The development of an efficient and sustainable synthetic route for formaldehyde production from renewable feedstock,especially in combination with a subsequent transformation to straightforwardly construct valuable c...The development of an efficient and sustainable synthetic route for formaldehyde production from renewable feedstock,especially in combination with a subsequent transformation to straightforwardly construct valuable chemicals,is highly desirable.Herein,we report a novel manganese-catalyzed dehydrogenative cyclization of methanol as a formaldehyde surrogate with a variety of dinucleophiles for facile synthesis of N-heterocycles.The in situ generated formaldehyde via catalytic methanol dehydrogenation can be selectively trapped by diverse dinucleophiles to avoid several possible side reactions.The utilty of this transformation is further highlighted by its successful appliation to the synthesis of 13C-labeled N-heterocycles using 13CH_(3)OH as a readily accessible 13C-isotope reagent.展开更多
Background and Originality Content Reduction of esters to alcohols is a fundamental transformation in organic chemistry,and is important for the production of a wide range of bulk and fine chemicals.Compared with trad...Background and Originality Content Reduction of esters to alcohols is a fundamental transformation in organic chemistry,and is important for the production of a wide range of bulk and fine chemicals.Compared with traditional approaches using stoichiometric amounts of metal hydride reagents,catalytic hydrogenation represents an environmentally benign and atom economic alternative.展开更多
基金This project was supported by the National Natural Science Foundation of China(Nos.91845107 and 21822106)the Foundation of the Department of Education of Guangdong Province(2018KZDXM070 and 2021KTSCX140)。
文摘The development of an efficient and sustainable synthetic route for formaldehyde production from renewable feedstock,especially in combination with a subsequent transformation to straightforwardly construct valuable chemicals,is highly desirable.Herein,we report a novel manganese-catalyzed dehydrogenative cyclization of methanol as a formaldehyde surrogate with a variety of dinucleophiles for facile synthesis of N-heterocycles.The in situ generated formaldehyde via catalytic methanol dehydrogenation can be selectively trapped by diverse dinucleophiles to avoid several possible side reactions.The utilty of this transformation is further highlighted by its successful appliation to the synthesis of 13C-labeled N-heterocycles using 13CH_(3)OH as a readily accessible 13C-isotope reagent.
基金We are grateful for the financial supports from the National Natural Science Foundation of China(Nos.21822106 and 91845107)the Beijing Municipal Commission of Science and Technology(No.Z 181100005118001).
文摘Background and Originality Content Reduction of esters to alcohols is a fundamental transformation in organic chemistry,and is important for the production of a wide range of bulk and fine chemicals.Compared with traditional approaches using stoichiometric amounts of metal hydride reagents,catalytic hydrogenation represents an environmentally benign and atom economic alternative.