Chen Jin, Mei Qingqing, Chen Yinlin, Marsh Christopher, An Bing, Han Xue, Silverwood Ian P, Li Ming, Cheng Yongqiang, He Meng, Chen Xi, Li Weiyao, Kippax-Jones Meredydd, Crawshaw Danielle, Frogley Mark D, Day Sarah J, García-Sakai Victoria, Manuel Pascal, Ramirez-Cuesta Anibal J, Yang Sihai, Schröder Martin
Department of Chemistry, The University of Manchester, Manchester M13 9PL, United Kingdom.
ISIS Neutron and Muon Source, Rutherford Appleton Laboratory, Didcot OX11 0QX, United Kingdom.
J Am Chem Soc. 2022 Jul 13;144(27):11969-11974. doi: 10.1021/jacs.2c04900. Epub 2022 Jul 1.
The development of materials showing rapid proton conduction with a low activation energy and stable performance over a wide temperature range is an important and challenging line of research. Here, we report confinement of sulfuric acid within porous MFM-300(Cr) to give MFM-300(Cr)·SO(HO), which exhibits a record-low activation energy of 0.04 eV, resulting in stable proton conductivity between 25 and 80 °C of >10 S cm. synchrotron X-ray powder diffraction (SXPD), neutron powder diffraction (NPD), quasielastic neutron scattering (QENS), and molecular dynamics (MD) simulation reveal the pathways of proton transport and the molecular mechanism of proton diffusion within the pores. Confined sulfuric acid species together with adsorbed water molecules play a critical role in promoting the proton transfer through this robust network to afford a material in which proton conductivity is almost temperature-independent.
开发出在较宽温度范围内具有低活化能且质子传导迅速、性能稳定的材料是一项重要且具有挑战性的研究方向。在此，我们报道了将硫酸限制在多孔MFM-300(Cr)中得到MFM-300(Cr)·SO(HO)，其展现出创纪录的0.04 eV低活化能，在25至80°C之间实现了大于10 S cm的稳定质子传导率。同步加速器X射线粉末衍射（SXPD）、中子粉末衍射（NPD）、准弹性中子散射（QENS）以及分子动力学（MD）模拟揭示了质子传输路径以及孔内质子扩散的分子机制。受限的硫酸物种与吸附的水分子在促进质子通过这个坚固网络进行转移方面起着关键作用，从而得到一种质子传导率几乎与温度无关的材料。
