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81.
Dr. Manussada Ratanasak Takumi Murata Taishin Adachi Prof. Jun-ya Hasegawa Prof. Tadashi Ema 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(58):e202202210
BPh3 catalyzes the N-methylation of secondary amines and the C-methylenation (methylene-bridge formation between aromatic rings) of N,N-dimethylanilines or 1-methylindoles in the presence of CO2 and PhSiH3; these reactions proceed at 30–40 °C under solvent-free conditions. In contrast, B(C6F5)3 shows little or no activity. 11B NMR spectra suggested the generation of [HBPh3]−. The detailed mechanism of the BPh3-catalyzed N-methylation of N-methylaniline ( 1 ) with CO2 and PhSiH3 was studied by using DFT calculations. BPh3 promotes the conversion of two substrates (N-methylaniline and CO2) into a zwitterionic carbamate to give three-component species [Ph(Me)(H)N+CO2−⋅⋅⋅BPh3]. The carbamate and BPh3 act as the nucleophile and Lewis acid, respectively, for the activation of PhSiH3 to generate [HBPh3]−, which is used to produce key CO2-derived species, such as silyl formate and bis(silyl)acetal, essential for the N-methylation of 1 . DFT calculations also suggested other mechanisms involving water for the generation of [HBPh3]− species. 相似文献
82.
Marco Masi Maria Chiara Zonno Alessio Cimmino Pierluigi Reveglia Alexander Berestetskiy Angela Boari 《Natural product research》2018,32(13):1537-1547
Ambrosia artemisiifolia L. is responsible for serious allergies induced on humans. Different approaches for its control were proposed during the COST Action FA1203 “Sustainable management of Ambrosia artemisiifolia in Europe” (SMARTER). Fungal secondary metabolites often show potential herbicidal activity. Three phytotoxins were purified from the fungal culture filtrates of Colletotrichum gloeosporioides, isolated from infected leaves of A. artemisiifolia. They were identified by spectroscopic and chemical methods as colletochlorin A, orcinol and tyrosol (1, 2 and 3). The absolute configuration 6’R to colletochlorin A was assigned for the first time applying the advanced Mosher’s method. When assayed by leaf-puncture on A. artemisiifolia only 1 caused the appearance of large necrosis. The same symptoms were also induced by 1 on ambrosia plantlets associated with plant wilting. On Lemna minor, colletochlorin A caused a clear fronds browning, with a total reduction in chlorophyll content. 相似文献
83.
张四保 《数学的实践与认识》2020,(7):273-276
设S(n)是Smarandache函数,其中n是一正整数.讨论Smarandache函数S(n)在数列F((2k),1)=F(n,1)=n2n+1(n=2k)与数列G(2n,1)=(2n)2n+1上的下界估计.基于初等方法证明了:当偶数n≥6时,有S(F((2k),1))=S(F(n,1))≥6×2n+1;当n≥4时,有S(G(2n,1))≥6×2n+1. 相似文献
84.
Long‐Zhang Dong Lei Zhang Jiang Liu Qing Huang Meng Lu Wen‐Xin Ji Ya‐Qian Lan 《Angewandte Chemie (International ed. in English)》2020,59(7):2659-2663
A series of stable heterometallic Fe2M cluster‐based MOFs ( NNU‐31‐M , M=Co, Ni, Zn) photocatalysts are presented. They can achieve the overall conversion of CO2 and H2O into HCOOH and O2 without the assistance of additional sacrificial agent and photosensitizer. The heterometallic cluster units and photosensitive ligands excited by visible light generate separated electrons and holes. Then, low‐valent metal M accepts electrons to reduce CO2, and high‐valent Fe uses holes to oxidize H2O. This is the first MOF photocatalyst system to finish artificial photosynthetic full reaction. It is noted that NNU‐31‐Zn exhibits the highest HCOOH yield of 26.3 μmol g?1 h?1 (selectivity of ca. 100 %). Furthermore, the DFT calculations based on crystal structures demonstrate the photocatalytic reaction mechanism. This work proposes a new strategy for how to design crystalline photocatalyst to realize artificial photosynthetic overall reaction. 相似文献
85.
A series of carbon-coated, nitrogen-doped titanium dioxide photocatalysts was produced and characterized. N-doped TiO2 powder samples were prepared using a sol-gel method and subsequently used for making doped-TiO2 thin films on glass substrates. Carbon layers were coated on the films by a thermal decomposition method using catechol. Diffuse reflectance spectra and Mott-Schottky analyses of the samples proved that nitrogen doping and carbon coating can slightly lower the band gap of TiO2, broaden its absorption to visible light and enhance its n-type character. According to photocatalytic tests against model contaminants, carbon-coated nitrogen-doped TiO2 films have better performance than simple TiO2 on the degradation of Rhodamine B dye molecules, but are poorly effective for degrading 4-chlorophenol molecules. Several possible explanations are proposed for this result, supported by scavenging experiments. This reveals the importance of a broad substrate scope when assessing new photocatalytic materials for water treatment, something which is often overlooked in many literature studies. 相似文献
86.
Although often used in molecular dynamics, in this work the Manning–Rosen potential is parameterized to compute the scattering phase shifts for the nucleon–nucleon and the alpha-nucleon systems by exploiting the standard phase function method. We obtain excellent agreement in phase shifts with the more sophisticated calculations up to partial waves ${\ell }=2.$ 相似文献
87.
《Physics letters. A》2020,384(26):126677
The Ising-like model of spin-crossover solid compounds with quenched random ligand field has been investigated by the mean-field (infinite-range) approximation. An exact solution for the problem is found within the replica formalism. The magnetic diagrams are obtained; the relations between the intermolecular coupling and the temperature as well as the reentrant phenomena of the magnetic ordered phase are discussed. 相似文献
88.
《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
89.
《Arabian Journal of Chemistry》2020,13(11):8424-8457
Nowadays, increasing extortions regarding environmental problems and energy scarcity have stuck the development and endurance of human society. The issue of inorganic and organic pollutants that exist in water from agricultural, domestic, and industrial activities has directed the development of advanced technologies to address the challenges of water scarcity efficiently. To solve this major issue, various scientists and researchers are looking for novel and effective technologies that can efficiently remove pollutants from wastewater. Nanoscale metal oxide materials have been proposed due to their distinctive size, physical and chemical properties along with promising applications. Cupric Oxide (CuO) is one of the most commonly used benchmark photocatalysts in photodegradation owing to the fact that they are cost-effective, non-toxic, and more efficient in absorption across a significant fraction of solar spectrum. In this review, we have summarized synthetic strategies of CuO fabrication, modification methods with applications for water treatment purposes. Moreover, an elaborative discussion on feasible strategies includes; binary and ternary heterojunction formation, Z-scheme based photocatalytic system, incorporation of rare earth/transition metal ions as dopants, and carbonaceous materials serving as a support system. The mechanistic insight inferring photo-induced charge separation and transfer, the functional reactive radical species involved in a photocatalytic reaction, have been successfully featured and examined. Finally, a conclusive remark regarding current studies and unresolved challenges related to CuO are put forth for future perspectives. 相似文献
90.