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Iridium-catalyzed asymmetric hydrogenation of quinazolinones
No full textEnantioselective hydrogenation of quinazolinones has been successfully realized by employing a chiral iridium/diphosphine complex as catalyst, furnishing the chiral dihydroquinazolinones with excellent yield and up to 98% enantioselectivity. Asymmetric hydrogenation at the gram scale was also conducted smoothly without loss of reactivity and enantioselectivity. Using the above methodology as the key step, the enantiopure bioactive Eg5 inhibitor and (-)-SDZ 267-489 could also be conveniently synthesized
Structures and Infrared Spectra of [M(CO2)(7)](+) (M = V, Cr, and Mn) Complexes
No full textGas-phase infrared photodissociation spectra of [V(CO2)(n)](+) complexes revealed three new vibrational bands at 1140, 1800, and 3008 cm(-1) at n = 7, the features of which are retained in the larger clusters (Ricks, A. M.; Brathwaite, A. D.; Duncan, M. A. J. Phys. Chem. A 2013, 117, 11490-11498). However, structural assignment of this intriguing feature remains open. Herein, quantum chemical calculations on [V(CO2)(7)](+) were carried out to identify the structure of the low-lying isomers and to assign the observed spectral features. The comparison of calculated infrared spectra of [V(CO2)(7)](+) with experimental infrared spectra identified the formation of a bent CO2 species, suggesting the ligand-induced activation of CO, by the vanadium cation. The structures and infrared spectra of [Cr(CO2)(7)](+) and [Mn(CO2)(7)](+) were also predicted and discussed
Global Quantification of Intact Proteins via Chemical Isotope Labeling and Mass Spectrometry
No full textAlthough thousands of intact proteins have been feasibly identified in recent years, global quantification of intact proteins is still challenging. Herein, we develop a high-throughput strategy for global intact protein quantification based on chemical isotope labeling. The isotope incorporation efficiency is as high as 99.2% for complex intact protein samples extracted from HeLa cells. Further, the pTop 2.0 software is developed for automated quantification of intact proteoforms in a high-throughput manner. The high quantification accuracy and reproducibility of this strategy have been demonstrated for both standard and complex cellular protein samples. A total of 2283 intact proteoforms originated from 660 protein accessions are successfully quantified under anaerobic and aerobic conditions and the differentially expressed proteins are observed to be involved in the important biological processes such as stress response
Toward High Power-High Energy Sodium Cathodes: A Case Study of Bicontinuous Ordered Network of 3D Porous Na-3(VO)(2)(PO4)(2)F/rGO with Pseudocapacitance Effect
No full textDeveloping high power-high energy electrochemical energy storage systems is an ultimate goal in the energy storage field, which is even more difficult but significant for low-cost sodium ion batteries. Here, fluoride is successfully prepared by the electrostatic spray deposition (ESD) technique, which greatly expands the application scope of ESD. A two-step strategy (solvothermal plus ESD method) is proposed to construct a bicontinuous ordered network of 3D porous Na-3(VO)(2)(PO4)(2)F/reduced graphene oxide (NVOPF/rGO). This two-step strategy makes sure that NVOPF can be prepared by ESD, since it avoids the loss of F element during synthesis. The obtained NVOPF particles are as small as 15 nm, and the carbon content is only 3.5% in the final nanocomposite. Such a bicontinuous ordered network and small size of electroactive particles lead to the significant contribution of the pseudocapacitance effect to sodium storage, resulting in real high power-high energy sodium cathodes. The cathode exhibits excellent rate capability and cycling stability, whose rate performance is one of the best ever reported in both half cells and full cells. Moreover, this work provides a general and promising strategy for developing high power-high energy electrode materials for various electrochemical energy storage systems
