Cooperative Trimerization of Carbon Monoxide by Lithium and Samarium Boryls

Journal of the American Chemical Society
Baoli WangZhaomin Hou

Abstract

The conversion of carbon monoxide (CO) to hydrocarbons and oxygenates on industrial solid catalysts (the Fischer-Tropsch reaction) largely relies on the cooperation of heteromultimetallic active sites composed of main group (such as alkali) and transition metals, but the mechanistic details have not been fully understood at the molecular level. Here we report the cooperative trimerization of CO by molecular lithium and samarium boryl complexes. We have found that, in the coexistence of a samarium boryl complex and a lithium boryl complex, the trimerization of CO selectively occurred to give a diborylallenetriolate skeleton "BC(O)C(O)C(O)B", in sharp contrast with the reaction of CO with either the lithium or the samarium boryl compound alone. The 13C-labeled experiments and computational studies have revealed that the CO trimerization reaction took place exclusively by coupling of a samarium boryl oxycarbene species, which was generated by insertion of one molecule of CO into the samarium-boryl bond, with a lithium ketenolate species formed by insertion of two molecules of CO into the lithium-boryl bond. These results offer unprecedented insight into CO oligomerization promoted by heteromultimetallic components and may help bet...Continue Reading

References

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Citations

Dec 12, 2018·Angewandte Chemie·Andrey V ProtchenkoSimon Aldridge
May 1, 2019·Chemical Communications : Chem Comm·Ravi YadavPeter W Roesky
Jun 13, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry·Richard Y Kong, Mark R Crimmin
Sep 16, 2018·Nature Communications·Helen R SharpeDeborah L Kays
Jul 29, 2021·Chemical Communications : Chem Comm·Sui HasegawaHiroyuki Kawaguchi
Oct 24, 2018·Journal of the American Chemical Society·Richard Y Kong, Mark R Crimmin
May 18, 2019·Journal of the American Chemical Society·K YuvarajCameron Jones
Nov 11, 2020·Journal of the American Chemical Society·Shaowei HuZhaomin Hou
Dec 6, 2018·Journal of the American Chemical Society·Yuwen WangMatthias Driess
Sep 14, 2021·Journal of the American Chemical Society·Qiu SunGerhard Erker
Jan 25, 2022·Journal of the American Chemical Society·Shiori Fujimori, Shigeyoshi Inoue

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