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Diastereo- and Enantioselective Copper-Catalyzed Decarboxylative Ring-Opening [3+2] Annulation of Tertiary Propargylic Carbamates through Regioselective alpha-Attack of gamma-Butenolides
No full textA copper-catalyzed regio-, diastereo-, and enantioselective decarboxylative ring-opening [3 + 2] annulation of tertiary propargylic carbamates with gamma-butenolides for the synthesis of optically active pyrrolidinones has been realized. The reaction proceeded through regioselective alpha-attack of gamma-butenolide and generated highly congested vicinal tertiary and all-carbon quaternary stereocenters in pyrrolidinone scaffolds, featuring high stereoselective induction and broad functional group tolerance. Critical to the successful development of this method was the employment of copper catalysis in concert with a diPh-Pybox ligand
Carbon molecular sieving membranes for butane isomer separation
No full textMembrane-based separations of hydrocarbon isomers are major challenges for the petrochemical industry. Herein, high quality carbon molecular sieving membranes (CMSMs) were prepared on gamma-alumina substrates from pyrolysis of P84 polymer membranes. Targeting at butane isomer separations, we tailored the slit-like ultramicropores of CMSMs at angstrom level by rational manipulations of the pyrolysis temperature. The crack-free CMSMs were obtained at 600 degrees C with the narrow and uniform ultramicropores centered at 6.0 a. A clear molecular size/shape discrimination was achieved successfully and remarkable n-butane permeance (384 GPU) and n-butane/iso-butane separation factor (74) was observed, which transcends the upper limit of well-intergrown crystalline zeolite membranes. Fine-tuning of the membrane thickness at sub-micron level, the n-butane permeance and n-butane/iso-butane separation factor were further optimized, which shows a great potential for petrochemical separation
pH-Responsive Polymer-Stabilized ZIF-8 Nanocomposites for Fluorescence and Magnetic Resonance Dual-Modal Imaging-Guided Chemo-/Photodynamic Combinational Cancer Therapy
No full textA multifunctional diagnosis and treatment integration platform is crucial in cancer treatments. Here, we show that by integrating Gd-doped silicon nanoparticles (Si-Gd NPs), chlorine e6 (Ce6), doxorubicin (DOX), zeolitic imidazolate framework-8 (ZIF-8), poly(2-(diethylamino)ethyl methacrylate) polymers (HOOC-PDMAEMA-SH), and folic acid-polyethylene glycol)-maleimide (MaL-PEG-FA) into one single nanoplatform by a self-assembly method, novel multifunctional MOFs (named FZIF-8/DOX-PD-FA) are synthesized with great biocompatibility and tumor targeting as well as pH responsiveness and no drug leakage for drug delivery. In the design, Si-Gd NPs and Ce6 embedded in the nanocomposites are used for magnetic resonance and fluorescence dual-modal imaging, respectively. DOX loaded by the FZIF-8/DOX-PD-FA porous structure is used for chemotherapy, while Ce6 is excited by near-infrared radiation (NIR) for photodynamic therapy. In addition, the pH-responsive ability of HOOC-PDMAEMA-SH to effectively prevent drug leakage is demonstrated by drug release studies in vitro. From the results of confocal microscopy imaging in vitro and fluorescence/magnetic resonance imaging in vivo, FZIF-8/DOX-PD-FA showed a targeting effect on MCF-7 cancer cells. More importantly, the results of treatment experiments on tumor-bearing mice showed that the tumor volume of the FZIF-8/DOX-PD-FA + NIR group is decreased the most compared to the original volume. Owing to the unique dual-modal imaging capability and excellent chemo-/photodynamic combinational cancer therapy effect, the present hybrid nanocarrier provides a new research platform for a new generation of theranostic nanoparticles
A Novel Anion Doping for Stable CsPbI2Br Perovskite Solar Cells with an Efficiency of 15.56% and an Open Circuit Voltage of 1.30 V
No full textThe Cs-based inorganic perovskite solar cells (PSCs), such as CsPbI2Br, have made a striking breakthrough with power conversion efficiency (PCE) over 16% and potential to be used as top cells for tandem devices. Herein, I- is partially replaced with the acetate anion (Ac-) in the CsPbI2Br framework, producing multiple benefits. The Ac- doping can change the morphology, electronic properties, and band structure of the host CsPbI2Br film. The obtained CsPbI2-xBr(Ac)(x) perovskite films present lower trap densities, longer carrier lifetimes, and fast charge transportation compared to the host CsPbI2Br films. Interestingly, the CsPbI2-xBr(Ac)(x) PSCs exhibit a maximum PCE of 15.56% and an ultrahigh open circuit voltage (V-oc) of 1.30 V without sacrificing photocurrent. Notably, such a remarkable V-oc is among the highest values of the previously reported CsPbI2Br PSCs, while the PCE far exceeds all of them. In addition, the obtained CsPbI2-xBr(Ac)(x) PSCs exhibit high reproducibility and good stability. The stable CsPbI2-xBr(Ac)(x) PSCs with high V-oc and PCE are desirable for tandem solar cell applications
