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91.
Rei Tomifuji Prof. Takuya Kurahashi Prof. Seijiro Matsubara 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(38):8987-8991
The development and use of a multiple-activation catalyst with ion-paired Lewis acid and Brønsted acid in an asymmetric aza-Diels–Alder reaction of simple dienes (non-Danishefsky-type electron-rich dienes) was achieved by utilizing the [FeBr2]+[FeBr4]− combination prepared in situ from FeBr3 and chiral phosphoric acid. Synergistic effects of the highly active ion-paired Lewis acid [FeBr2]+[FeBr4]− and a chiral Brønsted acid are important for promoting the reaction with high turnover frequency and high enantioselectivity. The multiple-activation catalyst system was confirmed using synchrotron-based X-ray absorption fine structure measurements, and theoretical studies. This study reveals that the developed catalyst promoted the reaction not only by the interaction offered by the ion-paired Lewis acid and the Brønsted acid but also noncovalent interactions. 相似文献
92.
93.
Dr. Johanna Scheck Lisa M. Fuhrer Dr. Baohu Wu Dr. Markus Drechsler Prof. Dr. Denis Gebauer 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(56):13002-13007
Hematite (α-Fe2O3) is thermodynamically stable under ambient conditions, of vast geological importance, and widely used in applications, for example, as corrosion protection and as a pigment. It forms at elevated temperatures, whereas room-temperature reactions typically yield metastable akaganéite or ferrihydrite. The mechanistic key changes underlying this observation were explored in the present study. The entropic contribution to the prenucleation hydrolysis reaction categorically implies the presence of prenucleation clusters (PNCs) as fundamental precursors. The formation of hematite is then due to a change in the reaction mechanism above approximately 50 °C, whereby the reaction limitation towards oxolation in phase-separated clusters is overcome. A model that rationalizes the occurrence of hematite, akaganéite, and ferrihydrite based on the chemistry of olation PNCs is proposed. Supersaturation and the temperature dependence of olation and oxolation rates from monomeric precursors are irrelevant in this nonclassical mechanism. 相似文献
94.
95.
Kexuan Zhang 《中国物理 B》2021,30(12):126802-126802
The interfacial enhanced ferromagnetism in maganite/ruthenate system is regarded as a promising path to broaden the potential of oxide-based electronic device applications. Here, we systematically studied the physical properties of LaLa1-xCaxMnO3/SrRuO3 superlattices and compared them with the LaLa1-xCaxMnO3 thin films and bulk compounds. The LaLa1-xCaxMnO3/SrRuO3 superlattices exhibit significant enhancement of Curie temperature (TC) beyond the corresponding thin films and bulks. Based on these results, we constructed an extended phase diagram of LaLa1-xCaxMnO3 under interfacial engineering. We considered the interfacial charge transfer and structural proximity effects as the origin of the interface-induced high TC. The structural characterizations revealed a pronounced increase of B-O-B bond angle, which could be the main driving force for the high TC in the superlattices. Our work inspires a deeper understanding of the collective effects of interfacial charge transfer and structural proximity on the physical properties of oxide heterostructures. 相似文献
96.
《Current Applied Physics》2020,20(2):337-343
Radiotherapy for cancer patients requires accurate measurement of the absorbed dose of radiation in a treatment planning step. Various types of radiation detectors are currently utilized for dose measurement. Among them, calorimeters are known to be the most precise detector for measuring absorbed dose, but their on-site application is limited by the large size of the equipment. We developed a miniaturized chip calorimeter for application as a radiation detector. The calorimetric radiation detector was built using micro/nano fabrication techniques, and consists of an SU-8 photoresist absorber and high-sensitivity vanadium oxide (VOx) thermistors. The thermistors had a temperature resolution of 135 μK, and the calorimeter showed a thermal conductance of 11 μW/K. The detector was irradiated with various X-ray dose rates from a linear accelerator, and the absorbed dose to SU-8 was measured. The detector responses showed high linearity with dose rates, demonstrating the feasibility of the radiation detector for practical uses. 相似文献
97.
