State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology , Dalian 116024, P. R. China.
Shanghai Baosteel Chemical Co., Ltd. , No. 3501 Tongji Road, Shanghai, P. R. China.
ACS Nano. 2016 Aug 23;10(8):7401-8. doi: 10.1021/acsnano.6b00888. Epub 2016 Jul 26.
Inspired by the vesicular structure of alveolus which has a porous nanovesicle structure facilitating the transport of oxygen and carbon dioxide, we designed a hollow nanovesicle assembly with metal-encapsulated hollow zeolite that would enhance diffusion of reactants/products and inhibit sintering and leaching of active metals. This zeolitic nanovesicle has been successfully synthesized by a strategy which involves a one-pot hydrothermal synthesis of hollow assembly of metal-containing solid zeolite crystals without a structural template and a selective desilication-recrystallization accompanied by leaching-hydrolysis to convert the metal-containing solid crystals into metal-encapsulated hollow crystals. We demonstrate the strategy in synthesizing a hollow nanovesicle assembly of Fe2O3-encapsulated hollow crystals of ZSM-5 zeolite. This material possesses a microporous (0.4-0.6 nm) wall of hollow crystals and a mesoporous (5-17 nm) shell of nanovesicle with macropores (about 350 nm) in the core. This hierarchical structure enables excellent Fe2O3 dispersion (3-4 nm) and resistance to sintering even at 800 °C; facilitates the transport of reactant/products; and exhibits superior activity and resistance to leaching in phenol degradation. Hollow nanovesicle assembly of Fe-Pt bimetal-encapsulated hollow ZSM-5 crystals was also prepared.
受肺泡的泡状结构的启发,肺泡具有多孔纳米囊泡结构,有利于氧气和二氧化碳的运输,我们设计了一种具有金属封装的空心沸石的中空纳米囊泡组装体,以增强反应物/产物的扩散,并抑制活性金属的烧结和浸出。这种沸石纳米囊泡是通过一种策略成功合成的,该策略涉及在没有结构模板的情况下一锅水热合成含金属的固体沸石晶体的中空组装体,以及伴随浸出水解的选择性脱硅再结晶,将含金属的固体晶体转化为金属封装的空心晶体。我们在合成 Fe2O3 封装的 ZSM-5 沸石空心晶体的中空纳米囊泡组装体中证明了这一策略。该材料具有微孔(0.4-0.6nm)壁的空心晶体和介孔(5-17nm)壳的纳米囊泡,以及核中的大孔(约 350nm)。这种分级结构使 Fe2O3 具有良好的分散性(3-4nm),即使在 800°C 下也能抵抗烧结;有利于反应物/产物的传输;并在苯酚降解中表现出优异的活性和抗浸出性。还制备了 Fe-Pt 双金属封装的空心 ZSM-5 晶体的中空纳米囊泡组装体。