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Pressure-induced amorphization of a dense coordination polymer and its impact on proton conductivity
12.V. V. Sinitsyn, E. G. Ponyatovskii, A. I. Baranov, A. V. Tregubchenko, L. A. Shuvalov, and J. G. Adashko, Sov. Phys.-JETP 73, 386 (1991).
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14.J.-C. Tan, B. Civalleri, C.-C. Lin, L. Valenzano, R. Galvelis, P.-F. Chen, T. D. Bennett, C. Mellot-Draznieks, C. M. Zicovich-Wilson, and A. K. Cheetham, Phys. Rev. Lett. 108, 095502 (2012).
See supplementary material at http://dx.doi.org/10.1063/1.4898806
for high-pressure cell assemblies used for impedance measurement and synchrotron X-ray study, and PXRD of 1 measured before and after 7 GPa pressing with the DIA-type cubic-anvil high-pressure apparatus.[Supplementary Material]
20.Although we could not confirm the reversibility in situ (i.e., the Bragg peaks of 1 was not observed again after the pressure was released), we relied on the results shown in Figs. 2(b) and S2 to conclude that the crystalline-to-amorphous transition of 1 is essentially reversible. We are not certain why the reversibility was not observed in the in situ X-ray measurements; however, plausible reasons include the pressure-hysteresis effect. Alternatively, the effect may become irreversible at pressures over a certain pressure (e.g., at pressures over 7 GPa), as is the case reported in Ref. 28.
24.N. Kamaya, K. Homma, Y. Yamakawa, M. Hirayama, R. Kanno, M. Yonemura, T. Kamiyama, Y. Kato, S. Hama, K. Kawamoto, and A. Mitsui, Nat. Mater. 10, 682 (2011).
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conductivity of a dense coordination polymer (CP) was investigated under high-pressure conditions. Impedance measurements under high pressures revealed that the proton
conductivity of the CP decreased more than 1000-fold at pressures of 3–7 GPa and that the activation energy for proton
conduction almost doubled compared with that at ambient pressure. A synchrotron X-ray study under high pressure identified the amorphization process of the CP during compression, which rationally explains the decrease in conductivity and increase in activation energy. This phenomenon is categorized as reversible pressure-induced amorphization of a dense CP and is regarded as a demonstration of the coupling of the mechanical and electrical properties of a CP.
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