Search Results

Angewandte Chemie, Wiley, Vol. 133, No. 51 ( 2021-12-13)

Online Resource

0044-8249, 1521-3757

English

Wiley

2021

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7

Physica Status Solidi (b), Wiley, Vol. 29, No. 1 ( 1968), p. K63-K64

Online Resource

0370-1972, 1521-3951

German

Wiley

1968

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 12 ( 2022-03-14)

Nitric acid is widely applied in agriculture and industry. The present manufacturing process via a combination of the Haber–Bosch process and the Ostwald oxidation process is accompanied by massive energy consumption and greenhouse gas emissions. The direct electrocatalytic nitrogen oxidation reaction (NOR) to nitric acid is a promising alternative, especially when it is driven by renewable energy sources. The standardization of performance evaluation is the prerequisite for the design and synthesis of efficient electrocatalysts for NOR. In this context, this Minireview first discusses the history of the development of HNO 3 manufacturing and the possible reaction mechanisms for electrocatalytic NOR. Then, a strict protocol for electrochemical NOR experiments is recommended. Finally, general research targets associated with techno‐economic analysis, challenges, and prospects for NOR are summarized for future studies.

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. 32, No. 1 ( 1969), p. 331-336

Online Resource

0370-1972, 1521-3951

German

Wiley

1969

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 33, No. 1 ( 1969-01), p. 91-102

Measurements of the thermal depolarization current (ITC) in V‐, Cr‐, Mn‐, Fe‐, Co‐, Ni‐, Cd‐, and Pb‐doped AgCl single crystals are reported. These currents show a maximum near 110°K and are caused by the thermal reorientation of the impurity cation–vacancy dipoles upon warming up (2°K/min), following a partial orientation by a static field at low temperature. From these electrical “glow curves”, the activation enthalpies for orientation jumps and the frequency factors may be evaluated as well as the dipole moments if the number of dipoles is known. Ni, Cd, and Pb additions yield simple ITC curves with one maximum. The more involved curves obtained with the other additions are decomposed into two single ITC bands. The corresponding two relaxation modes originate from the occupation of n.n. and n.n.n. sites by the vacancies, relative to the impurity ions.

Online Resource

0370-1972, 1521-3951

English

Wiley

1969

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 6 ( 2022-02)

A series of solid supramolecules based on acrylamide–phenylpyridium copolymers with various substituent groups (P−R: R=−CN, −CO 2 Et, −Me, −CF 3 ) and cucurbit[7]uril (CB[7] ) are constructed to exhibit tunable second‐level (from 0.9 s to 2.2 s) room‐temperature phosphorescence (RTP) in the amorphous state. Compared with other solid supramolecules P−R/CB[7] (R=−CN, −CO 2 Et, −Me), P−CF 3 /CB[7] displays the longest lifetime (2.2 s), which is probably attributed to the fluorophilic interaction of cucurbiturils leading to a uncommon host–guest interaction between 4‐phenylpyridium with −CF 3 and CB[7]. Furthermore, the RTP solid supramolecular assembly (donors) can further react with organic dyes Eosin Y or SR101 (acceptors) to form ternary supramolecular systems featuring ultralong phosphorescence energy transfer (PpET) and visible delayed fluorescence (yellow for EY at 568 nm and red for SR101 at 620 nm). Significantly, the ultralong multicolor PpET supramolecular assembly can be further applied in fields of anti‐counterfeiting and information encryption and painting.

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. 10 ( 2022-03)

The chemical reduction of π‐conjugated bilayer nanographene 1 (C 138 H 120 ) with K and Rb in the presence of 18‐crown‐6 affords [K + (18‐crown‐6)(THF) 2 ][{K + (18‐crown‐6)} 2 (THF) 0.5 ][C 138 H 122 3− ] ( 2 ) and [Rb + (18‐crown‐6) 2 ][{Rb + (18‐crown‐6)} 2 (C 138 H 122 3− )] ( 3 ). Whereas K + cations are fully solvent‐separated from the trianionic core thus affording a “naked” 1 .3 − anion, Rb + cations are coordinated to the negatively charged layers of 1 .3 − . According to DFT calculations, the localization of the first two electrons in the helicene moiety leads to an unprecedented site‐specific hydrogenation process at the carbon atoms located on the edge of the helicene backbone. This uncommon reduction‐induced site‐specific hydrogenation provokes dramatic changes in the (electronic) structure of 1 as the helicene backbone becomes more compressed and twisted upon chemical reduction, which results in a clear slippage of the bilayers.

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. 31, No. 2 ( 1969-01), p. 489-492

[Russian Text Ignored].

