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1.
J Am Chem Soc ; 140(1): 388-393, 2018 01 10.
Artigo em Inglês | MEDLINE | ID: mdl-29211458

RESUMO

Developing dopant-free hole transporting layers (HTLs) is critical in achieving high-performance and robust state-of-the-art perovskite photovoltaics, especially for the air-sensitive tin-based perovskite systems. The commonly used HTLs require hygroscopic dopants and additives for optimal performance, which adds extra cost to manufacturing and limits long-term device stability. Here we demonstrate the use of a novel tetrakis-triphenylamine (TPE) small molecule prepared by a facile synthetic route as a superior dopant-free HTL for lead-free tin-based perovskite solar cells. The best-performing tin iodide perovskite cells employing the novel mixed-cation ethylenediammonium/formamidinium with the dopant-free TPE HTL achieve a power conversion efficiency as high as 7.23%, ascribed to the HTL's suitable band alignment and excellent hole extraction/collection properties. This efficiency is one of the highest reported so far for tin halide perovskite systems, highlighting potential application of TPE HTL material in low-cost high-performance tin-based perovskite solar cells.

2.
Angew Chem Int Ed Engl ; 55(16): 5058-61, 2016 Apr 11.
Artigo em Inglês | MEDLINE | ID: mdl-26971709

RESUMO

The majority of lysosomal enzymes are targeted to the lysosome by post-translational tagging with N-glycans terminating in mannose-6-phosphate (M6P) residues. Some current enzyme replacement therapies (ERTs) for lysosomal storage disorders are limited in their efficacy by the extent to which the recombinant enzymes bear the M6P-terminated glycans required for effective trafficking. Chemical synthesis was combined with endo-ß-N-acetylglucosaminidase (ENGase) catalysis to allow the convergent synthesis of glycosyl amino acids bearing M6P residues. This approach can be extended to the remodeling of proteins, as exemplified by RNase. The powerful synergy of chemical synthesis and ENGase-mediated biocatalysis enabled the first synthesis of a glycoprotein bearing M6P-terminated N-glycans in which the glycans are attached to the peptide backbone by entirely natural linkages.


Assuntos
Glicoproteínas/síntese química , Acetilglucosaminidase/química , Sequência de Carboidratos , Glicoproteínas/química , Fosforilação
3.
Chem Commun (Camb) ; 53(43): 5898-5901, 2017 May 30.
Artigo em Inglês | MEDLINE | ID: mdl-28513666

RESUMO

Three new organic semiconductors with alkyl chain-substituted tetrathienoacene (TTAR) as the central core and both ends capped with thiophene (DT-TTAR), thienothiophene (DTT-TTAR) and dithienothiophene (DDTT-TTAR) have been synthesized and characterized for organic field effect transistor (OFET) applications. A hole mobility of 0.81 cm2 V-1 s-1 was achieved for the DDTT-TTAR film, which represents the highest mobility yet found for a solution-processable p-type TTAR-based small molecular semiconductors.

4.
Adv Mater ; 29(35)2017 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-28707742

RESUMO

New 3,3'-dithioalkyl-2,2'-bithiophene (SBT)-based small molecular and polymeric semiconductors are synthesized by end-capping or copolymerization with dithienothiophen-2-yl units. Single-crystal, molecular orbital computations, and optical/electrochemical data indicate that the SBT core is completely planar, likely via S(alkyl)⋯S(thiophene) intramolecular locks. Therefore, compared to semiconductors based on the conventional 3,3'-dialkyl-2,2'-bithiophene, the resulting SBT systems are planar (torsional angle <1°) and highly π-conjugated. Charge transport is investigated for solution-sheared films in field-effect transistors demonstrating that SBT can enable good semiconducting materials with hole mobilities ranging from ≈0.03 to 1.7 cm2 V-1 s-1 . Transport difference within this family is rationalized by film morphology, as accessed by grazing incidence X-ray diffraction experiments.

5.
Carbohydr Res ; 426: 40-5, 2016 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-27058295

RESUMO

Endo-ß-N-acetylglucosaminidases (ENGases) are versatile biocatalysts that allow access to a wide variety of defined homogenous N-linked glycoconjugates in a convergent manner. A hybrid-type N-glycan was accessed by total synthesis, converted to an oxazoline, and used as a donor substrate with both wild type Endo M and an N175Q glycosynthase Endo M mutant allowing the convergent synthesis of a glycosylated amino acid bearing a hybrid N-glycan structure.


Assuntos
Biocatálise , Manosil-Glicoproteína Endo-beta-N-Acetilglucosaminidase/metabolismo , Oxazóis/química , Oxazóis/metabolismo , Polissacarídeos/biossíntese , Polissacarídeos/química , Configuração de Carboidratos , Glicosilação , Manosil-Glicoproteína Endo-beta-N-Acetilglucosaminidase/química , Manosil-Glicoproteína Endo-beta-N-Acetilglucosaminidase/genética
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