1-phenylethanol, suggesting applications in enantioselective separation.

Hyperporous Carbons from Hypercrosslinked Polymers.

Abstract: Porous carbons with extremely high surface areas are produced through the carbonization of hypercrosslinked benzene, pyrrole, and thiophene. Such carbons show largely microporous and mesoporous domains and exhibit Brunaeur-Emmett-Teller surface areas up to 4300 m(2) g(-1) . The best performing material also displays exceptionally high CO2 and H2 uptakes.

Porous Organic Cages for Gas Chromatography Separations

Abstract: compounds 13 and to separate both krypton/xenon mixtures and chiral alcohols. 14 Here, we show that CC3 can also be used as a chromatographic stationary phase by coating it inside a standard capillary column. We show that such columns can be used for the GC separation of a range of mixtures including aromatic compounds, racemic mixtures, and branched alkanes. Homochiral CC3-R was produced by a one-pot imine condensation of 1,3,5-triformylbenzene with (R,R)-1,2-cyclohexanediamine, catalyzed by trifluoroacetic acid (Scheme 1). CC3-R has tetrahedral symmetry and includes four windows that are large enough to be penetrated by small molecules such as gases, 10 iodine, 15 or common organic solvents. 16 In the solid state, CC3-R packs window-to-window, resulting in a 3-D interconnected pore structure that runs through the center of each cage. This leads to high levels of permanent microporosity in the crystals after desolvation, with apparent BrunauerEmmett-Teller surface areas (SABET) of up to 800 m 2 g −1 , depending on the level of crystallinity. 17 A distinguishing

Supramolecular engineering of intrinsic and extrinsic porosity in covalent organic cages.

Abstract: Control over pore size, shape, and connectivity in synthetic porous materials is important in applications such as separation, storage, and catalysis. Crystalline organic cage molecules can exhibit permanent porosity, but there are few synthetic methods to control the crystal packing and hence the pore connectivity. Typically, porosity is either ‘intrinsic’ (within the molecules) or ‘extrinsic’ (between the molecules)—but not both. We report a supramolecular approach to the assembly of porous organic cages which involves bulky directing groups that frustrate the crystal packing. This generates, in a synthetically designed fashion, additional ‘extrinsic’ porosity between the intrinsically porous cage units. One of the molecular crystals exhibits an apparent Brunauer–Emmett–Teller surface area of 854 m2 g–1, which is higher than that of unfunctionalized cages of the same dimensions. Moreover, connectivity between pores, and hence guest uptakes, can be modulated by the introduction of halogen bonding motifs ...

Fast parallel algorithms for short-range molecular dynamics

Abstract: Three parallel algorithms for classical molecular dynamics are presented. The first assigns each processor a fixed subset of atoms; the second assigns each a fixed subset of inter-atomic forces to compute; the third assigns each a fixed spatial region. The algorithms are suitable for molecular dynamics models which can be difficult to parallelize efficiently—those with short-range forces where the neighbors of each atom change rapidly. They can be implemented on any distributed-memory parallel machine which allows for message-passing of data between independently executing processors. The algorithms are tested on a standard Lennard-Jones benchmark problem for system sizes ranging from 500 to 100,000,000 atoms on several parallel supercomputers--the nCUBE 2, Intel iPSC/860 and Paragon, and Cray T3D. Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems. For large problems, the spatial algorithm achieves parallel efficiencies of 90% and a 1840-node Intel Paragon performs up to 165 faster than a single Cray C9O processor. Trade-offs between the three algorithms and guidelines for adapting them to more complex molecular dynamics simulations are also discussed.

