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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:12/0  |  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.


  
Climate and plant community diversity in space and time 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (9) : 4464-4470
作者:  Harrison, Susan;  Spasojevic, Marko J.;  Li, Daijiang
收藏  |  浏览/下载:6/0  |  提交时间:2020/05/13
aridification  climate change  drought  functional diversity  phylogenetic diversity  
Biogeographic historical legacies in the net primary productivity of Northern Hemisphere forests 期刊论文
ECOLOGY LETTERS, 2020, 23 (5) : 800-810
作者:  Conradi, Timo;  Van Meerbeek, Koenraad;  Ordonez, Alejandro;  Svenning, Jens-Christian
收藏  |  浏览/下载:10/0  |  提交时间:2020/07/02
Climate change  ecosystem functioning  functional diversity  historical contingency  NPP  species pool  
Geographically divergent evolutionary and ecological legacies shape mammal biodiversity in the global tropics and subtropics 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (3) : 1559-1565
作者:  Rowan, John;  Beaudrot, Lydia;  Franklin, Janet;  Reed, Kaye E.;  Smail, Irene E.;  Zamora, Andrew;  Kamilar, Jason M.
收藏  |  浏览/下载:9/0  |  提交时间:2020/05/13
biogeography  functional ecology  human impacts  paleoclimate legacies  phylogenetic diversity  
Land-use history impacts functional diversity across multiple trophic groups 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (3) : 1573-1579
作者:  Le Provost, Gaetane;  Badenhausser, Isabelle;  Le Bagousse-Pinguet, Yoann;  Clough, Yann;  Henckel, Laura;  Violle, Cyrille;  Bretagnolle, Vincent;  Roncoroni, Marilyn;  Manning, Peter;  Gross, Nicolas
收藏  |  浏览/下载:15/0  |  提交时间:2020/05/13
agricultural ecosystems  biodiversity loss  functional diversity  grasslands  land-use changes  
Giant virus diversity and host interactions through global metagenomics 期刊论文
NATURE, 2020: 1-+
作者:  Su, Jie;  Morgani, Sophie M.;  David, Charles J.;  Wang, Qiong;  Er, Ekrem Emrah;  Huang, Yun-Han;  Basnet, Harihar;  Zou, Yilong;  Shu, Weiping;  Soni, Rajesh K.;  Hendrickson, Ronald C.;  Hadjantonakis, Anna-Katerina;  Massague, Joan
收藏  |  浏览/下载:20/0  |  提交时间:2020/07/03

Analysis of metagenomics data revealed that large and giant viruses are globally widely distributed and are associated with most major eukaryotic lineages.


Our current knowledge about nucleocytoplasmic large DNA viruses (NCLDVs) is largely derived from viral isolates that are co-cultivated with protists and algae. Here we reconstructed 2,074 NCLDV genomes from sampling sites across the globe by building on the rapidly increasing amount of publicly available metagenome data. This led to an 11-fold increase in phylogenetic diversity and a parallel 10-fold expansion in functional diversity. Analysis of 58,023 major capsid proteins from large and giant viruses using metagenomic data revealed the global distribution patterns and cosmopolitan nature of these viruses. The discovered viral genomes encoded a wide range of proteins with putative roles in photosynthesis and diverse substrate transport processes, indicating that host reprogramming is probably a common strategy in the NCLDVs. Furthermore, inferences of horizontal gene transfer connected viral lineages to diverse eukaryotic hosts. We anticipate that the global diversity of NCLDVs that we describe here will establish giant viruses-which are associated with most major eukaryotic lineages-as important players in ecosystems across Earth'  s biomes.


  
Growing-season temperature and precipitation are independent drivers of global variation in xylem hydraulic conductivity 期刊论文
GLOBAL CHANGE BIOLOGY, 2019
作者:  He, Pengcheng;  Gleason, Sean M.;  Wright, Ian J.;  Weng, Ensheng;  Liu, Hui;  Zhu, Shidan;  Lu, Mingzhen;  Luo, Qi;  Li, Ronghua;  Wu, Guilin;  Yan, Enrong;  Song, Yanjun;  Mi, Xiangcheng;  Hao, Guangyou;  Reich, Peter B.;  Wang, Yingping;  Ellsworth, David S.;  Ye, Qing
收藏  |  浏览/下载:12/0  |  提交时间:2020/02/17
biome  climate  functional types  hydraulic diversity  species distribution  water transport  
The spatial frequency of climatic conditions affects niche composition and functional diversity of species assemblages: the case of Angiosperms 期刊论文
ECOLOGY LETTERS, 2020, 23 (2) : 254-264
作者:  Fournier, Bertrand;  Vazquez-Rivera, Hector;  Clappe, Sylvie;  Donelle, Louis;  Braga, Pedro Henrique Pereira;  Peres-Neto, Pedro R.
收藏  |  浏览/下载:8/0  |  提交时间:2020/07/02
Angiosperms  climate frequency  climate heterogeneity  functional diversity  functional trait  generalist  niche breadth  specialist  
The spatial frequency of climatic conditions affects niche composition and functional diversity of species assemblages: the case of Angiosperms 期刊论文
ECOLOGY LETTERS, 2020, 23 (2) : 254-264
作者:  Fournier, Bertrand;  Vazquez-Rivera, Hector;  Clappe, Sylvie;  Donelle, Louis;  Braga, Pedro Henrique Pereira;  Peres-Neto, Pedro R.
收藏  |  浏览/下载:14/0  |  提交时间:2020/02/17
Angiosperms  climate frequency  climate heterogeneity  functional diversity  functional trait  generalist  niche breadth  specialist  
The many dimensions of phytochemical diversity: linking theory to practice 期刊论文
ECOLOGY LETTERS, 2019
作者:  Wetzel, William C.;  Whitehead, Susan R.
收藏  |  浏览/下载:10/0  |  提交时间:2020/02/17
Beta diversity  chemical ecology  functional diversity  Phytochemical diversity  plant secondary metabolism  plant-insect interactions  scale  species interactions  trait variability