Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2020-05-27 , DOI: 10.1016/j.micromeso.2020.110358 Ying Wang , Tinglong Yang , Fei Liu , Tianxiang Zhao , Xiaodan Wang , Jianxin Cao
The ZSM-5@t-ZrO2 coated composite with t-ZrO2 as a shell phase, was fabricated using polyelectrolyte-based layer by layer assembly strategy, to enhance the selectivity of methanethiol by the confinement effect of base sites distributed on the shell layer. The study showed that polyelectrolyte functionalization of the t-ZrO2 surface was crucial to avoid phase separation during the hydrothermal coating process. The fully coated composite obtained via polyelectrolyte modification in order of PDDA+/PSS−/PDDA+ exhibited superior catalytic performance toward methanethiol selectivity of up to 95% and methanol conversion rate close to 90%. Methanethiol selectivity increased by approx. 20% compared with the unmodified composite. The interfacial interaction between the ZSM-5 and t-ZrO2 phases was related to the coated structure, which subsequently caused a series of favorable alterations to the composite's physicochemical properties. Moreover, the confinement effect produced by the fully coated structure with t-ZrO2 as the shell phase primarily contributed to enhancement of methanethiol selectivity of ZSM-5@t-ZrO2 in the thiolation of methanol with H2S to methanethiol.
中文翻译:
在包含ZSM-5和t-ZrO 2的涂层复合材料上甲硫醇合成中的高选择性
采用基于聚电解质的层层组装策略,制备了以t-ZrO 2为壳相的ZSM-5 @ t-ZrO 2涂层复合材料,通过限制分布在壳上的碱基来提高甲硫醇的选择性。层。研究表明,t-ZrO 2表面的聚电解质功能化对于避免水热涂覆过程中的相分离至关重要。完全包覆复合经由聚电解质改性得到的顺序为PDDA + / PSS - / PDDA +对甲醇的选择性高达95%,甲醇转化率接近90%。甲硫醇的选择性提高了约 与未改性的复合材料相比,为20%。ZSM-5和t-ZrO 2相之间的界面相互作用与涂层结构有关,这随后对复合材料的物理化学性质产生了一系列有利的变化。而且,由t-ZrO 2作为壳相的完全涂覆结构产生的限制作用主要有助于在甲醇与H 2 S硫醇化为甲硫醇时提高ZSM-5 @ t-ZrO 2的甲硫醇选择性。