Modulating inherent lewis acidity at the intergrowth interface of mortise-tenon zeolite catalyst

Huiqiu Wang; Boyuan Shen; Xiao Chen; Hao Xiong; Hongmei Wang; Wenlong Song; Chaojie Cui; Fei Wei; Weizhong Qian

doi:10.1038/s41467-022-30538-7

Modulating inherent lewis acidity at the intergrowth interface of mortise-tenon zeolite catalyst

Nat Commun. 2022 May 25;13(1):2924. doi: 10.1038/s41467-022-30538-7.

Authors

Huiqiu Wang^#¹, Boyuan Shen^#^{1

2}, Xiao Chen³, Hao Xiong¹, Hongmei Wang¹, Wenlong Song¹, Chaojie Cui¹, Fei Wei⁴, Weizhong Qian⁵

Affiliations

¹ Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, China.
² Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, 199 Ren'ai Road, 215123, Suzhou, Jiangsu, PR China.
³ Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, China. chenx123@tsinghua.edu.cn.
⁴ Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, China. wf-dce@tsinghua.edu.cn.
⁵ Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology, Department of Chemical Engineering, Tsinghua University, 100084, Beijing, China. qianwz@tsinghua.edu.cn.

^# Contributed equally.

Abstract

The acid sites of zeolite are important local structures to control the products in the chemical conversion. However, it remains a great challenge to precisely design the structures of acid sites, since there are still lack the controllable methods to generate and identify them with a high resolution. Here, we use the lattice mismatch of the intergrown zeolite to enrich the inherent Lewis acid sites (LASs) at the interface of a mortise-tenon ZSM-5 catalyst (ZSM-5-MT) with a 90° intergrowth structure. ZSM-5-MT is formed by two perpendicular blocks that are atomically resolved by integrated differential phase contrast scanning transmission electron microscopy (iDPC-STEM). It can be revealed by various methods that novel framework-associated Al (Al_FR) LASs are generated in ZSM-5-MT. Combining the iDPC-STEM results with other characterizations, we demonstrate that the partial missing of O atoms at interfaces results in the formation of inherent Al_FR LASs in ZSM-5-MT. As a result, the ZSM-5-MT catalyst shows a higher selectivity of propylene and butene than the single-crystal ZSM-5 in the steady conversion of methanol. These results provide an efficient strategy to design the Lewis acidity in zeolite catalysts for tailored functions via interface engineering.