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      Zero-strain reductive intercalation in a molecular framework†

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          Abstract

          Intercalation of potassium into the molecular framework silver hexacyanoferrate occurs with remarkably small volume strain.

          Abstract

          Reductive intercalation of potassium within the molecular framework Ag 3[Fe(CN) 6] gives rise to a volume strain that is an order of magnitude smaller than is typical for common ion-storage materials. We suggest that framework flexibility might be exploited as a general strategy for reducing cycling strain in battery and ion-storage materials.

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          Rapid planetesimal formation in turbulent circumstellar discs

          Anders Johansen, Jeffrey S. Oishi, Mordecai-Mark Mac Low … (2007)
          The initial stages of planet formation in circumstellar gas discs proceed via dust grains that collide and build up larger and larger bodies (Safronov 1969). How this process continues from metre-sized boulders to kilometre-scale planetesimals is a major unsolved problem (Dominik et al. 2007): boulders stick together poorly (Benz 2000), and spiral into the protostar in a few hundred orbits due to a head wind from the slower rotating gas (Weidenschilling 1977). Gravitational collapse of the solid component has been suggested to overcome this barrier (Safronov 1969, Goldreich & Ward 1973, Youdin & Shu 2002). Even low levels of turbulence, however, inhibit sedimentation of solids to a sufficiently dense midplane layer (Weidenschilling & Cuzzi 1993, Dominik et al. 2007), but turbulence must be present to explain observed gas accretion in protostellar discs (Hartmann 1998). Here we report the discovery of efficient gravitational collapse of boulders in locally overdense regions in the midplane. The boulders concentrate initially in transient high pressures in the turbulent gas (Johansen, Klahr, & Henning 2006), and these concentrations are augmented a further order of magnitude by a streaming instability (Youdin & Goodman 2005, Johansen, Henning, & Klahr 2006, Johansen & Youdin 2007) driven by the relative flow of gas and solids. We find that gravitationally bound clusters form with masses comparable to dwarf planets and containing a distribution of boulder sizes. Gravitational collapse happens much faster than radial drift, offering a possible path to planetesimal formation in accreting circumstellar discs.
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            High-performance lithium-ion anodes using a hierarchical bottom-up approach.

            A Magasinski, P. Dixon, B. Hertzberg … (2010)
            Si-based Li-ion battery anodes have recently received great attention, as they offer specific capacity an order of magnitude beyond that of conventional graphite. The applications of this transformative technology require synthesis routes capable of producing safe and easy-to-handle anode particles with low volume changes and stable performance during battery operation. Herein, we report a large-scale hierarchical bottom-up assembly route for the formation of Si on the nanoscale--containing rigid and robust spheres with irregular channels for rapid access of Li ions into the particle bulk. Large Si volume changes on Li insertion and extraction are accommodated by the particle's internal porosity. Reversible capacities over five times higher than that of the state-of-the-art anodes (1,950 mA h g(-1)) and stable performance are attained. The synthesis process is simple, low-cost, safe and broadly applicable, providing new avenues for the rational engineering of electrode materials with enhanced conductivity and power.
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              Versatile Photocatalytic Systems for H2 Generation in Water Based on an Efficient DuBois-Type Nickel Catalyst

              Manuela Groß, Anna Reynal, James R. Durrant … (2013)
              The generation of renewable H2 through an efficient photochemical route requires photoinduced electron transfer (ET) from a light harvester to an efficient electrocatalyst in water. Here, we report on a molecular H2 evolution catalyst (NiP) with a DuBois-type [Ni(P2 R′N2 R″)2]2+ core (P2 R′N2 R″ = bis(1,5-R′-diphospha-3,7-R″-diazacyclooctane), which contains an outer coordination sphere with phosphonic acid groups. The latter functionality allows for good solubility in water and immobilization on metal oxide semiconductors. Electrochemical studies confirm that NiP is a highly active electrocatalyst in aqueous electrolyte solution (overpotential of approximately 200 mV at pH 4.5 with a Faradaic yield of 85 ± 4%). Photocatalytic experiments and investigations on the ET kinetics were carried out in combination with a phosphonated Ru(II) tris(bipyridine) dye (RuP) in homogeneous and heterogeneous environments. Time-resolved luminescence and transient absorption spectroscopy studies confirmed that directed ET from RuP to NiP occurs efficiently in all systems on the nano- to microsecond time scale, through three distinct routes: reductive quenching of RuP in solution or on the surface of ZrO2 (“on particle” system) or oxidative quenching of RuP when the compounds were immobilized on TiO2 (“through particle” system). Our studies show that NiP can be used in a purely aqueous solution and on a semiconductor surface with a high degree of versatility. A high TOF of 460 ± 60 h–1 with a TON of 723 ± 171 for photocatalytic H2 generation with a molecular Ni catalyst in water and a photon-to-H2 quantum yield of approximately 10% were achieved for the homogeneous system.
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                Author and article information

                Journal
                Journal ID (nlm-ta): CrystEngComm
                Journal ID (iso-abbrev): CrystEngComm
                Title: Crystengcomm / Rsc
                Publisher: Royal Society of Chemistry
                ISSN (Electronic): 1466-8033
                Publication date (Print): 21 April 2015
                Publication date (Electronic): 16 January 2015
                Volume: 17
                Issue: 15
                Pages: 2925-2928
                Affiliations
                [a ] Department of Chemistry , University of Oxford , Inorganic Chemistry Laboratory , South Parks Road , Oxford , OX1 3QR , UK . Email: andrew.goodwin@ 123456chem.ox.ac.uk ; Fax: +44 (0)1865 274690 ; Tel: +44 (0)1865 272137
                Article
                Publisher ID: c4ce02364a
                DOI: 10.1039/c4ce02364a
                PMC ID: 4396389
                SO-VID: 73b978af-7373-4e70-a76f-168f42816c19
                Copyright © This journal is © The Royal Society of Chemistry 2015
                License:

                This is an Open Access article distributed under the terms of the Creative Commons Attribution Non-Commercial License ( http://creativecommons.org/licenses/by-nc/2.0/uk/) which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited.

                History
                Date received : 29 November 2014
                Date accepted : 22 December 2014
                Categories
                Subject: Chemistry

                Notes

                †Electronic supplementary information (ESI) available: Synthesis, experimental methods, and sample characterisation; X-ray powder diffraction refinement details. See DOI: 10.1039/c4ce02364a


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