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An engineered PET depolymerase to break down and recycle plastic bottles 期刊论文
NATURE, 2020, 580 (7802) : 216-+
作者:  Zhao, Evan Wenbo;  Liu, Tao;  Jonsson, Erlendur;  Lee, Jeongjae;  Temprano, Israel;  Jethwa, Rajesh B.;  Wang, Anqi;  Smith, Holly;  Carretero-Gonzalez, Javier;  Song, Qilei;  Grey, Clare P.
收藏  |  浏览/下载:86/0  |  提交时间:2020/07/03

Present estimates suggest that of the 359 million tons of plastics produced annually worldwide(1), 150-200 million tons accumulate in landfill or in the natural environment(2). Poly(ethylene terephthalate) (PET) is the most abundant polyester plastic, with almost 70 million tons manufactured annually worldwide for use in textiles and packaging(3). The main recycling process for PET, via thermomechanical means, results in a loss of mechanical properties(4). Consequently, de novo synthesis is preferred and PET waste continues to accumulate. With a high ratio of aromatic terephthalate units-which reduce chain mobility-PET is a polyester that is extremely difficult to hydrolyse(5). Several PET hydrolase enzymes have been reported, but show limited productivity(6,7). Here we describe an improved PET hydrolase that ultimately achieves, over 10 hours, a minimum of 90 per cent PET depolymerization into monomers, with a productivity of 16.7 grams of terephthalate per litre per hour (200 grams per kilogram of PET suspension, with an enzyme concentration of 3 milligrams per gram of PET). This highly efficient, optimized enzyme outperforms all PET hydrolases reported so far, including an enzyme(8,9) from the bacterium Ideonella sakaiensis strain 201-F6 (even assisted by a secondary enzyme(10)) and related improved variants(11-14) that have attracted recent interest. We also show that biologically recycled PET exhibiting the same properties as petrochemical PET can be produced from enzymatically depolymerized PET waste, before being processed into bottles, thereby contributing towards the concept of a circular PET economy.


Computer-aided engineering produces improvements to an enzyme that breaks down poly(ethylene terephthalate) (PET) into its constituent monomers, which are used to synthesize PET of near-petrochemical grade that can be further processed into bottles.


  
Copper-mediated synthesis of drug-like bicyclopentanes 期刊论文
NATURE, 2020, 580 (7802) : 220-+
作者:  Canavelli, Pierre;  Islam, Saidul;  Powner, Matthew W.
收藏  |  浏览/下载:8/0  |  提交时间:2020/07/03

Multicomponent reactions are relied on in both academic and industrial synthetic organic chemistry owing to their step- and atom-economy advantages over traditional synthetic sequences(1). Recently, bicyclo[1.1.1]pentane (BCP) motifs have become valuable as pharmaceutical bioisosteres of benzene rings, and in particular 1,3-disubstituted BCP moieties have become widely adopted in medicinal chemistry as para-phenyl ring replacements(2). These structures are often generated from [1.1.1]propellane via opening of the internal C-C bond through the addition of either radicals or metal-based nucleophiles(3-13). The resulting propellane-addition adducts are then transformed to the requisite polysubstituted BCP compounds via a range of synthetic sequences that traditionally involve multiple chemical steps. Although this approach has been effective so far, a multicomponent reaction that enables single-step access to complex and diverse polysubstituted drug-like BCP products would be more time efficient compared to current stepwise approaches. Here we report a one-step three-component radical coupling of [1.1.1]propellane to afford diverse functionalized bicyclopentanes using various radical precursors and heteroatom nucleophiles via a metallaphotoredox catalysis protocol. This copper-mediated reaction operates on short timescales (five minutes to one hour) across multiple (more than ten) nucleophile classes and can accommodate a diverse array of radical precursors, including those that generate alkyl, alpha-acyl, trifluoromethyl and sulfonyl radicals. This method has been used to rapidly prepare BCP analogues of known pharmaceuticals, one of which is substantially more metabolically stable than its commercial progenitor.


A one-step, three-component radical coupling of [1.1.1]propellane by a photoredox reaction mediated by a copper catalyst produces drug-like bicyclopentanes.


  
Complexity-based approach for El Nino magnitude forecasting before the spring predictability barrier 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2020, 117 (1) : 177-183
作者:  Meng, Jun;  Fan, Jingfang;  Ludescher, Josef;  Agarwal, Ankit;  Chen, Xiaosong;  Bunde, Armin;  Kurths, Juergen;  Schellnhuber, Hans Joachim
收藏  |  浏览/下载:9/0  |  提交时间:2020/05/13
ENSO  system complexity  entropy  spring barrier  forecasting  
Anti-Markovnikov alcohols via epoxide hydrogenation through cooperative catalysis 期刊论文
SCIENCE, 2019, 364 (6442) : 764-+
作者:  Yao, Chengbo;  Dahmen, Tobias;  Gansaeuer, Andreas;  Norton, Jack
收藏  |  浏览/下载:26/0  |  提交时间:2019/11/27
Rare earth elements: Mendeleev's bane, modern marvels 期刊论文
SCIENCE, 2019, 363 (6426) : 489-493
作者:  Cheisson, Thibault;  Schelter, Eric J.
收藏  |  浏览/下载:9/0  |  提交时间:2019/11/27
Night-sky radiometry can revolutionize the characterization of light-pollution sources globally 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (16) : 7712-7717
作者:  Kocifaj, Miroslav;  Antonio Solano-Lamphar, Hector;  Videen, Gorden
收藏  |  浏览/下载:5/0  |  提交时间:2019/11/27
skyglow  night-sky radiometry  light-pollution sources  upward emission function  
Economic carbon cycle feedbacks may offset additional warming from natural feedbacks 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (3) : 759-764
作者:  Woodard, Dawn L.;  Davis, Steven J.;  Randerson, James T.
收藏  |  浏览/下载:9/0  |  提交时间:2019/11/27
carbon cycle feedbacks  climate change  economic damages  integrated assessment models  fossil fuels  
Fine particulate matter damages and value added in the US economy 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (40) : 19857-19862
作者:  Tschofen, Peter;  Azevedo, Ines L.;  Muller, Nicholas Z.
收藏  |  浏览/下载:10/0  |  提交时间:2019/11/27
externalities  air pollution  environmental accounting  value added  environmental policy  
Economic resilience of Carthage during the Punic Wars: Insights from sediments of the Medjerda delta around Utica (Tunisia) 期刊论文
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2019, 116 (20) : 9764-9769
作者:  Delile, Hugo;  Pleuger, Elisa;  Blichert-Toft, Janne;  Goiran, Jean-Philippe;  Fagel, Nathalie;  Gadhoum, Ahmed;  Abichou, Abdelhakim;  Ben Jerbania, Imed;  Fentress, Elizabeth;  Wilson, Andrew I.
收藏  |  浏览/下载:10/0  |  提交时间:2019/11/27
paleopollution  mining resources  Medjerda river  Punic Wars  Utica  
Flawed analyses of US auto fuel economy standards A 2018 analysis discarded at least $112 billion in benefits 期刊论文
SCIENCE, 2018, 362 (6419) : 1119-+
作者:  Bento, Antonio M.;  Gillinghan, Kenneth;  Jacobsen, Mark R.;  Knittel, Christopher R.;  Leard, Benjamin;  Linn, Joshua;  McConnell, Virginia;  Rapson, David;  Sallee, James M.;  van Benthem, Arthur A.;  Whitefoot, Kate S.
收藏  |  浏览/下载:11/0  |  提交时间:2019/11/27