Ultracapacitors: Why, How, and Where is the Technology

Abstract: The science and technology of ultracapacitors are reviewed for a number of electrode materials, including carbon, mixed metal oxides, and conducting polymers. More work has been done using microporous carbons than with the other materials and most of the commercially available devices use carbon electrodes and an organic electrolytes. The energy density of these devices is 3¯5 Wh/kg with a power density of 300¯500 W/kg for high efficiency (90¯95%) charge/discharges. Projections of future developments using carbon indicate that energy densities of 10 Wh/kg or higher are likely with power densities of 1¯2 kW/kg. A key problem in the fabrication of these advanced devices is the bonding of the thin electrodes to a current collector such the contact resistance is less than 0.1 cm2. Special attention is given in the paper to comparing the power density characteristics of ultracapacitors and batteries. The comparisons should be made at the same charge/discharge efficiency.

Stable Metal-Organic Frameworks: Design, Synthesis, and Applications.

Abstract: Metal-organic frameworks (MOFs) are an emerging class of porous materials with potential applications in gas storage, separations, catalysis, and chemical sensing. Despite numerous advantages, applications of many MOFs are ultimately limited by their stability under harsh conditions. Herein, the recent advances in the field of stable MOFs, covering the fundamental mechanisms of MOF stability, design, and synthesis of stable MOF architectures, and their latest applications are reviewed. First, key factors that affect MOF stability under certain chemical environments are introduced to guide the design of robust structures. This is followed by a short review of synthetic strategies of stable MOFs including modulated synthesis and postsynthetic modifications. Based on the fundamentals of MOF stability, stable MOFs are classified into two categories: high-valency metal-carboxylate frameworks and low-valency metal-azolate frameworks. Along this line, some representative stable MOFs are introduced, their structures are described, and their properties are briefly discussed. The expanded applications of stable MOFs in Lewis/Bronsted acid catalysis, redox catalysis, photocatalysis, electrocatalysis, gas storage, and sensing are highlighted. Overall, this review is expected to guide the design of stable MOFs by providing insights into existing structures, which could lead to the discovery and development of more advanced functional materials.

Zr-based metal-organic frameworks: design, synthesis, structure, and applications.

Abstract: Among the large family of metal–organic frameworks (MOFs), Zr-based MOFs, which exhibit rich structure types, outstanding stability, intriguing properties and functions, are foreseen as one of the most promising MOF materials for practical applications. Although this specific type of MOF is still in its early stage of development, significant progress has been made in recent years. Herein, advances in Zr-MOFs since 2008 are summarized and reviewed from three aspects: design and synthesis, structure, and applications. Four synthesis strategies implemented in building and/or modifying Zr-MOFs as well as their scale-up preparation under green and industrially feasible conditions are illustrated first. Zr-MOFs with various structural types are then classified and discussed in terms of different Zr-based secondary building units and organic ligands. Finally, applications of Zr-MOFs in catalysis, molecule adsorption and separation, drug delivery, and fluorescence sensing, and as porous carriers are highlighted. Such a review based on a specific type of MOF is expected to provide guidance for the in-depth investigation of MOFs towards practical applications.

Chemical, thermal and mechanical stabilities of metal–organic frameworks

Abstract: The construction of thousands of well-defined, porous, metal–organic framework (MOF) structures, spanning a broad range of topologies and an even broader range of pore sizes and chemical functionalities, has fuelled the exploration of many applications. Accompanying this applied focus has been a recognition of the need to engender MOFs with mechanical, thermal and/or chemical stability. Chemical stability in acidic, basic and neutral aqueous solutions is important. Advances over recent years have made it possible to design MOFs that possess different combinations of mechanical, thermal and chemical stability. Here, we review these advances and the associated design principles and synthesis strategies. We focus on how these advances may render MOFs effective as heterogeneous catalysts, both in chemically harsh condensed phases and in thermally challenging conditions relevant to gas-phase reactions. Finally, we briefly discuss future directions of study for the production of highly stable MOFs. Metal–organic frameworks (MOFs) have shown promise in a broad range of applications, including catalysis. In this Review, the chemical, thermal and mechanical stabilities of MOFs, in particular with catalytic uses in mind, are discussed.