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Epoxidation of 1-hexene with hydrogen peroxide over nitrogen-incorporated TS-1 zeolite
Affiliation:1. College of Chemical Engineering, Xiangtan University, Xiangtan 411105, China;2. School of Chemistry and Chemical Engineering, Central South University, Changsha 410083, China;1. State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, PR China;2. EMS Energy Institute, PSU-DUT Joint Center for Energy Research and Department of Energy & Mineral Engineering, Pennsylvania State University,University Park, PA 16802, USA;3. Network and Informationization Center, Dalian University of Technology, Dalian 116024, PR China;1. State Key Laboratory of Heavy Oil Processing, School of Chemical Engineering, China University of Petroleum, Qingdao 266580, China;2. State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China;3. Department of Chemical Engineering, Norwegian University of Science and Technology, Trondheim 7491, Norway;1. School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300350, PR China;2. School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang, 212003, Jiangsu, PR China
Abstract:Nitrogen-incorporated TS-1 zeolite (N-TS-1) was synthesized by direct calcining the as-synthesized TS-1 powder in NH3 flow at high temperature. Epoxidation of 1-hexene with dilute H2O2 over N-TS-1 was studied. The results showed that the catalytic activity and selectivity of TS-1 were greatly improved upon post-synthetic nitridation. A new Tisingle bondOOH intermediate with double hydrogen bonds was proposed. The new intermediate was more stable due to the presence of another hydrogen bond, which was formed between the stable nitrogen species and the H atom of the conventional five-member-ring intermediate, thereby improving the epoxidation activity.
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