Key Lab of Biomass Chemical Engineering of Ministry of Education, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, China.
These authors contributed equally to this work.
Science. 2021 Apr 2;372(6537):76-80. doi: 10.1126/science.abe7935.
Oxidative dehydrogenation of propane (ODHP) is a key technology for producing propene from shale gas, but conventional metal oxide catalysts are prone to overoxidation to form valueless CO Boron-based catalysts were recently found to be selective for this reaction, and B-O-B oligomers are generally regarded as active centers. We show here that the isolated boron in a zeolite framework without such oligomers exhibits high activity and selectivity for ODHP, which also hinders full hydrolysis for boron leaching in a humid atmosphere because of the B-O-SiO linkage, achieving superior durability in a long-period test. Furthermore, we demonstrate an isolated boron with a -B[OH…O(H)-Si] structure in borosilicate zeolite as the active center, which enables the activation of oxygen and a carbon-hydrogen bond to catalyze the ODHP.
丙烷的氧化脱氢(ODHP)是从页岩气生产丙烯的关键技术,但传统的金属氧化物催化剂容易过度氧化形成无价值的 CO。最近发现硼基催化剂对此反应具有选择性,B-O-B 齐聚物通常被认为是活性中心。我们在这里表明,沸石骨架中没有此类齐聚物的孤立硼表现出 ODHP 的高活性和选择性,由于 B-O-SiO 键,这也阻碍了硼在潮湿气氛中的完全水解浸出,在长期测试中实现了优异的耐久性。此外,我们证明了硼硅酸盐沸石中具有 -B[OH…O(H)-Si]结构的孤立硼作为活性中心,能够激活氧和碳-氢键以催化 ODHP。