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Regeneration of a Spent TS-1 Zeolite Catalyst for Liquid-Phase Epoxidation of Propylene and H2O2
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-07-27 , DOI: 10.1021/acs.iecr.3c01141 Yue Li 1 , Yanhui Yi 1 , Xiangsheng Wang 1 , Bize Gao 1 , Yitong Guo 1 , Guoxing Wu 1 , Zhaochi Feng 2 , Hongchen Guo 1
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-07-27 , DOI: 10.1021/acs.iecr.3c01141 Yue Li 1 , Yanhui Yi 1 , Xiangsheng Wang 1 , Bize Gao 1 , Yitong Guo 1 , Guoxing Wu 1 , Zhaochi Feng 2 , Hongchen Guo 1
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This paper carries out a systematic deactivation and regeneration study on a spent TS-1 zeolite extrudate catalyst, which was obtained from a scale-up propylene liquid-phase epoxidation test after a 1800 h time on stream under simulated industrial conditions. Results show that the catalyst deactivation is mainly due to blocking of zeolitic framework Ti active sites by heavier oligomers and surface-adsorbed low-boiling-point substances. These blocking substances are easy to be thoroughly cleared away by H2O2 washing or high-temperature calcination regeneration, and consequently, the catalyst’s activity can be restored satisfactorily. However, the regenerated catalysts show deterioration of durability and reduction of initial PO selectivity, which are closely related to the irreversible hydrolysis of the Ti–O–Si bond of the TS-1 zeolite catalyst by H2O2 solution, increasing surface hydroxyl groups and acidity. This irreversible hydrolysis can occur during the epoxidation reaction process, and thus future studies will be focused on measures to cope with this tough challenge.
中文翻译：
用于丙烯和 H2O2 液相环氧化的废 TS-1 沸石催化剂的再生
本文对废旧TS-1沸石挤出催化剂进行了系统的失活和再生研究，该催化剂是在模拟工业条件下运行1800小时后在丙烯液相环氧化放大试验中获得的。结果表明，催化剂失活主要是由于较重的低聚物和表面吸附的低沸点物质堵塞了沸石骨架Ti活性位点。这些阻塞物质很容易被H 2 O 2彻底清除掉通过水洗或高温焙烧再生，催化剂的活性可以得到满意的恢复。然而，再生后的催化剂表现出耐久性的恶化和初始PO选择性的降低，这与H 2 O 2溶液对TS-1沸石催化剂的Ti-O-Si键的不可逆水解，增加表面羟基密切相关。和酸度。这种不可逆的水解可能发生在环氧化反应过程中，因此未来的研究将集中于应对这一严峻挑战的措施。
更新日期：2023-07-27
中文翻译：
用于丙烯和 H2O2 液相环氧化的废 TS-1 沸石催化剂的再生
本文对废旧TS-1沸石挤出催化剂进行了系统的失活和再生研究，该催化剂是在模拟工业条件下运行1800小时后在丙烯液相环氧化放大试验中获得的。结果表明，催化剂失活主要是由于较重的低聚物和表面吸附的低沸点物质堵塞了沸石骨架Ti活性位点。这些阻塞物质很容易被H 2 O 2彻底清除掉通过水洗或高温焙烧再生，催化剂的活性可以得到满意的恢复。然而，再生后的催化剂表现出耐久性的恶化和初始PO选择性的降低，这与H 2 O 2溶液对TS-1沸石催化剂的Ti-O-Si键的不可逆水解，增加表面羟基密切相关。和酸度。这种不可逆的水解可能发生在环氧化反应过程中，因此未来的研究将集中于应对这一严峻挑战的措施。
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