Latest ArticlesCarbon-mediated persulfate advanced oxidation processes (PS-AOPs) are appealing in contaminant remediation. For the first time, S,B-co-doped carbon-based persulfate activators were synthesized through direct carbonization of sodium lignosulfonate and boric acid. By degrading sulfamethoxazole (SMX), CSB-750 obtained 98.7% removal and 81.4% mineralization within 30 min. In comparison with solo S or B doping, S and B co-doped carbon showed the coupling effect for enhanced catalysis. The rate constant (kobs) of 0.1679 min–1 was 22.38- and 279.83-fold higher than those of CS-750 (0.0075 min–1) and CB-750 (0.0006 min–1), respectively. The degradation was efficient at strong acidic and weak basic conditions (pH 3–9). Substantial inhibition effect was presented at strong basic condition (pH 10.95) and in presence of CO32–. The CO32–-caused inhibition was the combined result of the cooperation of pH and quenching O2·–. Thiophene sulfur, BC3, BC2O, and structural defects were identified as the active sites for PS activation. Radical and nonradical pathways were both involved in the CSB-750/PS/SMX system, where 1O2 dominated the degradation, SO4·–, ·OH and direct electron transfer played the subordinate role, and O2·– served as a precursor for the formation of partial 1O2. The toxicity of degradation system, the effect of real water matrix, and the reusability of carbocatalysts were comprehensively analyzed. Nine possible degradation pathways were proposed. This work focuses on the catalytic performance improvement through the coupling effect of S, B co-doping, and develops an advanced heteroatom doping system to fabricate carbonaceous persulfate activators.
Inhibitor targeting immune checkpoint is a promising new anticancer therapy. Blocking the interaction between PD-1 and PD-L1 can reverse the immunosuppression state and improve the lethality of immune cells to tumor cells. Here, we report PROTAC-based PD-L1 degraders to enhance T cell killing activity against melanoma. Four series of PD-L1 degraders were designed and synthesized to VHL, CRBN, MDM2 or cIAP E3 ligase system, in which CRBN-ligand-based compound BMS-37-C3 was identified as the most active PROTAC molecule. BMS-37-C3 also significantly enhanced the killing ability of T cells in a co-culture model of A375 and T cells. Furthermore, western blot data and flow cytometry demonstrated that BMS-37-C3 could reduce the protein levels of PD-L1 in dose and time dependent manner, which may provide a new therapeutic method for tumor immunotherapy.
A new nanocomposite of hollow covalent organic framework (COF) conjugated with the apatinib (AP) and loading microwave-sensitizer (ionic liquid, IL) was prepared by layer by layer (LBL) method and hyaluronic acid (HA) coating, named as COF-AP-IL@HA. AP loading rate in COF hollow-spheres (~30 nm shell thickness) was ~40.3%, due to the interactions of hydrogen and π-π bonds between AP and COF shell, and acidic environment destroyed COF structure, promoting AP release. Microwave sensitization of loaded IL in COF hollow-spheres could enhance the microwave heat-effect, and combined AP therapeutic ability, leading to their higher inhibitation on tumor, due to targeting ability of HA and the local release of apatinib. 88.9% of inhibition rate of COF-AP-IL@HA under microwave on the in vivo tumor was significantly higher than those without microwave (12.3%) and COF-IL@HA with microwave (37.5%), indicating a synergism of sensitized microwave hyperthermia and AP therapy on the reduced expression of VEGF via the downregulation pathway of hypoxia inducible factor. These results indicated that COF-AP-IL@HA was potential to the application in the combination therapy of tumor of the sensitized microwave hyperthermia and apatinib.
Comprehensive surgical staging or optimal tumor cytoreductive surgery of malignant ovarian cancer directly affects disease prognosis. Therefore, a fluorescent selenium nanoparticle (Se@RGD/S2.2) decorated with cancer-targeting Arg-Gly-Asp (RGD) peptides and GCAGTTGATCCTTTGGATACCCTGG aptamer (S2.2) was developed for use as a diagnostic agent to achieve rapid, noninvasive diagnosis and visualization of microinvasive lesions during surgery for malignant ovarian cancer.
Deuterated ethylene is an important building block for manufacturing various deuterated polyolefins and chemicals. However, low-cost and large-scale production of deuterated ethylene still remain a great challenge. Herein, with D2O as the D source, we first propose an electrocatalytic deuteration strategy for continuous production of deuterated ethylene from acetylene under ambient conditions. Specially, Ag nanoparticles exhibit a very high deuterated ethylene Faradic efficiency of up to 99.3% at –0.6 V vs. reversible hydrogen electrode. Meanwhile, Ag nanoparticles achieve a deuterated ethylene production rate of 3.72 × 103 mmol h–1 gcat–1 and an excellent long-term stability with deuterated ethylene Faradaic efficiencies of ~95% in a two-electrode flow cell, which substantially outperform state-of-the-art values for previously reported deuterated alkenes. In-situ electrochemical Infrared absorption and Raman spectroscopies reveal superior acetylene absorption and formation of deuterated ethylene on Ag nanoparticles. This efficient electrocatalytic deuteration strategy opens a new window for continuous and economic production of deuterated alkenes.
