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具有分级孔隙率的二氧化硅中吸附诱导变形的原位小角中子散射研究

In Situ Small-Angle Neutron Scattering Investigation of Adsorption-Induced Deformation in Silica with Hierarchical Porosity.

作者信息

Ludescher Lukas, Morak Roland, Balzer Christian, Waag Anna M, Braxmeier Stephan, Putz Florian, Busch Sebastian, Gor Gennady Y, Neimark Alexander V, Hüsing Nicola, Reichenauer Gudrun, Paris Oskar

机构信息

Institute of Physics , Montanuniversitaet Leoben , Franz-Josef-Str. 18 , 8700 Leoben , Austria.

Bavarian Center for Applied Energy Research , Magdalene-Schoch-Str. 3 , 97074 Wuerzburg , Germany.

出版信息

Langmuir. 2019 Sep 3;35(35):11590-11600. doi: 10.1021/acs.langmuir.9b01375. Epub 2019 Aug 22.

Abstract

Adsorption-induced deformation of a series of silica samples with hierarchical porosity has been studied by in situ small-angle neutron scattering (SANS) and in situ dilatometry. Monolithic samples consisted of a disordered macroporous network of struts formed by a 2D lattice of hexagonally ordered cylindrical mesopores and disordered micropores within the mesopore walls. Strain isotherms were obtained at the mesopore level by analyzing the shift of the Bragg reflections from the ordered mesopore lattice in SANS data. Thus, SANS essentially measured the radial strain of the cylindrical mesopores including the volume changes of the mesopore walls due to micropore deformation. A HO/DO adsorbate with net zero coherent neutron scattering length density was employed in order to avoid apparent strain effects due to intensity changes during pore filling. In contrast to SANS, the strain isotherms obtained from in situ dilatometry result from a combination of axial and radial mesopore deformation together with micropore deformation. Strain data were quantitatively analyzed with a theoretical model for micro-/mesopore deformation by combining information from nitrogen and water adsorption isotherms to estimate the water-silica interaction. It was shown that in situ SANS provides complementary information to dilatometry and allows for a quantitative estimate of the elastic properties of the mesopore walls from water adsorption.

摘要

通过原位小角中子散射(SANS)和原位膨胀测量法研究了一系列具有分级孔隙率的二氧化硅样品的吸附诱导变形。整体样品由由六方有序圆柱形介孔的二维晶格形成的无序支柱大孔网络和介孔壁内的无序微孔组成。通过分析SANS数据中来自有序介孔晶格的布拉格反射的位移,在介孔水平获得应变等温线。因此,SANS基本上测量了圆柱形介孔的径向应变,包括由于微孔变形导致的介孔壁的体积变化。为了避免由于孔隙填充过程中的强度变化而产生的明显应变效应,使用了具有净零相干中子散射长度密度的HO/DO吸附质。与SANS不同,原位膨胀测量法获得的应变等温线是轴向和径向介孔变形以及微孔变形共同作用的结果。通过结合来自氮气和水吸附等温线的信息,用微/介孔变形的理论模型对应变数据进行了定量分析,以估计水-二氧化硅相互作用。结果表明,原位SANS为膨胀测量法提供了补充信息,并允许从水吸附定量估计介孔壁的弹性性质。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/d75f/6733155/d186215d54fd/la9b01375_0001.jpg

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