Yang Liu, Wang Chang, Zhang Lina, Dai Weili, Chu Yueying, Xu Jun, Wu Guangjun, Gao Mingbin, Liu Wenjuan, Xu Zhaochao, Wang Pengfei, Guan Naijia, Dyballa Michael, Ye Mao, Deng Feng, Fan Weibin, Li Landong
School of Materials Science and Engineering, and National Institute for Advanced Materials, Nankai University, Tianjin, P.R. China.
Key Laboratory of Advanced Energy Materials Chemistry of the Ministry of Education, Collaborative Innovation Center of Chemical Science and Engineering, Nankai University, Tianjin, P.R. China.
Nat Commun. 2021 Aug 2;12(1):4661. doi: 10.1038/s41467-021-24403-2.
As a commercial MTO catalyst, SAPO-34 zeolite exhibits excellent recyclability probably due to its intrinsic good hydrothermal stability. However, the structural dynamic changes of SAPO-34 catalyst induced by hydrocarbon pool (HP) species and the water formed during the MTO conversion as well as its long-term stability after continuous regenerations are rarely investigated and poorly understood. Herein, the dynamic changes of SAPO-34 framework during the MTO conversion were identified by 1D Al, P MAS NMR, and 2D P-Al HETCOR NMR spectroscopy. The breakage of T-O-T bonds in SAPO-34 catalyst during long-term continuous regenerations in the MTO conversion could be efficiently suppressed by pre-coking. The combination of catalyst pre-coking and water co-feeding is established to be an efficient strategy to promote the catalytic efficiency and long-term stability of SAPO-34 catalysts in the commercial MTO processes, also sheds light on the development of other high stable zeolite catalyst in the commercial catalysis.
作为一种商业甲醇制烯烃（MTO）催化剂，SAPO-34沸石表现出优异的可回收性，这可能归因于其固有的良好水热稳定性。然而，关于烃池（HP）物种和MTO转化过程中形成的水引起的SAPO-34催化剂的结构动态变化以及其连续再生后的长期稳定性，很少有人研究且了解甚少。在此，通过一维铝、磷魔角旋转核磁共振（MAS NMR）和二维磷-铝异核相关（HETCOR）核磁共振光谱确定了MTO转化过程中SAPO-34骨架的动态变化。在MTO转化的长期连续再生过程中，通过预焦化可以有效抑制SAPO-34催化剂中T-O-T键的断裂。建立催化剂预焦化和水共进料的组合是提高SAPO-34催化剂在商业MTO工艺中的催化效率和长期稳定性的有效策略，这也为商业催化中其他高稳定性沸石催化剂的开发提供了思路。
Zotero 插件
