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11.
M. Sc. Akash Kaithal Pit van Bonn Dr. Markus Hölscher Prof. Dr. Walter Leitner 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(1):221-226
Highly selective β-methylation of alcohols was achieved using an earth-abundant first row transition metal in the air stable molecular manganese complex [Mn(CO)2Br[HN(C2H4PiPr2)2]] 1 ([HN(C2H4PiPr2)2]=MACHO-iPr). The reaction requires only low loadings of 1 (0.5 mol %), methanolate as base and MeOH as methylation reagent as well as solvent. Various alcohols were β-methylated with very good selectivity (>99 %) and excellent yield (up to 94 %). Biomass derived aliphatic alcohols and diols were also selectively methylated on the β-position, opening a pathway to “biohybrid” molecules constructed entirely from non-fossil carbon. Mechanistic studies indicate that the reaction proceeds through a borrowing hydrogen pathway involving metal–ligand cooperation at the Mn-pincer complex. This transformation provides a convenient, economical, and environmentally benign pathway for the selective C−C bond formation with potential applications for the preparation of advanced biofuels, fine chemicals, and biologically active molecules 相似文献
12.
Ryuichi Yamamoto 《Physica A》2010,389(6):1208-1214
Recent empirical research has documented asymmetric volatility and volatility clustering in stock markets. We conjecture that a limit of arbitrage due to a borrowing constraint and herding behavior by investors are related to these phenomena. This study conducts simulation analyses on a spin model where borrowing constrained agents imitate their nearest neighbors but switch their strategies to a different one intermittently. We show that herding matters for volatility clustering while a borrowing constraint intensifies the asymmetry of volatility through the herding effect. 相似文献
13.
Pedro J. Llabres-Campaner Patricia Woodbridge-Ortega Rafael Ballesteros-Garrido Rafael Ballesteros Belén Abarca 《Tetrahedron letters》2017,58(52):4880-4882
A borrowing hydrogen reaction with different diols was employed for the preparation of complex beta- gamma- or epsilon-amino alcohols from p-toluidine and tetrahydroquinoline with the aim of better understanding the applicability of the Pd/C ZnO heterogeneous catalyst. 相似文献
14.
The admissible efficient portfolio selection problem for risky assets has been discussed by Zhang and Nie. In this paper, the admissible efficient portfolio model is proposed under the assumption that there exists the borrowing (money or a risk free asset) case. The admissible efficient frontiers are developed by the spreads of expected return and risk from admissible errors. The analytic forms of the admissible efficient frontiers when short sales are not allowed on all risky assets are derived from two cases: the borrowing with an upper bound constraint, or without an upper bound constraint. The influence on the admissible efficient frontier is explained under the different interest rates of the borrowing. The differences between the results with the borrowing and the results without the borrowing is revealed by a real numerical example. 相似文献
15.
以基于借氢策略的苯甲醇和苯胺一步合成N-苯基苄胺为模型反应,研究了三种不同表面结构的氧化铝对其负载的Pt-Sn催化剂上N-烷基化合成仲胺反应性能的影响.采用N2吸附-脱附法、压汞法、X射线衍射、透射电镜、扫描电镜、CO脉冲吸附、H2-程序升温还原及NH3-程序升温脱附等技术对载体和Pt-Sn/Al2O3催化剂进行了表征.结果表明,与Al2O3相互作用较弱且高度分散的Pt颗粒具有很高的催化活性,Al2O3载体较大的孔体积和大孔分布的孔结构有助于反应物扩散和吸附到催化剂表面并提高反应活性.同时也有利于反应产物从催化剂表面离开,从而提高催化剂的稳定性.然而Al2O3较强的酸性及酸性分布降低了产物仲胺的选择性和催化剂稳定性. 相似文献
16.
Teng Wei Ng Ran Tao Willy Wei Li See Si Bei Poh Yu Zhao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(2):e202212528
We disclose herein a catalytic borrowing hydrogen method that enables an unprecedented, economical one-pot access to enantiopure tetrahydropyridines with minimal reagent use or waste formation. This method couples a few classes of readily available substrates with commercially available 1,3-amino alcohols, and delivers the valuable tetrahydropyridines of different substitution patterns free of N-protection. Such transformations are highly challenging to achieve, as multiple redox steps need to be realized in a cascade and numerous side reactions including a facile aromatization have to be overcome. Highly diastereoselective functionalizations of tetrahydropyridines also result in a general access to enantiopure di- and tri-substituted piperidines, which ranks the topmost frequent N-heterocycle in commercial drugs. 相似文献
17.
Feixiang Sun Jiamin Huang Dr. Zhihong Wei Prof. Dr. Conghui Tang Prof. Dr. Weiping Liu 《Angewandte Chemie (International ed. in English)》2023,62(26):e202303433
A homogeneous manganese-catalyzed cross-coupling of two secondary alcohols for the divergent synthesis of γ-disubstituted alcohols and β-disubstituted ketones is reported. Employing the well-defined Mn-MACHOPh as the catalyst, this novel protocol has a broad substrate scope with good functional group tolerance and affords a diverse library of valuable disubstituted alcohols and ketones in moderate to good yields. The strong influence of the reaction temperature on the selective formation of alcohol products was theorized in preliminary DFT studies. Studies have shown that the Gibbs free energy of the formation of alcohols is thermodynamically more favourable than corresponding ketones at a lower temperature. 相似文献