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11.
Derek Yiren Ong Zhihao Yen Asami Yoshii Julia RevilloImbernon Ryo Takita Shunsuke Chiba 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(15):5046-5051
New protocols for controlled reduction of carboxamides to either alcohols or amines were established using a combination of sodium hydride (NaH) and zinc halides (ZnX2). Use of a different halide on ZnX2 dictates the selectivity, wherein the NaH‐ZnI2 system delivers alcohols and NaH‐ZnCl2 gives amines. Extensive mechanistic studies by experimental and theoretical approaches imply that polymeric zinc hydride (ZnH2)∞ is responsible for alcohol formation, whereas dimeric zinc chloride hydride (H?Zn?Cl)2 is the key species for the production of amines. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2018,130(10):2678-2682
A low‐temperature ammonia synthesis process is required for on‐site synthesis. Barium‐doped calcium amide (Ba‐Ca(NH2)2) enhances the efficacy of ammonia synthesis mediated by Ru and Co by 2 orders of magnitude more than that of a conventional Ru catalyst at temperatures below 300 °C. Furthermore, the presented catalysts are superior to the wüstite‐based Fe catalyst, which is known as a highly active industrial catalyst at low temperatures and pressures. Nanosized Ru–Ba core–shell structures are self‐organized on the Ba‐Ca(NH2)2 support during H2 pretreatment, and the support material is simultaneously converted into a mesoporous structure with a high surface area (>100 m2 g−1). These self‐organized nanostructures account for the high catalytic performance in low‐temperature ammonia synthesis. 相似文献
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《Helvetica chimica acta》2017,100(9)
Here we report the direct chemical synthesis of coenzyme B12 (AdoCbl) from Coβ ‐5′‐deoxyadenosylcobyric acid (AdoCby) and the preparation of the latter from crystalline CN ,H2O‐cobyric acid (CN ,H2OC by). AdoCby is a suggested common key intermediate in the biosynthesis of AdoCbl and of other cobamides in microorganisms. AdoCby was thoroughly characterized by spectroscopic means, including homo‐nuclear and hetero‐nuclear NMR , as such data are not available in published work. AdoCbl was prepared from AdoCby in one‐step in over 85% yield, by covalent attachment in aqueous solution of the integral B12‐nucleotide moiety using 1‐ethyl‐3‐(3‐dimethylaminopropyl)‐carbodiimide (EDC ·HC l) and N‐hydroxybenzotriazole (HOB t) as coupling reagents. By the same procedure crystalline vitamin B12 (CNC bl) was also prepared in 92% yield from CN ,H2OC by. Coordination of the B12‐nucleotide base at the Coα ‐face of AdoCby or of CN ,H2OC by was indicated to assist in the efficient covalent coupling at the activated f‐side chain function to furnish the complete corrinoids AdoCbl and CNC bl. 相似文献
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《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(47):15188-15192
The first example of base‐metal‐catalysed synthesis of amides from the coupling of primary amines with either alcohols or esters is reported. The reactions are catalysed by a new manganese pincer complex and generate hydrogen gas as the sole byproduct, thus making the overall process atom‐economical and sustainable. 相似文献