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physica status solidi (b), Wiley, Vol. 40, No. 2 ( 1970), p. 657-665

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 39, No. 2 ( 1970), p. 515-526

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 18 ( 2022-04-25)

Um das Potenzial von Enzymen in der zellfreien Biokatalyse voll auszuschöpfen, ist eine Stabilisierung der katalytisch aktiven Proteine und deren Integration in effiziente Reaktorsysteme erforderlich. Obwohl in den letzten Jahren erste Schritte zur Immobilisierung solcher Biomoleküle in metallorganischen Gerüsten (MOFs) unternommen wurden, waren diese Demonstrationen auf Batch‐Experimente und wässrige Bedingungen beschränkt. Hier demonstrieren wir ein kontinuierliches Enzymreaktorsystem auf MOF‐Basis mit hoher Produktivität und Stabilität, das auch für organische Lösungsmittel geeignet ist. Unter wässrigen Bedingungen wurde die Stabilität des Enzyms um das 30‐fache erhöht, und die Raum‐Zeit‐Ausbeute übertraf die mit anderen Enzym‐Immobilisierungsstrategien erzielten Werte um eine Größenordnung. Es ist herauszuheben, dass die hier gezeigte Infiltration der Proteine in das MOF keine zusätzliche Funktionalisierung erfordert, was eine zeit‐ und kosteneffiziente Herstellung der Biokatalysatoren mit markierungsfreien Enzymen ermöglicht.

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7

physica status solidi (b), Wiley, Vol. 39, No. 1 ( 1970), p. 61-65

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 39, No. 2 ( 1970), p. 531-537

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 40, No. 2 ( 1970), p. 687-690

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 39, No. 2 ( 1970), p. 539-550

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 39, No. 1 ( 1970), p. 95-107

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 40, No. 2 ( 1970), p. 717-724

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 15 ( 2022-04-04)

A rational approach towards precision two‐dimensional (2D) assemblies by crystallization‐driven self‐assembly (CDSA) of poly(L‐lactides) (PLLAs), end‐capped with dipolar dyes like merocyanine (MC) or naphthalene monoimide (NMI) and hydrophobic pyrene (PY) or benzene (Bn) is described. PLLA chains crystallize into diamond‐shaped platelets in isopropanol, which forces the terminal dyes to assemble into a 2D array on the platelet surface by either dipolar interactions or π‐stacking and exhibit tunable emission. Dipolar dyes play a critical role in imparting colloidal stability and structural uniformity to the 2D crystals, which is partly compromised for hydrophobic ones. Co‐crystallization between NMI‐ and PY‐labeled PLLAs yields similar diamond‐shaped co‐platelets with highly efficient (≈80 %) Förster Resonance Energy Transfer on the 2D surface. Further, the “living” CDSA method confers enlarged, segmented block co‐platelets using one of the homopolymers as “seed” and the other as “unimer”.

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7

Angewandte Chemie, Wiley, Vol. 134, No. 15 ( 2022-04-04)

Analyzing complex single‐nucleotide‐polymorphism (SNP) combinations in the genome is important for research and clinical applications, given that different SNP combinations can generate different phenotypic consequences. Recent works have shown that DNA‐based molecular computing is powerful for simultaneously sensing and analyzing complex molecular information. Here, we designed a switching circuit‐based DNA computational scheme that can integrate the sensing of multiple SNPs and simultaneously perform logical analysis of the detected SNP information to directly report clinical outcomes. As a demonstration, we successfully achieved automatic and accurate identification of 21 different blood group genotypes from 83 clinical blood samples with 100 % accuracy compared to sequencing data in a more rapid manner (3 hours). Our method enables a new mode of automatic and logical sensing and analyzing subtle molecular information for clinical diagnosis, as well as guiding personalized medication.

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7

physica status solidi (b), Wiley, Vol. 39, No. 2 ( 1970), p. 581-598

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 14 ( 2022-03-28)

Herein, a general procedure for the synthesis of multifunctional MRs, which simultaneously exhibit i) chiral, ii) magnetic, and iii) fluorescent properties in combination with iv) self‐propulsion, is reported. Self‐propelled Ni@Pt superparamagnetic microrockets have been functionalized with fluorescent CdS quantum dots carrying a chiral host biomolecule as β‐cyclodextrin (β‐CD). The “on‐the‐fly” chiral recognition potential of MRs has been interrogated by taking advantage of the β‐CD affinity to supramolecularly accommodate different chiral biomolecules (i.e., amino acids). As a proof‐of‐concept, tryptophan enantiomers have been discriminated with a dual‐mode (optical and electrochemical) readout. This approach paves the way to devise intelligent cargo micromachines with “built‐in” chiral supramolecular recognition capabilities to elucidate the concept of “enantiorecognition‐on‐the‐fly”, which might be facilely customized by tailoring the supramolecular host–guest encapsulation.

