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Modulating proton diffusion and conductivity in metal-organic frameworks by incorporation of accessible free carboxylic acid groups

DOI: 10.1039/C8SC03022G DOI Help

Authors: Peter Rought (University of Manchester) , Christopher Marsh (University of Manchester) , Simona Pili (University of Manchester) , Ian P. Silverwood (University College London (UCL)) , Victoria Garcia Sakai (ISIS Pulsed Neutron and Muon Source) , Ming Li (University of Nottingham) , Martyn Brown (University of Manchester) , Stephen P. Argent (University of Warwick) , Inigo Vitorica-yrezabal (University of Manchester) , George Whitehead (University of Manchester) , Mark R. Warren (Diamond Light Source) , Sihai Yang (University of Manchester) , Martin Schroeder (University of Manchester)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Chemical Science

State: Published (Approved)
Published: November 2018
Diamond Proposal Number(s): 13650 , 12517

Open Access Open Access

Abstract: Three multi-carboxylic acid functionalised ligands have been designed, synthesised and utilised to synthesise the new barium-based MOFs, MFM-510, -511, and -512, which show excellent stability to water-vapour. MFM-510 and MFM-511 show moderate proton conductivities (2.1 x10-5 and 5.1 x10-5 S cm-1, respectively) at 99RH% and 298 K, attributed to the lack of free protons or hindered proton diffusion within the framework structures. In contrast, MFM-512, which incorporates a pendant carboxylic acid group directed into the pore of the framework, shows a two orders of magnitude enhancement in proton conductivity (2.9 x10-3 S cm-1). Quasi-elastic neutron scattering (QENS) suggests that the proton dynamics of MFM-512 are mediated by “free diffusion inside a sphere” confirming that incorporation of free carboxylic acid groups within the pores of MOFs is an efficient albeit a synthetically challenging strategy to improve proton conductivity.

Subject Areas: Chemistry, Materials


Instruments: I19-Small Molecule Single Crystal Diffraction

Other Facilities: ISIS

Documents:
c8sc03022g.pdf