Hierarchically organized porous materials can provide multidimensional spatial networks on different length scales with improved characteristics relevant to molecular diffusion. [1] Zeolites that are microporous crystalline materials having pores and channels at molecular dimensions are of great importance for industrial applications. [2] However, the presence of only micropores in zeolite frameworks often limits the molecular diffusion and therefore, restricts the transport of bulky molecules. This problem can be resolved by shortening the effective diffusion path lengths, which has been achieved by miniaturizing zeolite crystals, [3] delaminating or exfoliating layered zeolites, [4] synthesizing zeolite nanosheets, [5] and introducing mesopores into zeolite particles. [6][7][8][9][10][11][12] Among these solutions, the fabrication of hierarchical zeolites with micro-and mesoporosity is of interest because it combines intrinsic micropores with bypass-interconnected mesopores, and therefore, enhances both the micropore accessibility and molecular traffic within zeolite particles. [1, 7b, 12] Hierarchical zeolites have been produced using several techniques, including top-down desilication by alkali postsynthetic treatment [6] and bottom-up directed assembly by hard [7] or soft [8][9][10][11] templates. The hard-template method requires multistep procedures and is therefore unfavorable for large-scale production. Alternatively, the direct introduction of organic mesopore-generating agents (mesoporogens) during zeolite synthesis can create uniform mesopores. The use of such mesoporogens is currently one of the most promising methods for the single-step construction of hierarchical zeolites. Progress has been made using well-designed mesoporogens composed of long hydrophobic chains and hydrophilic zeolitic structure-directing groups to generate zeolites with tunable mesoporosity [9a, 10] and to direct the hierarchical assembly of zeolite nanosheets, yielding mesoporous zeolites with house-of-cards-like structures. [5a, 9c, 11] These hierarchical nanosheets showed excellent catalytic performance in several important reactions because the presence of thin layers with specific crystalline faces facilitates catalysis at the exteriors or pore mouths. [13] Such mesoporogens are probably necessary for the direct, singlestep synthesis of hierarchical zeolites.Herein we report an alternative, mesoporogen-free approach for the construction of hierarchically organized MFI zeolites by sequential intergrowth using a simple organic structure-directing agent (OSDA). The selection of an appropriate OSDA and optimized synthesis conditions that can form plate-like zeolites with enhanced 908 rotational intergrowths seems to be a key to achieving a hierarchical structure with three classes of porosity in one structure: the intrinsic microporosity of the zeolite framework together with mesoporosity existing within the zeolite plates and macroporosity stemming from the complex intergrown structure.Epitaxial and rotational int...
The climactic phase of the 2011 eruption at Shinmoe-dake was a mixture of subplinian and vulcanian eruptive events, successive lava accumulation (lava dome) within the crater, and repetition of vulcanian events after the dome growth. It was preceded by inflation and elevated seismicity for about one year and by phreatomagmatic explosions of one week before. Small pyroclastic flows and ash-cloud surges formed during the subplinian events, when the eruption column reached the highest level and the vent was widened. A lava dome, which was extruded close to the vent of subplinian events, grew by swelling upward and filling the crater. After the vent was covered by the lava, an intense vulcanian event occurred from the base of the dome and the swelled dome became deflated. After that, vulcanian events were repeated for three months. Simultaneous eruption styles in the crater (vulcanian events, continuous ash emission and dome growth) and some phreatomagmatic events in the vulcanian stage probably are due to a complex upper-conduit system developed in water-saturated country rock.
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