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科学期刊 - Nature 系列 - Nature挂了 #10448

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http://localhost:1200/nature/research/nature - Success ```rss <![CDATA[Nature (Nature) | Latest Research]]> https://www.nature.com/nature/research-articles RSSHub i@diygod.me (DIYgod) zh-cn Fri, 12 Aug 2022 12:21:01 GMT 5 <![CDATA[An Asymmetric sp3–sp3 Cross-Electrophile Coupling Using ‘Ene’-Reductases]]>

Abstract

The catalytic asymmetric construction of Csp3–Csp3 bonds remains one of the foremost challenges in organic synthesis.1 Metal-catalyzed cross-electrophile couplings (XEC) have emerged as a powerful tool for C–C bond formation.2-5 However, coupling two distinct Csp3-electrophiles with high cross- and stereoselectivity continues as an unmet challenge. Here, we report a highly chemo- and enantioselective Csp3–Csp3 XEC between alkyl halides and nitroalkanes catalyzed by flavin-dependent ‘ene’-reductases. Photoexcitation of the enzyme-templated charge-transfer complex between an alkyl halide and flavin cofactor enables the chemoselective reduction of alkyl halide over the thermodynamically favored nitroalkane partner. The key C–C bond-forming step occurs via the reaction of an alkyl radical with an in situ generated nitronate to form a nitro radical anion that collapses to form nitrite and an alkyl radical. An enzyme-controlled hydrogen atom transfer affords high levels of enantioselectivity. This reactivity is unknown in small molecule catalysis and highlights the potential for enzymes to use new mechanisms to address long-standing synthetic challenges.

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Authors and Affiliations

  1. Department of Chemistry and Chemical Biology, Cornell University, Ithaca, New York, USA

    Haigen Fu, Jingzhe Cao, Tianzhang Qiao & Todd K. Hyster

  2. Department of Chemistry, Princeton University, Princeton, New Jersey, USA

    Jingzhe Cao & Samuel Garfinkle

  3. Prozomix. Building 4, West End Ind. Estate, Haltwhistle, Northumberland, UK

    Yuyin Qi & Simon J. Charnock

Authors
  1. Haigen Fu
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  2. Jingzhe Cao
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  3. Tianzhang Qiao
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  4. Yuyin Qi
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  5. Simon J. Charnock
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  6. Samuel Garfinkle
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  7. Todd K. Hyster
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Corresponding author

Correspondence to Todd K. Hyster.

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Fu, H., Cao, J., Qiao, T. et al. An Asymmetric sp3–sp3 Cross-Electrophile Coupling Using ‘Ene’-Reductases. Nature (2022). https://doi.org/10.1038/s41586-022-05167-1

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  • DOI: https://doi.org/10.1038/s41586-022-05167-1

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]]> Thu, 11 Aug 2022 00:00:00 GMT https://www.nature.com/articles/s41586-022-05167-1 https://www.nature.com/articles/s41586-022-05167-1 Biocatalysis Photocatalysis Science Humanities and Social Sciences multidisciplinary <![CDATA[Pandemic-Scale Phylogenomics Reveals The SARS-CoV-2 Recombination Landscape]]>

Abstract

Accurate and timely detection of recombinant lineages is crucial for interpreting genetic variation, reconstructing epidemic spread, identifying selection and variants of interest, and accurately performing phylogenetic analyses 1–4. During the SARS-CoV-2 pandemic, genomic data generation has exceeded the capacities of existing analysis platforms, thereby crippling real-time analysis of viral evolution 5. Here, we use a novel phylogenomic method to search a nearly comprehensive SARS-CoV-2 phylogeny for recombinant lineages. In a 1.6M sample tree from May 2021, we identify 589 recombination events, which indicate that approximately 2.7% of sequenced SARS-CoV-2 genomes have detectable recombinant ancestry. Recombination breakpoints are inferred to occur disproportionately in the 3’ portion of the genome that contains the spike protein. Our results highlight the need for timely analyses of recombination for pinpointing the emergence of recombinant lineages with the potential to increase transmissibility or virulence of the virus. We anticipate that this approach will empower comprehensive real time tracking of viral recombination during the SARS-CoV-2 pandemic and beyond.

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Author notes

  1. These authors contributed equally: Yatish Turakhia and Bryan Thornlow

Authors and Affiliations

  1. Department of Biomolecular Engineering, University of California, Santa Cruz, Santa Cruz, CA, USA

    Yatish Turakhia, Bryan Thornlow, Jakob McBroome, Nicolas Ayala, David Haussler & Russell Corbett-Detig

  2. Genomics Institute, University of California, Santa Cruz, Santa Cruz, CA, USA

    Yatish Turakhia, Bryan Thornlow, Angie Hinrichs, Jakob McBroome, Nicolas Ayala, David Haussler & Russell Corbett-Detig

  3. Department of Electrical and Computer Engineering, University of California, San Diego, San Diego, CA, USA

    Yatish Turakhia & Cheng Ye

  4. Department of Biological Sciences, University of California, San Diego, San Diego, CA, USA

    Kyle Smith

  5. European Molecular Biology Laboratory, European Bioinformatics Institute (EMBL-EBI), Wellcome Genome Campus, Cambridge, UK

    Nicola De Maio

  6. Howard Hughes Medical Institute, University of California, Santa Cruz, Santa Cruz, CA, USA

    David Haussler

  7. Department of Ecology and Evolution, Research School of Biology, Australian National University, Canberra, ACT, Australia

    Robert Lanfear

Authors
  1. Yatish Turakhia
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  2. Bryan Thornlow
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  3. Angie Hinrichs
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  4. Jakob McBroome
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  5. Nicolas Ayala
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  6. Cheng Ye
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  7. Kyle Smith
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  8. Nicola De Maio
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  9. David Haussler
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  10. Robert Lanfear
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  11. Russell Corbett-Detig
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Corresponding authors

Correspondence to Yatish Turakhia or Russell Corbett-Detig.

Supplementary information

Supplementary Information

This file contains Supplementary Text S1-S18 referenced in the main text; legends for Supplementary Tables 1–4 and Supplementary References.

Reporting Summary

Peer Review File

Supplementary Table S1

This file contains acknowledgments recognizing originating laboratories responsible for obtaining the specimens, as well as the submitting laboratories where the genome data were generated and shared via GISAID.

Supplementary Table S2

This file contains acknowledgments recognizing originating and submitting laboratories for data from the China National Center for Bioinformation.

Supplementary Table S3

This file contains acknowledgments recognizing originating and submitting laboratories for data from the COVID-19 Genomics UK (COG-UK) Consortium.

Supplementary Table S4

This file contains acknowledgments recognizing originating and submitting laboratories for data from the National Center for Biotechnology Information database.

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