Stabilizing the framework of SAPO-34 zeolite toward long-term methanol-to-olefins conversion.
Stabilizing the framework of SAPO-34 zeolite toward long-term methanol-to-olefins conversion.
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DOI：
10.1038/s41467-021-24403-2
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发表时间：
2021-08-02
影响因子：
16.6
通讯作者：
Li L
中科院分区：
文献类型：
--
作者：
Yang L;Wang C;Zhang L;Dai W;Chu Y;Xu J;Wu G;Gao M;Liu W;Xu Z;Wang P;Guan N;Dyballa M;Ye M;Deng F;Fan W;Li L
SAPO-34分子筛作为一种工业化的MTO催化剂，由于其固有的良好的水热稳定性而具有良好的可循环性。然而，SAPO-34催化剂的结构动态变化所引起的烃池（HP）物种和水形成的MTO转化过程中，以及它的长期稳定性后，连续再生很少研究和了解甚少。在此，SAPO-34骨架在MTO转化过程中的动态变化通过1D 27 Al，31 P MAS NMR和2D 31 P-27 Al HETCOR NMR谱来确定。预结焦可有效抑制SAPO-34催化剂在MTO转化过程中长时间连续再生时T-O-T键的断裂。催化剂预结焦与水共进料相结合是提高SAPO-34催化剂在MTO工业化过程中的催化效率和长期稳定性的有效策略，也为开发其他高稳定性沸石催化剂在工业化催化过程中的应用提供了借鉴。沸石催化剂的稳定性是商业甲醇至烯烃转化的高度期望的性质，但实现起来极具挑战性。在这里，作者联合收割机的催化剂预焦化和水的共同进料，开发一种有效的策略，以提高SAPO-34催化剂的长期稳定性。
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 27Al, 31P MAS NMR, and 2D 31P-27Al 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. Stability of zeolite catalysts is a highly desirable property for commercial methanol to olefins conversion but extremely challenging to achieve. Here, the authors combine the catalyst pre-coking and water co-feeding to develop an efficient strategy to enhance the long-term stability of SAPO-34 catalyst.
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