Online Resource

0370-1972, 1521-3951

English

Wiley

1969

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 32, No. 1 ( 1969), p. 383-390

Online Resource

0370-1972, 1521-3951

German

Wiley

1969

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 6 ( 2022-02)

Herein, we disclose a straightforward, robust, and simple route to access β‐substituted desaturated cyclic amines via an electrochemically driven desaturative β‐functionalization of cyclic amines. This transformation is based on multiple single‐electron oxidation processes using catalytic amounts of ferrocene. The reaction proceeds in the absence of stoichiometric amounts of electrolyte under mild conditions, affording the desired products with high chemo‐ and regioselectivity. The reaction was tolerant of a broad range of substrates and also enables late‐stage β‐C(sp 3 )−H acylation of potentially valuable products. Preliminary mechanistic studies using cyclic voltammetry reveal the key role of ferrocene as a redox mediator in the reaction.

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. 5 ( 2022-01-26)

Cathepsin B (CTSB) is a lysosomal protease that is overexpressed in the early stage of many cancer types. Precise evaluation of CTSB expression in vivo may provide a promising method for the early diagnosis of cancers. By virtue of the high‐resolution PA imaging modality, a “smart” photoacoustic (PA) probe Cypate‐CBT , which can self‐assemble to cypate‐containing nanoparticles in response to abundant GSH and CTSB inside tumor cells, was developed for the sensitive and specific detection of CTSB activity. Compared with unmodified Cypate, our probe Cypate‐CBT exhibited a 4.9‐fold or 4.7‐fold PA signal enhancement in CTSB‐overexpressing MDA‐MB‐231 cancer cells or tumors, respectively, revealing intracellular accumulation of the probe after CTSB‐initiated self‐assembly. We expect Cypate‐CBT to be employed as an effective PA imaging agent for clinical diagnosis of cancer at early stages.

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. 7 ( 2022-02-07)

Herein, we report a universal boronate‐affinity crosslinking‐amplified dynamic light scattering (DLS) immunoassay for point‐of‐care (POC) glycoprotein detection in complex samples. This enhanced DLS immunoassay consists of two elements, i.e., antibody‐coated magnetic nanoparticles (MNP@mAb) for target capture and DLS signal transduction, and phenylboronic acid‐based boronate‐affinity materials as crosslinking amplifiers. Upon the addition of targets, glycoproteins are first captured by MNP@mAb and amplified by target‐induced crosslinking stemming from the selective binding between the boronic acid ligand and cis ‐diol‐containing glycoprotein, thereby resulting in a remarkably increased DLS signal in the average nanoparticle size. Benefiting from the multivalent binding and fast boronate‐affinity reaction between glycoproteins and crosslinkers, the proposed immunosensing strategy has achieved the ultrasensitive and rapid quantitative assay of glycoproteins at the fM level within 15 min. Overall, this work provides a promising and versatile design strategy for extending the DLS technique to detect glycoproteins even in the field or at POC.

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. 9 ( 2022-02-21)

Accurate quantification of disease‐signature microRNAs (miRNAs) in biomedical samples is in high demand for clinical diagnosis but still challenging because of the low abundance of miRNAs and complicating interferences in the milieus. Here, we report a multi‐amplification strategy based on paper‐spray mass spectrometry (PS MS) for the analysis of miRNAs in blood. A toehold‐mediated DNA‐strand‐displacement reaction (TSD) is employed to amplify the signal chain and to ensure the specificity. The signal chain is then cleaved by UV light to release signal molecules for detection. Moreover, the paper spray method can efficiently filter out interfering substances in the blood and further enhance the sensitivity of detection. This concept is successfully demonstrated in the prototypical detection of the cancer biomarker miRNA‐141 in blood and serum. The proposed TSD‐PS MS approach provides an efficient method for the sensitive detection of oligonucleotides at low concentration in complicated milieus.

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. 32, No. 1 ( 1969), p. 439-442

Online Resource

0370-1972, 1521-3951

German

Wiley

1969

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 32, No. 2 ( 1969-01), p. 715-730

In neun verschiedenen Kristallen mit Steinsalzstruktur wurde die latente Verfestigung als Funktion der Vorspannung untersucht. Die latente Verfestigung eines LiF‐Kristalls wurde auch als Funktion der Temperatur gemessen. Es wurde gefunden, daß das Verhältnis der latenten Verfestigung eines Kristalls von 1,0 bei der Spannung 0 zu einem Maximum bei etwa 0,5 bis 1,5% Kompressionsspannung ansteigt, und dann auf einen konstanten Wert etwas oberhalb 1,0 abfällt. Das Maximum des Verhältnisses der latenten Verfestigung variiert von 3,9 für LiF bis zu 1,2 für AgCl. Die Differenz in der Spannung zwischen dem latenten und dem primären System in LiF bleibt bei allen Temperaturen von 450 bis 4 °K im wesentlichen konstant. Das Verhältnis der latenten Verfestigung bei 0,5% Vorspannung beträgt 3,1 bei 300 °K und 1,6 bei 4 °K. Die latente Verfestigung wurde sogar oberhalb 300 °K beobachtet, wo die Fließspannungen des primären und des latenten Systems von der Deformationsgeschwindigkeit und Temperatur im wesentlichen unabhängig sind. Die Versetzungen, durch Ätzgruben nachgewiesen, waren während des primären Gleitens gleichmäßig verteilt, jedoch durch Bänder mit weiten Zwischenräumen während des latenten Verfestigungsprozesses getrennt. Es wird geschlossen, daß die latente Verfestigung in Kristallen vom Steinsalztyp primär durch die Wechselwirkung der Gleitversetzungen im latenten Gleitsystem mit den Dipolen und Versetzungen im primären Gleitsystem nach der Versetzungsreaktion verursacht wird.

