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1.
Nat Commun ; 14(1): 3198, 2023 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-37268636

RESUMO

The development of chemically recyclable polymers serves as an attractive approach to address the global plastic pollution crisis. Monomer design principle is the key to achieving chemical recycling to monomer. Herein, we provide a systematic investigation to evaluate a range of substitution effects and structure-property relationships in the ɛ-caprolactone (CL) system. Thermodynamic and recyclability studies reveal that the substituent size and position could regulate their ceiling temperatures (Tc). Impressively, M4 equipped with a tert-butyl group displays a Tc of 241 °C. A series of spirocyclic acetal-functionalized CLs prepared by a facile two-step reaction undergo efficient ring-opening polymerization and subsequent depolymerization. The resulting polymers demonstrate various thermal properties and a transformation of the mechanical performance from brittleness to ductility. Notably, the toughness and ductility of P(M13) is comparable to the commodity plastic isotactic polypropylene. This comprehensive study is aimed to provide a guideline to the future monomer design towards chemically recyclable polymers.

2.
ACS Macro Lett ; 11(2): 173-178, 2022 Feb 15.
Artigo em Inglês | MEDLINE | ID: mdl-35574765

RESUMO

Monomer design plays an important role in the development of polymers with desired thermal properties and chemical recyclability. Here we prepared a class of seven-membered ring carbonates containing trans-cyclohexyl fused rings. These monomers showed excellent activity for ring-opening polymerization (ROP) with turnover frequency (TOF) up to 6 × 105 h-1 and catalyst loading down to 50 ppm, which yielded high-molecular-weight polycarbonates (Mn up to 673 kg/mol) with great thermostability (Td > 300 °C). Ultimately, the resulting polycarbonates can completely depolymerize into their corresponding cyclic dimers that can repolymerize to synthesize the starting polymers in moderate yields, demonstrating a potential route to achieve chemical recycling. Postfunctionalization of the unsaturated polycarbonate was conducted through cross-linking reaction and "click" reaction under UV irradiation.

3.
Org Biomol Chem ; 18(25): 4843-4847, 2020 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-32608447

RESUMO

A simple and practical method for the synthesis of phosphoryl-substituted indolo[2,1-a]isoquinolin-6(5H)-ones and benzimidazo[2,1-a]isoquinolin-6(5H)-ones through manganese(iii)-promoted tandem phosphinoylation/cyclization of 2-arylindoles or 2-arylbenzimidazoles with disubstituted phosphine oxides was developed. In this transformation, new C-P bond and C-C bond were constructed simultaneously under silver-free conditions, exhibiting a broad substrate scope. It was noted that not only diarylphosphine oxides but also dialkyl and arylalkyl-phosphine oxides were compatible with the conditions.

4.
Chem Commun (Camb) ; 56(55): 7585-7588, 2020 Jul 14.
Artigo em Inglês | MEDLINE | ID: mdl-32510076

RESUMO

A new external oxidant-free electrochemical dehydrogenative cross-coupling of xanthenes and ketones for the preparation of functionalized 9-alkyl-9H-xanthenes was developed. This method enables the formation of a new C(sp3)-C(sp3) bond through release of H2 as the major byproduct at room temperature, and features mild conditions, high atom economy, excellent functional-group tolerance, scalability and facile applications in pharmaceutical chemistry.

5.
Org Biomol Chem ; 18(11): 2170-2174, 2020 03 18.
Artigo em Inglês | MEDLINE | ID: mdl-32140694

RESUMO

A copper-catalyzed C-H [3 + 2] annulation of N-substituted anilines with α-carbonyl alkyl bromides for the synthesis of 3,3'-disubstituted oxindoles is developed. Tandem C-H cycloamidation reactions of various α-carbonyl alkyl bromide derivatives including tertiary-α-bromoalkyl ketone esters, malonic esters and cycloalkanes, with N-aryl or alkyl substituted anilines, can be performed using this system, affording a vast array of valuable 3,3'-disubstituted oxindoles in moderate to good yields.

6.
Chem Commun (Camb) ; 55(85): 12805-12808, 2019 Nov 04.
Artigo em Inglês | MEDLINE | ID: mdl-31595274

RESUMO

A new silver-mediated 1,2-alkylesterification of alkenes with nitriles and acids promoted by a catalytic amount of nickel catalyst for producing acyloxylated nitriles has been developed via a C(sp3)-H functionalization process. By employing the NiI2 and Ag2CO3 catalytic systems, the method features broad substrate scope with respect to carboxylic acids, including linear alkyl acids, cyclic acids, aryl acids and amino acids.

7.
Chem Commun (Camb) ; 55(61): 8995-8998, 2019 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-31290859

RESUMO

A new, practical directed anodic C-H sulfonylation of N,N-disubstituted anilines with sodium sulfinates for producing o- or p-amino arylsulfones and diarylsulfones is described. Employing the anodic strategy, the reaction proceeds efficiently under mild (room temperature) and transition-metal- and chemical oxidant-free conditions, and enables the formation of C-S bonds via directed activation of ortho- or para-C-H bond to the amino group with broad substrate scope and excellent site selectivity.

8.
Chem Commun (Camb) ; 55(30): 4371-4374, 2019 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-30912541

RESUMO

A highly para-selective amination of anilines with phenothiazines for producing various functionalized 10-aryl-10H-phenothiazines is reported. The oxidative amination reaction proceeds electrochemically at room temperature, thereby avoiding the use of metals and oxidizing reagents with excellent functional group tolerance and broad substrate scope.

9.
Artigo em Chinês | WPRIM (Pacífico Ocidental) | ID: wpr-318897

RESUMO

Schizophrenia (MIM 181500) is a complex disorder affecting approximately 1% of the population worldwide. Epidemiologic evidences, together with recent linkage and association studies, have clearly demonstrated the high heritability of schizophrenia (up to 80%). Uncovering the genetic mechanism of schizophrenia has became one of the greatest challenges for both psychiatry and genetics. In recent years, remarkable advances in the genetics of this disorder has been achieved with the rapid growth of human genome information and experiment technologies. Several candidate genes within some of the best-supported linkage regions have been reported and, more importantly, replicated. Moreover, these genes present a significant connection in the signaling pathways implicated in the development of schizophrenia, especially NMDA receptor-mediated glutamate transmission. In this review, we summarize the recent advances in the genetics of schizophrenia, focusing particularly on linkage disequilibrium analysis and the latest understanding of the neurobiology of the disorder.


Assuntos
Humanos , Aciltransferases , Genética , Proteínas de Transporte , Genética , Disbindina , Proteínas Associadas à Distrofina , Proteínas de Membrana , Genética , Proteínas do Tecido Nervoso , Genética , Neuregulina-1 , Receptores de N-Metil-D-Aspartato , Genética , Esquizofrenia , Genética
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