A new series of five three-dimensional Ln(III) metal-organic frameworks (MOFs) formulated as [Ln(μ-L)(μ-HCOO)(μ-OH)(μ-O)(DMF)(HO)] {Ln = Tb (1), Eu (2), Gd (3), Dy (4), and Er (5)} was successfully obtained via a solvothermal reaction between the corresponding lanthanide(III) nitrates and 2-(6-carboxypyridin-3-yl)terephthalic acid (HL). All of the obtained compounds were fully characterized, and their structures were established by single-crystal X-ray diffraction. All products are isostructural and possess porous 3D networks of the fluorite topological type, which are driven by the cubane-like [Ln(μ-OH)(μ-O)(μ-HCOO)] blocks and μ-L spacers. Luminescent and sensing properties of 1-5 were investigated in detail, revealing a unique capability of Tb-MOF (1) for sensing acetone and metal(III) cations (Fe or Ce) with high efficiency and selectivity. Apart from a facile recyclability after sensing experiments, the obtained Tb-MOF material features a remarkable stability in a diversity of environments such as common solvents, aqueous solutions of metal ions, and solutions with a broad pH range from 4 to 11. In addition, compound 1 represents a very rare example of the versatile Ln-MOF probe capable of sensing Ce or Fe cations or acetone molecules.
Trichalcogenasumanenes were synthesized on a multigram scale through a two-step approach that takes advantage of non-pyrolytic cyclization and solventless ring contraction. Solid-state structure and photophysical investigations demonstrate that these compounds are promising candidates for electronic materials.
Scheme 6. The [3+2] cycloaddition of cyclic nitrone with methyl propiolate.Figure 3. Rationalization of the high selectivity for the formation of 7 b. Angewandte Chemie 8949
A novel and efficient aerobic protocol for the oxidative synthesis of 2-aryl quinazolines via benzyl C-H bond amination by a one-pot reaction of arylmethanamines with 2-aminobenzoketones and 2-aminobenzaldehydes has been carried out using the 4-hydroxy-TEMPO radical as the catalyst, without any metals or additives.
The global pandemic caused by the 2019 coronavirus (COVID-19) has led to a dramatic increase in medical waste worldwide. This tremendous increase in medical waste is an important transmission medium for the virus and thus poses new and serious challenges to urban medical waste management. This study investigates the response of medical waste management to the COVID-19 pandemic and subsequent changes in Wuhan City based on the most detailed data available, including waste generation, storage, transportation, and disposal. The results show that despite a 5-fold increase in the demand for daily medical waste disposal in the peak period, the quick responses in the storage, transportation, and disposal sectors during the pandemic ensured that all medical waste was disposed of within 24 hours of generation. Furthermore, this paper discusses medical waste management during future emergencies in Wuhan. The ability of the medical waste management system in Wuhan to successfully cope with the rapid increase in medical waste caused by major public health emergencies has important implications for other cities suffering from the pandemic and demonstrates the need to establish resilient medical emergency systems in urban areas.
cis-Beta-[Ru(II)(salen(A))(CO)(2)] (salen(A) = N,N'-bis(3-R(1)-5-R(2)-salicylidene)-1,2-cyclohexenediamine dianion; R(1) = R(2) = Bu(t), 1a; R(1) = Pr(i), R(2) = H, 1b; R(1) = Bu(t), R(2) = H, 1c) complexes were prepared by treating Ru(3)(CO)(12) with the respective H(2)salen(A) in 1,2,4-trichlorobenzene and structurally characterized by X-ray crystallography. Complexes 1a-c catalyze intramolecular cyclopropanation of trans-allylic diazoacetates N(2)CHCO(2)CH(2)CH=CHR (3, R = Ph, 4-ClC(6)H(4), 4-BrC(6)H(4), 4-MeC(6)H(4), 4-MeOC(6)H(4), 2-MeC(6)H(4), 2-furanyl) under light irradiation to give cyclopropyl lactones 4 in up to 96% yield and up to 98% ee. DFT calculations on intramolecular cyclopropanation of 3a (R = Ph) with model catalyst cis-beta-[Ru(II)(salen(A0))(CO)(2)] (salen(A0) = N,N'-bis(salicylidene)-1,2-cyclohexenediamine dianion) reveal the intermediacy of both cis-beta- and trans-[Ru(salen(A0))(CHCO(2)CH(2)CH=CHPh)(CO)] bearing salen(A0) in a nonplanar and planar coordination mode, respectively, with the cis-beta-carbene species being a major intermediate in the catalytic carbenoid transfer reaction. The intramolecular cyclopropanation from the cis-beta-carbene species is the most favorable pathway and features an early transition state and an asynchronous concerted [2 + 1] addition mechanism. Enantioselectivities in the reactions involving [Ru(salen(A0))(CHCO(2)CH(2)CH=CHPh)(CO)] were predicted to be 77% ee for the trans-carbene species and 96% ee for the cis-beta-carbene species; the former dramatically increases to 98% ee, whereas the latter slightly increases to 99% ee, upon replacing salen(A0) with salen(A1) (R(1) = R(2) = B(t)). The observed variation in enantioselectivity (90-98% ee) for the conversion of 3a to 4a catalyzed by 1a-c could result from an equilibrium between cis-beta (major) and trans (minor) ruthenium-carbene intermediates.
An efficient sensor for Zn(2+) and Cu(2+) was designed based on different binding modes. The sensor displays ratiometric signals for Zn(2+), due to the Zn(2+)-triggered amide tautomerization; while dual-mode selective behaviors for Cu(2+) result from the deprotonation of the amide tautomer.
The intramolecular addition of hydrazone radicals to carbon-carbon double bonds was achieved by using TEMPO (2,2,6,6-tetramethyl-1-piperidinyloxy) or DIAD (diisopropyl azodicarboxylate) as the hydrazone radical initiator as well as the carbon radical scavenger. Consequently, alkenes were difunctionalized to afford pyrazolines and tetrahydropyridazines via C-N forming 5-exo-trig and 6-exo-trig cyclizations, respectively, and allyls were trifunctionalized to afford pyrazolines via C-N forming tandem 1,5-H-shift/5-exo-trig cyclizations under metal-free neutral conditions.
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