《Current Applied Physics》2020,20(1):102-105
We demonstrate a practical way to identify the presence of a perovskite phase in rare-earth nickelates (RNiO3) using X-ray photoelectron spectroscopy (XPS). By varying the calcination temperature, we prepared RNiO3 powders with different degrees of chemical reaction. We found that perovskite RNiO3 becomes predominant after high-temperature calcination (≥1,000 °C) in X-ray diffraction and XPS (at Ni 3p and O 1s edges) measurements. While the observed spectra at the Ni 3p edge are similar for all powders, a sizable difference was observed in the O 1s-edge spectra depending on the calcination temperature. With the formation of a perovskite phase with a trivalent Ni3+ state, an XPS peak corresponding to oxygen ions in the perovskite lattice distinctly emerges. Our work shows that the Ni3+ state cannot be determined by analyzing the Ni 3p edge solely and rather, the O 1s edge should be simultaneously monitored for explicit identification. 相似文献
98.
Chao He Mingyuan Li Jue Zhang Bingqing Yan Weifeng Zhao Shudong Sun Changsheng Zhao 《Macromolecular bioscience》2020,20(8)
Excessive bilirubin in the body of patient with liver dysfunction or metabolic obstruction may cause jaundice with irreversible brain damage, and new type of adsorbent for bilirubin is under frequent investigation. Herein, graphene oxide based core @ polyethersulfone‐based shell beads are fabricated by phase inversion method, amides and heparin‐like polymer are introduced to functionalize the core‐shell beads. The beads are successfully prepared with obvious core‐shell structure, adequate thermostability and porous shell. Clotting times and protein adsorption are investigated to inspect the hemocompatibility property of the beads. The adsorption of bilirubin is systematically investigated by evaluating the effects of contacting time, initial concentration and temperature on the adsorption, which exhibits improved bilirubin adsorption amount for the beads with amides contained cores or/and shells. It is worth believing that the amides and heparin‐like polymer co‐functionalized core‐shell beads may be utilized in the field of hemoperfusion for bilirubin adsorption. 相似文献
99.
《Arabian Journal of Chemistry》2020,13(2):3934-3945
A hierarchical nanostructure consisting of uniform copper oxide nanowires vertically grown on three-dimensional copper framework (CuO NWs/3D-Cu foam) was prepared by a two-step synthetic process. The uniform CuO NWs anchored onto the 3D foam exhibited outstanding electrocatalytic activity towards hydrogen peroxide reduction due to the unique one‐dimensional direction with its excellent catalytic activity and large surface area of 3D substrate, which enhanced electroactive sites and charge conductivity. As a result, a wide linear detection range of 1 µM–1 mM, good sensitivity of 8.87 µA/(mM ⋅ cm2), low detection limit of 0.98 µM, and rapid response time of 5 s to hydrogen peroxide were achieved under a working potential of −0.4 V in phosphate buffer solution (pH of 7.4). In addition, the CuO NWs/3D-Cu foam material showed excellent selectivity to hydrogen peroxide and good resistance against poisonous interferents, including ascorbic acid, dopamine, urea, uric acid, and potassium chloride. Furthermore, the CuO NWs/3D-Cu foam presented good reproducibility, stability, and accurate detection for hydrogen peroxide in real sample; therefore, it may be considered to be a potential free-standing hydrogen peroxide sensor in practical analysis applications. 相似文献
100.
《Arabian Journal of Chemistry》2020,13(4):4869-4881
Herein, we report for the first time, an eco-compatible hydrothermal route for the synthesis of carbon enriched mesoporous material (CuO NFs@MP) using fruit waste (Pulp) obtained from Citrus limetta’s (Mausambi) decorated irregular shaped CuO nanoflakes (NFs). The CuO NFs@MP nanocomposite was fully characterized through several spectroscopic-cum-analytical techniques such as TEM and XPS, which further confirmed the presence of CuO NFs. CuO NFs@MP could serve as an excellent catalyst for N-Arylation reaction and also paves promising peroxidase mimic activity. The preliminary results indicated that CuO NFs@MP shows the catalytic advantage of higher yields, shorter reaction time and greener conditions. Simultaneously, the oxidation of colorless TMB with H2O2 into blue-green colored ox-TMB was also observed in 60 s with CuO NFs@MP. The present nanocomposite is easy to synthesize, economical, retrievable and a reusable catalyst for synthesizing a varied range of N-Arylated products and could also mimic peroxidase without significant loss of activity. 相似文献