Division of Fossil Energy Conversion, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2017 Oct 2;56(41):12553-12556. doi: 10.1002/anie.201706566. Epub 2017 Sep 1.
The rational design of zeolite-based catalysts calls for flexible tailoring of porosity and acidity beyond micropore dimension. To date, dealumination has been applied extensively as an industrial technology for the tailoring of zeolite in micropore dimension, whereas desilication has separately shown its potentials in the creation of mesoporosities. The free coupling of dealumination with desilication will bridge the tailoring at micro/mesopore dimensions; however, such coupling has been prevailingly confirmed as an impossible mission. In this work, a consecutive dealumination-desilication process enables the introduction of uniform intracrystalline mesopores (4-6 nm) into the microporous Al-rich zeolites. The decisive impacts of steaming step have been firstly discovered. These findings revitalize the functions of dealumination in porosity tailoring, and stimulate the pursuit of new methods for the tailoring of industrially relevant Al-rich zeolites.
沸石基催化剂的合理设计需要灵活调整孔结构和酸度,不仅限于微孔尺寸。迄今为止,脱铝已被广泛应用于工业技术中,用于调整沸石的微孔尺寸,而脱硅则分别显示出在中孔形成方面的潜力。脱铝与脱硅的自由偶联将在微/介孔尺寸的调整中架起桥梁;然而,这种偶联普遍被认为是不可能完成的任务。在这项工作中,连续的脱铝-脱硅过程使均一的晶内介孔(4-6nm)能够引入到富铝沸石的微孔中。首先发现了蒸汽处理步骤的决定性影响。这些发现使脱铝在孔结构调整方面的功能得到了恢复,并激发了人们对工业相关富铝沸石的新的调整方法的追求。