Photocatalytic oxidative desulfurization (PODS) over efficient earth-abundant catalysts to obtain clean fuel oil is of great importance for the environmental protection. In this work, a series of Ce-doped MIL-125-NH2 photocatalysts were successfully prepared via a simple in-situ doping method and exhibited superior PODS performance of dibenzothiophene (DBT) under mild reaction conditions. The 1.0 mol% Ce/MIL-125-NH2 catalyst achieved 100% sulfur removal within 22 min at 30 ℃ under visible light illumination, which is mainly attributed to the high surface area and the formation of Ce-Ti-oxo clusters due to electronic coupling. The valence transformation of Ce4+/Ce3+ and Ti4+/Ti3+ redox mediators could not only expose abundant Lewis acid sites, but also promote the separation and transfer of photogenerated charges. In addition, increasing the reaction temperature has been demonstrated to be effective in promoting the PODS performance. Additionally, a thermo-enhanced PODS mechanism was proposed over Ce/MIL-125-NH2, demonstrating the great potential of thermal energy to promote the desulfurization activity.
Understanding the influence of sulfates over catalysts for selective catalytic reduction of NO with NH3 (NH3-SCR) is crucial due to the universal presence of SO2 in exhaust gas. Depending on the degree of sulfation, there mainly exist surface and bulk sulfates and NH3-SCR activity is generally considered to suffer more from bulk sulfates. Herein, the unique function of bulk sulfates over CeO2 in promoting high-temperature SCR reaction is revealed. Notably, compared with CeO2 dominated with surface sulfates (S-CeO2–4h) and commercial V2O5-WO3/TiO2, CeO2 with bulk sulfates (S-CeO2–72h) exhibits admirable NO conversion at the temperature range of 400–550 ℃. Bulk sulfates provide more Brønsted acid sites with stronger strength for NH3 adsorption. Moreover, the oxidation ability of CeO2 is significantly inhibited due to electron-withdrawing effect from bulk sulfates, which alleviates NH3 oxidation at high temperatures. More NH3 adsorption with high stability and limited NH3 oxidation capacity ensure the excellent catalytic performance for S-CeO2–72h in high-temperature denitration. This work provides new insight of bulk sulfates in promoting SCR activity and open a new avenue to design deNOx catalysts employed at high temperatures.
Metal-free carbon catalysts with excellent conduction performance have drawn much research attention in reduction reactions. Herein, a N, B co-doped carbon catalyst with high pyrrolic N proportion (35.75%) and excellent surface area (1409 m2/g) was successfully prepared via carbonizing covalent organic framework materials (COFs) containing N and B atoms assisted by ZnCl2 molten salt. The presence of ZnCl2 maintains the micropore structure of COFs to provide high specific surface areas and abundant lattice defects for carbon materials. In addition, electron-withdrawing B heteroatom further facilitates the formation of pyrrolic N at defect sites by modifying the electronic structure of carbon network. The tuning of surface areas and active N species in carbon catalysts successfully improve the selective hydrogenation of nitrobenzene to aniline. The optimized carbon material exhibits excellent nitrobenzene conversion (99.9%) and aniline selectivity (> 99%) within 15 min, as well as excellent substrate suitability. This work provides a certain guiding for the design and application of metal-free catalysis.
Carbon dioxide (CO2) is an attractive C1 building block in chemical synthesis due to its abundance, availability and sustainability. However, the low reactivity and high stability generally limits its transformations under mild conditions to value added chemicals. Recent advances in flow chemistry provide effective means for the chemical transformation of CO2, and many new methods and techniques that fully utilized the advantages of continuous flow platforms for the chemical fixation of CO2 have been realized. In view of the rapid development and the urgent need for continuous transformation of CO2, herein we wish to present an update of the recent advances in this research area.
Mechanical force between cells relates to many biological processes of cell development. The cellular collective migration comes from cell-cell cooperation, and studying the intercellular mechanical properties helps elucidate collective cell migration. Herein, we studied cell-cell junctions, intercellular tensile force and the related cellular energetic costs in confined microchannels. Using the intercellular force sensor, we found that cells adapt to different confinement environments by regulating intercellular force, and thereby the relationship between collective cell migration and cell-cell junction were verified. Through the observation of cell orientation, actomyosin contractility, energetic costs, and glucose uptake, we can make a reasonable explanation of cell-force driven migration in different confined environments. Under highly confined conditions, the intercellular force and energetic costs are greater, and the cell orientation is more orderly. The collective migration behavior in confined spaces is closely related to the intercellular force and energetic costs, which is helpful to understand the collective migration behaviors in various confined spaces.
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