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61.
Wenxiang Liu Lele Lu Qiang Li Boyuan Wu Ruizhe Zhang Wei Shi Peng Cheng 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(53):12206-12211
Photocatalytic hydrogen evolution by water splitting is highly important for the application of hydrogen energy and the replacement of fossil fuel by solar energy, which needs the development of efficient catalysts with long-term catalytic stability under light irradiation in aqueous solution. Herein, Zn0.5Cd0.5S solid solution was synthesized by a metal–organic framework-templated strategy and then loaded with MoS2 by a hydrothermal method to fabricate a MoS2/Zn0.5Cd0.5S heterojunction for photocatalytic hydrogen evolution. The composition of MoS2/Zn0.5Cd0.5S was fine-tuned to obtain the optimized 5 wt % MoS2/Zn0.5Cd0.5S heterojunction, which showed a superior hydrogen evolution rate of 23.80 mmol h−1 g−1 and steady photocatalytic stability over 25 h. The photocatalytic performance is due to the appropriate composition and the formation of an intimate interface between MoS2 and Zn0.5Cd0.5S, which endows the photocatalyst with high light-harvesting ability and effective separation of photogenerated carriers. 相似文献
62.
Yichen Zhou Mingmin Jia Dr. Xiongfei Zhang Prof. Dr. Jianfeng Yao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(35):7918-7922
Zeolite ZIF-8 has been etched with acid to form microporous ZIF-8-E crystals. These were then introduced into a polyethersulfone (PES) membrane matrix to enhance its CO2/N2 separation performance. Open through pores of size about 100 nm formed in the ZIF-8 crystals allow the ingrowth of polyethersulfone chains, ensuring a reduction in the number of nonselective voids, thereby achieving better interaction between ZIF-8-E and PES. As a result, the CO2/N2 separation performance of the ZIF-8-E/PES membrane increased significantly, showing a CO2 permeability of 15.7 Barrer and a CO2/N2 ideal selectivity of 6.5. 相似文献
63.
Maëva-Charlotte Kervarec Prof. Dr. Erhard Kemnitz Priv.-Doz. Dr. Gudrun Scholz Dr. Svemir Rudić Prof. Dr. Thomas Braun Prof. Dr. Christian Jäger Dr. Adam A. L. Michalchuk Priv.-Doz. Dr. Franziska Emmerling 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(32):7314-7322
The very strong Lewis acid aluminium chlorofluoride (ACF) was loaded with anhydrous HF. The interaction between the surface of the catalyst and HF was investigated using a variety of characterization methods, which revealed the formation of polyfluorides. Moreover, the reactivity of the HF-loaded ACF towards the hydrofluorination of alkynes was studied. 相似文献
64.
Adam I. Green Dr. Fruzsina Hobor Dr. Christopher P. Tinworth Dr. Stuart Warriner Prof. Andrew J. Wilson Prof. Adam Nelson 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(47):10682-10689
Protein–protein interactions (PPIs) provide a rich source of potential targets for drug discovery and biomedical science research. However, the identification of structural-diverse starting points for discovery of PPI inhibitors remains a significant challenge. Activity-directed synthesis (ADS), a function-driven discovery approach, was harnessed in the discovery of the p53/hDM2 PPI. Over two rounds of ADS, 346 microscale reactions were performed, with prioritisation on the basis of the activity of the resulting product mixtures. Four distinct and novel series of PPI inhibitors were discovered that, through biophysical characterisation, were shown to have promising ligand efficiencies. It was thus shown that ADS can facilitate ligand discovery for a target that does not have a defined small-molecule binding site, and can provide distinctive starting points for the discovery of PPI inhibitors. 相似文献
65.
Huiye Zhong Wei-Shang Lo Tiantian Man Benjamin P. Williams Dan Li Dr. Sheng-Yu Chen Prof. Dr. Hao Pei Prof. Dr. Li Li Prof. Dr. Chia-Kuang Tsung 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(57):12931-12935
DNAzymes are a promising class of bioinspired catalyst; however, their structural instability limits their potential. Herein, a method to stabilize DNAzymes by encapsulating them in a metal–organic framework (MOF) host is reported. This biomimetic mineralization process makes DNAzymes active under a wider range of conditions. The concept is demonstrated by encapsulating hemin-G-quadruplex (Hemin-G4) into zeolitic imidazolate framework-90 (ZIF-90), which indeed increases the DNAzyme's structural stability. The stabilized DNAzymes show activities in the presence of Exonuclease I, organic solvents, or high temperature. Owing to its elevated stability and heterogeneous nature, it is possible to perform catalysis under continuous-flow conditions, and the DNAzyme can be reactivated in situ by introducing K+. Moreover, it is found that the encapsulated DNAzyme maintains its high enantiomer selectivity, demonstrated by the sulfoxidation of thioanisole to (S)-methyl phenyl sulfoxide. This concept of stabilizing DNAzymes expands their potential application in chemical industry. 相似文献
66.
