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A general carbonyl alkylative amination for tertiary amine synthesis 期刊论文
NATURE, 2020
作者:  Ouyang, David;  He, Bryan;  Ghorbani, Amirata;  Yuan, Neal;  Ebinger, Joseph;  Langlotz, Curtis P.;  Heidenreich, Paul A.;  Harrington, Robert A.;  Liang, David H.;  Ashley, Euan A.;  Zou, James Y.
收藏  |  浏览/下载:27/0  |  提交时间:2020/07/03

The ubiquity of tertiary alkylamines in pharmaceutical and agrochemical agents, natural products and small-molecule biological probes(1,2) has stimulated efforts towards their streamlined synthesis(3-9). Arguably the most robust method for the synthesis of tertiary alkylamines is carbonyl reductive amination(3), which comprises two elementary steps: the condensation of a secondary alkylamine with an aliphatic aldehyde to form an all-alkyl-iminium ion, which is subsequently reduced by a hydride reagent. Direct strategies have been sought for a '  higher order'  variant of this reaction via the coupling of an alkyl fragment with an alkyl-iminium ion that is generated in situ(10-14). However, despite extensive efforts, the successful realization of a '  carbonyl alkylative amination'  has not yet been achieved. Here we present a practical and general synthesis of tertiary alkylamines through the addition of alkyl radicals to all-alkyl-iminium ions. The process is facilitated by visible light and a silane reducing agent, which trigger a distinct radical initiation step to establish a chain process. This operationally straightforward, metal-free and modular transformation forms tertiary amines, without structural constraint, via the coupling of aldehydes and secondary amines with alkyl halides. The structural and functional diversity of these readily available precursors provides a versatile and flexible strategy for the streamlined synthesis of complex tertiary amines.


The synthesis of tertiary amines is achieved through a carbonyl alkylative amination reaction facilitated by visible light, in which an aldehyde and an amine condense to form an iminium ion that subsequently reacts with alkyl radical.


  
Power generation from ambient humidity using protein nanowires 期刊论文
NATURE, 2020, 578 (7796) : 550-+
作者:  Luong, Duy X.;  Bets, Ksenia V.;  Algozeeb, Wala Ali;  Stanford, Michael G.;  Kittrell, Carter;  Chen, Weiyin;  Salvatierra, Rodrigo V.;  Ren, Muqing;  McHugh, Emily A.;  Advincula, Paul A.;  Wang, Zhe;  Bhatt, Mahesh;  Guo, Hua;  Mancevski, Vladimir;  Shahsavari, Rouzbeh;  Yakobson, Boris I.;  Tour, James M.
收藏  |  浏览/下载:116/0  |  提交时间:2020/07/03

Harvesting energy from the environment offers the promise of clean power for self-sustained systems(1,2). Known technologies-such as solar cells, thermoelectric devices and mechanical generators-have specific environmental requirements that restrict where they can be deployed and limit their potential for continuous energy production(3-5). The ubiquity of atmospheric moisture offers an alternative. However, existing moisture-based energy-harvesting technologies can produce only intermittent, brief (shorter than 50 seconds) bursts of power in the ambient environment, owing to the lack of a sustained conversion mechanism(6-12). Here we show that thin-film devices made from nanometre-scale protein wires harvested from the microbe Geobacter sulfurreducens can generate continuous electric power in the ambient environment. The devices produce a sustained voltage of around 0.5 volts across a 7-micrometre-thick film, with a current density of around 17 microamperes per square centimetre. We find the driving force behind this energy generation to be a self-maintained moisture gradient that forms within the film when the film is exposed to the humidity that is naturally present in air. Connecting several devices linearly scales up the voltage and current to power electronics. Our results demonstrate the feasibility of a continuous energy-harvesting strategy that is less restricted by location or environmental conditions than other sustainable approaches.


A new type of energy-harvesting device, based on protein nanowires from the microbe Geobacter sulforreducens, can generate a sustained power output by producing a moisture gradient across the nanowire film using natural humidity.


  
Rethinking Resilience in Industrial Symbiosis: Conceptualization and Measurements 期刊论文
ECOLOGICAL ECONOMICS, 2017, 137
作者:  Fraccascia, Luca;  Giannoccaro, Ilaria;  Albino, Vito
收藏  |  浏览/下载:21/0  |  提交时间:2019/04/09
Industrial Symbiosis Network  Resilience  Ecological systems  Diversity  Ubiquity  Measurements