Preparation of Bimodal Mesoporous Silica Molecular Sieves from Organotrialkoxysilane and Tetraethoxysilane

The synthesis of silica with bimodal, disordered mesopores structure, by template-mediated sol-gel processing and subsequent heat-treatment process, was investigated. In the presence of nonionic surfactant Tx-15, the organically modified mesostructured nano-particles were synthesized by co-condensation of organosiloxane （RTES） and tetraethoxysilane （TEOS） in the first step, and then the bimodal porous silica was formed by the removal of the incorporated organic groups using programmed calcination. Here, RTES used was methyltriethoxysilane （MTES）, vinyltriethoxysilane （VTES） and phenyltriethoxysilane （PhTES）, respectively. Organotrialkoxysilane, TEOS and Tx-15 formed MSU-2-1iked assemblies, around which the nano-particles aggregated and cross-linked, considerably influencing the pore size distribution of both primary pores and secondary pores. By changing the type and amount of the organotrialkoxysilane added, a broad variety of silica with a controlled bimodal mesopore distribution could be easily synthesized. Textural and structural properties were determined by X-ray diffraction, high-resolution transmission electron microscopy, N2 adsorption/desorption, and thermogravimetric analysis.

Synthesis and Characterization of Bimodal Mesoporous Silica

Mesoporous silica with controllable bimodal pore size distribution was synthesized with cetyltrimethylammonium bromide （CTAB） as chemical template for small mesopores and silica gel as physical template for large mesopores. The structure of synthesized samples were characterized by Fourier transform infrared （FT-IR） spectroscopy, X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM） and N2 adsorption-desorption measurements. The experimental results show that bimodal mesoporous silica consists of small mesopores of about 3 nm and large mesopores of about 45 nm. The small mesopores which were formed on the external surface and pore walls of the silica gel had similar characters with those of MCM-41, while large mesopores were inherited from parent silica gel material. The pore size distribution of the synthesized silica can be adjusted by changing the relative content of TEOS and silica gel or the feeding sequence of silica gel and NH4OH.

Boosting xenon adsorption with record capacity in microporous carbon molecular sieves

Xenon/krypton(Xe/Kr)separation is an important task in industry,yet it remains challenging to develop adsorbents with high Xe/Kr selectivity and adsorption capacity of Xe,especially at low partial pressures.Herein,we report a series of microporous carbon molecular sieves(CMSs)for Xe/Kr separation.Those materials have ideal bimodal pore size distributions that not only provide substantial space for the accommodation of gas molecules,but also allow selective diffusion of gas molecules.Additionally,the carbon frameworks decorated with polar oxygen-containing functional groups afford higher affinity for Xe than Kr,which is proven by density functional theory(DFT)calculations and charge density difference analysis.The optimal CPVDC-700 exhibits a high selectivity of Xe/Kr and,more importantly,a record-high uptake of Xe(2.93 mmol g^(-1))at 0.2 bar and298 K,which is the highest among all the reported carbon adsorbents.Breakthrough experiments confirm the excellent performance of such CMSs for Xe/Kr separation,and the dynamic adsorption uptake of Xe and productivity of high-purity Kr are calculated to be 2.91 mmol g^(-1)and 208 m L g^(-1)(9.29 mmol g^(-1)),respectively,which also set up a new benchmark for Xe/Kr separation of carbon adsorbents.