Journal
SCIENCE
Volume 372, Issue 6537, Pages 76-+Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.abe7935
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Funding
- National Key Research and Development Program of China [2018YFB0604801]
- National Natural Science Foundation of China [21822203, 21932006, 22032005, U1908203]
- Natural Science Foundation of Zhejiang Province [LR18B030002]
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Isolated boron in a zeolite framework without B-O-B oligomers exhibits high activity and selectivity for oxidative dehydrogenation of propane (ODHP). The boron-silicon bonding structure hinders boron leaching in a humid atmosphere, enhancing catalyst durability. The -B[OH center dot center dot center dot O(H)-Si](2) structure in borosilicate zeolite serves as the active center for activating oxygen and carbon-hydrogen bonds to catalyze ODHP.
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 COx. 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-SiOx linkage, achieving superior durability in a longperiod test. Furthermore, we demonstrate an isolated boron with a -B[OH center dot center dot center dot O(H)-Si](2) structure in borosilicate zeolite as the active center, which enables the activation of oxygen and a carbon-hydrogen bond to catalyze the ODHP.
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