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7

Angewandte Chemie, Wiley, Vol. 134, No. 16 ( 2022-04-11)

In vivo microelectrodes are essential for neuroscience studies. However, development of microelectrodes with both flexibility and multifunctionality for recording chemical and electrical signals in the same extracellular microspace and modulating neural activity remains challenging. Here, we find that pure PEDOT:PSS fibers (i.e., support‐free) exhibit high conductivity, fast heterogeneous electron transfer, and suitable charge storage and injection capabilities, and can thus directly act as microelectrodes not only for chemical and electrophysiological recording in the same extracellular microspace, but also for electromodulation of neural microcircuit activity. Moreover, the microelectrodes mechanically match with neural tissues, exhibiting less foreign body responses. Given the multifunctionality, flexibility, and biocompatibility, the support‐free PEDOT:PSS‐based microelectrodes offer a new avenue to microelectrode technology for neuroscience research, diagnostics and therapeutics.

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7

Angewandte Chemie, Wiley, Vol. 134, No. 14 ( 2022-03-28)

Carboxyl methyltransferase (CMT) enzymes catalyse the biomethylation of carboxylic acids under aqueous conditions and have potential for use in synthetic enzyme cascades. Herein we report that the enzyme FtpM from Aspergillus fumigatus can methylate a broad range of aromatic mono‐ and dicarboxylic acids in good to excellent conversions. The enzyme shows high regioselectivity on its natural substrate fumaryl‐ l ‐tyrosine, trans , trans ‐muconic acid and a number of the dicarboxylic acids tested. Dicarboxylic acids are generally better substrates than monocarboxylic acids, although some substituents are able to compensate for the absence of a second acid group. For dicarboxylic acids, the second methylation shows strong pH dependency with an optimum at pH 5.5–6. Potential for application in industrial biotechnology was demonstrated in a cascade for the production of a bioplastics precursor (FDME) from bioderived 5‐hydroxymethylfurfural (HMF).

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7

physica status solidi (b), Wiley, Vol. 40, No. 1 ( 1970), p. 257-266

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 16 ( 2022-04-11)

D‐Luciferin (D‐LH 2 ), a substrate of firefly luciferase (Fluc), is important for a wide range of bioluminescence applications. This work reports a new and green method using enzymatic reactions (HELP, HadA Enzyme for Luciferin Preparation) to convert 19 phenolic derivatives to 8 D‐LH 2 analogues with ≈51 % yield. The method can synthesize the novel 5′‐methyl‐D‐LH 2 and 4′,5′‐dimethyl‐D‐LH 2 , which have never been synthesized or found in nature. 5′‐Methyl‐D‐LH 2 emits brighter and longer wavelength light than the D‐LH 2 . Using HELP, we further developed LUMOS (Luminescence Measurement of Organophosphate and Derivatives) technology for in situ detection of organophosphate pesticides (OPs) including parathion, methyl parathion, EPN, profenofos, and fenitrothion by coupling the reactions of OPs hydrolase and Fluc. The LUMOS technology can detect these OPs at parts per trillion (ppt) levels. The method can directly detect OPs in food and biological samples without requiring sample pretreatment.

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7

Angewandte Chemie, Wiley, Vol. 134, No. 18 ( 2022-04-25)

Most metal–organic frameworks (MOFs) lack charge mobility, which is crucial for realizing their use in optoelectronic applications. This work proposes the design of a MOF using triarylamine‐based ligands (Zr‐NBP) as the lone pair electron spacer to enhance the hole mobility in the MOF while maintaining its luminescent properties. Zr‐NBP has strong fluorescence with a good hole mobility of 1.05×10 −6  cm 2  V −1  s −1 , which is comparable to organic materials used in optoelectronic devices. We also employed a Zr‐NBP nanofilm in the pure phase as both a non‐doped emissive layer and a hole‐transporting layer within organic light‐emitting diodes (OLEDs). The obtained OLED device produced a bright green light with a low turn‐on voltage of 3.9 V. This work presents an advance in developing the electronic properties of MOFs by modifying the chemical properties of its building blocks, and will likely inspire further design of MOF materials as active layers in optoelectronic devices.

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7

physica status solidi (b), Wiley, Vol. 40, No. 1 ( 1970), p. 267-270

Online Resource

0370-1972, 1521-3951

German

Wiley

1970

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 21 ( 2022-05-16)

At the forefront of chemistry and biology research, development timelines are fast‐paced and large quantities of pure targets are rarely available. Herein, we introduce a new framework, which is built upon an automated, online trapping‐enrichment multi‐dimensional liquid chromatography platform (TE‐ Dt ‐mDLC) that enables: 1) highly efficient separation of complex mixtures in a first dimension ( 1 D ‐UV); 2) automated peak trapping‐enrichment and buffer removal achieved through a sequence of H 2 O and D 2 O washes using an independent pump setup; and 3) a second dimension separation ( 2 D ‐UV‐MS) with fully deuterated mobile phases and fraction collection to minimize protic residues for immediate NMR analysis while bypassing tedious drying processes and minimizing analyte degradation. Diverse examples of target isolation and characterization from organic synthesis and natural product chemistry laboratories are illustrated, demonstrating recoveries above 90 % using as little as a few micrograms of material.

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7