Juan A. Allegretto Agustín Iborra Dr. Juan M. Giussi Dr. Catalina von Bilderling Dr. Marcelo Ceolín Dr. Sergio Moya Dr. Omar Azzaroni Dr. Matias Rafti 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(54):12388-12396
This work reports on a novel and versatile approach to control the structure of metal–organic framework (MOFs) films by using polymeric brushes as 3D primers, suitable for triggering heterogeneous MOF nucleation. As a proof-of-concept, this work explores the use of poly(1-vinylimidazole) brushes primer obtained via surface-initiated atom transfer radical polymerization (SI-ATRP) for the synthesis of Zn-based ZIF-8 MOF films. By modifying the grafting density of the brushes, smooth porous films were obtained featuring inherently hydrophobic microporosity arising from ZIF-8 structure, and an additional constructional interparticle mesoporosity, which can be employed for differential adsorption of targeted adsorbates. It was found that the grafting density modulates the constructional porosity of the films obtained; higher grafting densities result in more compact structures, while lower grafting density generates increasingly inhomogeneous films with a higher proportion of interparticle constructional porosity. 相似文献
67.
Dr. Yong-Zhi Li Gang-Ding Wang Hong-Yun Yang Prof. Lei Hou Prof. Yao-Yu Wang Prof. Zhonghua Zhu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(69):16402-16407
To develop efficient adsorbent materials for storage and separation of C2H2, an unprecedented supercage MOF, [Me2NH2]⋅[Zn3(ALP)(TDC)2.5]⋅3.5DMF⋅2 H2O ( 1 ) was constructed through medicinal molecule allopurinol (ALP) and S-containing 2,5-thiophenedicarboxylic acid (H2TDC). 1 contains a novel linear trinuclear cluster that is composed by ALP and carboxylates and forms a final uncommon 5-connected yfy topological framework. The framework possesses three types of interlinked cages decorated by rich functional sites, and reveals not only high adsorption capacity for C2H2 but also excellent selective separation for C2H2/CO2 and C2H2/CH4 at 298 K. Dynamic breakthrough experiments on C2H2/CO2 (1:1) mixture and C2H2/CH4 (1:1) mixture also demonstrated the potential of the material to separate C2H2 from CO2 or CH4 mixtures. Molecular simulations were also studied to identify the different CO2- and C2H2- binding sites in 1 , such as carboxylate groups, S atoms and carbonyl groups. 相似文献
68.
Prof. Dr. Fa-Guang Zhang Xue-Qi Wang Yin Zhou Hong-Song Shi Zhe Feng Prof. Dr. Jun-An Ma Prof. Dr. Ilan Marek 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(67):15378-15396
Remote functionalization reactions have the power to transform a C−H (or C−C) bond at a distant position from a functional group. This Review summarizes recent advances and key breakthroughs in remote fluorination, trifluoromethylation, difluoromethylation, trifluoromethylthiolation, and fluoroalkenylation reactions. Several powerful strategies have emerged to control the reactivity and distal selectivity such as the undirected radical approach, the 1,5-hydrogen atom transfer, the metal migration, the use of distant directing groups, and the ring-opening reactions. These unconventional and predictable C−H (and C−C) functionalization transformations should allow for the preparation of a wide range of otherwise-difficult-to-access alkyl, aromatic, heteroaromatic, and structurally complex fluorides. 相似文献
69.
Prof. Dr. Bernhard Kräutler 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(67):15438-15445
The recently delineated structure- and reactivity-based concept of antivitamins B12 has begun to bear fruit by the generation, and study, of a range of such B12-dummies, either vitamin B12-derived, or transition metal analogues that also represent potential antivitamins B12 or specific B12-antimetabolites. As reviewed here, this has opened up new research avenues in organometallic B12-chemistry and bioinorganic coordination chemistry. Exploratory studies with antivitamins B12 have, furthermore, revealed some of their potential, as pharmacologically interesting compounds, for inducing B12-deficiency in a range of organisms, from hospital resistant bacteria to laboratory mice. The derived capacity of antivitamins B12 to induce functional B12-deficiency in mammalian cells and organs also suggest their valuable potential as growth inhibitors of cancerous human and animal cells. 相似文献
70.
Nobutaka Yoshimura Dr. Atsushi Kobayashi Dr. Masaki Yoshida Prof. Masako Kato 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(70):16939-16946
To investigate the effect of the surface structure of dye-sensitized photocatalyst nanoparticles, we prepared three types of RuII-photosensitizer (PS)-double-layered Pt-cocatalyst-loaded TiO2 nanoparticles with different surface structures, Zr- RuCP6 -Zr- RuP6 @N wt %Pt-TiO2, RuCP6 -Zr- RuP6 @N wt %Pt-TiO2, and RuCP2 -Zr- RuP6 @N wt %Pt-TiO2 (N=0.2, 1, and 5), and evaluated their photocatalytic H2 evolution activity in the presence of redox-reversible iodide as the electron donor. Although the driving force of the electron injection from I− to the photo-oxidized RuIII PS is comparable, the activity increased in the following order: RuCP2 -Zr- RuP6 @1 wt %Pt-TiO2 < RuCP6 -Zr- RuP6 @1 wt %Pt-TiO2 < Zr- RuCP6 -Zr- RuP6 @1 wt %Pt-TiO2. The apparent quantum yield of Zr- RuCP6 -Zr- RuP6 @1 wt %Pt-TiO2 in the first hour reached 1 %. Zeta-potential measurements suggest that the surface Zr4+-phosphate groups attracted I− anions to the nanoparticle–solution interface. Our results indicate that the surface modification of dye-sensitized photocatalysts is a promising approach to enhance photocatalytic activity with various redox mediators. 相似文献