Online Resource

0370-1972, 1521-3951

English

Wiley

1969

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 7 ( 2022-02-07)

Delays in evaluating cancer response to radiotherapy (RT) usually reduce therapy effect or miss the right time for treatment optimization. Hence, exploring timely and accurate methods enabling one to gain insights of RT response are highly desirable. In this study, we have developed an apoptosis enzyme (caspase‐3) activated nanoprobe for early evaluation of RT efficacy. The nanoprobe bridged the nanogapped gold nanoparticles (AuNNPs) and the second near‐infrared window (NIR‐II) fluorescent (FL) molecules (IR‐1048) through a caspase‐3 specific peptide sequence (DEVD) (AuNNP@DEVD‐IR1048). After X‐ray irradiation, caspase‐3 was activated to cut DEVD, turning on both NIR‐II FL and PA imaging signals. The increased NIR‐II FL/PA signals exhibited a positive correlation with the content of caspase‐3. Moreover, the amount of the activated caspase‐3 was negatively correlated with the tumor size. The results underscore the role of the caspase‐3 activated by X‐ray irradiation in bridging the imaging signals variation and tumor inhibition rate. Overall, activatable NIR‐II FL/PA imaging was successfully used to timely predict and evaluate the RT efficacy. The evaluation system based on biomarker‐triggered living imaging has the capacity to guide treatment decisions for numerous cancer types.

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. 9 ( 2022-02-21)

The main protease (M pro ) and papain‐like protease (PL pro ) play critical roles in SARS‐CoV‐2 replication and are promising targets for antiviral inhibitors. The simultaneous visualization of M pro and PL pro is extremely valuable for SARS‐CoV‐2 detection and rapid inhibitor screening. However, such a crucial investigation has remained challenging because of the lack of suitable probes. We have now developed a dual‐color probe (3MBP5) for the simultaneous detection of M pro and PL pro by fluorescence (or Förster) resonance energy transfer (FRET). This probe produces fluorescence from both the Cy3 and Cy5 fluorophores that are cleaved by M pro and PL pro . 3MBP5‐activatable specificity was demonstrated with recombinant proteins, inhibitors, plasmid‐transfected HEK 293T cells, and SARS‐CoV‐2‐infected TMPRSS2‐Vero cells. Results from the dual‐color probe first verified the simultaneous detection and intracellular distribution of SARS‐CoV‐2 M pro and PL pro . This is a powerful tool for the simultaneous detection of different proteases with value for the rapid screening of inhibitors.

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. 32, No. 1 ( 1969), p. 455-458

Online Resource

0370-1972, 1521-3951

German

Wiley

1969

208851-4

1481096-7

physica status solidi (b), Wiley, Vol. 32, No. 2 ( 1969-01), p. 745-748

Wegen der Vernachlässigung eines Terms bezüglich des analytischen Integrals begeht man bei der Berechnung der Momente der ESR‐Absorptionslinien aus den Ableitungen nach der gewöhnlichen Methode der numerischen Integration der ungeraden Momente einen Fehler. In der vorliegenden Arbeit wird gezeigt, daß dieser Fehler für die zweiten Momente einer abgeschnittenen Lorentzkurve bedeutend ist und abnimmt, je mehr die Linienform sich einer Gausskurve nähert.

Online Resource

0370-1972, 1521-3951

English

Wiley

1969

208851-4

1481096-7

Angewandte Chemie, Wiley, Vol. 134, No. 7 ( 2022-02-07)

Lithium–sulfur (Li–S) batteries are deemed as future energy storage devices due to ultrahigh theoretical energy density. Cathodic polysulfide electrocatalysts have been widely investigated to promote sluggish sulfur redox kinetics. Probing the surface structure of electrocatalysts is vital to understanding the mechanism of polysulfide electrocatalysis. In this work, we for the first time identify surface gelation on disulfide electrocatalysts. Concretely, the Lewis acid sites on disulfides trigger the ring‐opening polymerization of the dioxolane solvent to generate a surface gel layer, covering disulfides and reducing the electrocatalytic activity. Accordingly, a Lewis base triethylamine (TEA) is introduced as a competitive inhibitor. Consequently, Li–S batteries with disulfide electrocatalysts and TEA afford high specific capacity and improved rate responses. This work affords new insights on the actual surface structure of electrocatalysts in Li–S batteries.

Online Resource

0044-8249, 1521-3757

English

Wiley

2022

505868-5

506609-8

514305-6

505872-7

1479266-7

505867-3

506259-7