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Sn-Ag Synergistic Effect Enhances High-Rate Electrocatalytic CO2-to-Formate Conversion on Porous Poly(Ionic Liquid) Support
No full textThe electrocatalytic transformation of carbon dioxide (CO2) to formate is a promising route for highly efficient conversion and utilization of CO2 gas, due to the low production cost and the ease of storage of formate. In this work, porous poly(ionic liquid) (PPIL)-based tin-silver (Sn-Ag) bimetallic hybrids (PPILm-SnxAg10-x) are prepared for high-performance formate electrolytic generation. Under optimal conditions, an excellent formate Faradaic efficiency of 95.5% with a high partial current density of 214.9 mA cm(-2) is obtained at -1.03 V (vs reversible hydrogen electrode). Meanwhile, the high selectivity of formate (>approximate to 83%) is maintained in a wide potential range (>630 mV). Mechanistic studies demonstrate that the presence of Ag-species is vital for the formation, maintenance, and high dispersion of tetravalent Sn(IV)-species, which accounts for the active sites for CO2-to-formate conversion. Further, the introduction of Ag-species significantly enhances the activity by increasing the electron density near the Fermi energy level
Engineered NanoAlum from aluminum turns cold tumor hot for potentiating cancer metalloimmunotherapy
No full textThe poor cancer immunotherapy outcome has been closely related to immunosuppressive tumor microenvironment (TME), which usually inactivates the antitumor immune cells and leads to immune tolerance. Metalloimmunotherapy by supplementing nutritional metal ions into TME has emerged as a potential strategy to activate the tumor-resident immune cells. Herein, we engineered a magnesium-contained nano-aluminum adjuvant (NanoAlum) through hydrolyzing a mixture of Mg(OH)2 and Al(OH)3, which has highly similar components to commercial Imject Alum. Peritumoral injection of NanoAlum effectively neutralized the acidic TME while releasing Mg2+ to activate the tumor-resident T cells. Meanwhile, NanoAlum also blocked the autophagy pathway in tumor cells and subsequently induced cell apoptosis. The in vivo studies showed that merely peritumoral injection of NanoAlum successfully inhibited the growth of solid tumors in mice. On this basis, NanoAlum combined with chemical drug methotrexate or immunomodulatory adjuvant CpG further induced potent antigen-specific antitumor immunity. Overall, our study first provides a rational design for engineering tumortargeted nanomodulator from clinical adjuvants to achieve effective cancer metalloimmunotherapy against solid tumors
Understanding the hydroxyl adsorption behavior at Pt electrode surface in high-temperature alkaline solutions
No full textSince the application in fuel cell, the electrochemical adsorption of hydroxyl has received considerable attention in recent years. While most research mainly focus on the room temperature, in this paper, the electrochemical adsorption of hydroxyl in alkaline solution at high temperature was investigated. An unusual oxidation peak was observed at -0.27 V, suggesting new behavior of hydroxyl adsorption occurred. As is known two kinds of cation hydrated clusters exist in alkaline solution, (H2O)X-1M'-H2O-OadH and (H2O)XM'-OadH. For K' and Cs', the cluster shows unstable structure due to the weak interaction between hydrated cation and OH- especially at high temperature. However, For Li', Na' the cluster structure would be stable, as the interaction force between the hydrated cation and OH- is so strong. It was revealed that the unusual oxidation peak has some relationship with the (H2O)X-1M'-H2O-OadH cluster (K' and Cs') absorbed at Pt electrode surface. When the temperature was raised, (H2O)X-1M'-H2O- and -OadH was disconnected, then the OadH absorbed at Pt surface got oxidated. Based on the SEM observation, it was showed the unusual electrochemical oxidation reaction would generate platinum oxides, blocking the reactive sites at Pt electrode surface, thus reducing the electrochemical reactivity of Pt electrode. Accordingly, parameters of alkaline concentration and temperature were systematically studied, it was found that increase temperature or alkaline concentration was in favor of the unusual oxidation reaction. This study provides more understanding of hydroxyl adsorption behavior at Pt electrode surface for the high temperature water solution environment. (c) 2022 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved
A new process to produce battery grade lithium carbonate from salt lake brines by purification, synergistic solvent extraction and carbon dioxide stripping
No full textThere are abundant lithium resources in China, and the demand for lithium salts is high. However, lithium re-sources of the sulfate salt lakes in Tibet, such as Baqiancuo Salt Lake, have not been effectively utilised. This study proposes a synergistic extraction system composed of LIX 54, TRPO, and surfactant ADD-1 for efficient lithium extraction from the brine and separation of impurities. The CO2 gas stripped lithium and produced high -purity lithium bicarbonate solution. Thermal decomposition produced lithium carbonate solid from the loaded strip solution. The comprehensive yield of lithium was higher than 95%, and the quality of the lithium carbonate product reached the battery chemical grade standard. This new process offers a new way for the utilisation of lithium resources in salt lakes
Impacts of solid physical properties on the performances of a slurry external airlift loop reactor integrating mixing and separation
No full textSolid physical properties are vital for the design, optimization, and scale-up of gas-liquid-solid multiphase reactors. The complex and interactional effects of the solid physical properties, including particle diameter, density, wettability, and sphericity, on the hydrodynamic behaviors in a new external airlift loop reactor (EALR) integrating mixing and separation are decoupled in this work. Two semi-empirical equations are proposed and validated to predict the overall gas holdup and liquid circulating velocity satisfactorily, and then the individual influence of such solid physical properties is further investigated. The results demonstrate that both the overall gas holdup in the riser and the liquid circulating velocity in the downcomer increase with the contact angle, but decrease with particle size, density, and sphericity. Additionally, the impact of the particle size on the liquid circulating velocity is also profoundly revealed on a micro-level considering the particle size distribution. Moreover, the axial solid concentration distribution is discussed, and the uniformity of the slurry is described by the mixing index of the solid particles. The results show that a more homogeneous mixture can be achieved by adding finer particles other than attaining violent turbulence. Therefore, this work lays a foundation for the design, scale-up, and industrialization of the EALRs.(c) 2022 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved
How do antimicrobial peptides disrupt the lipopolysaccharide membrane leaflet of Gram-negative bacteria?
No full textHypothesis: It is widely regarded that antimicrobial peptides (AMPs) kill bacteria by physically disrupting microbial membranes and causing cytoplasmic leakage, but it remains unclear how AMPs disrupt the outer membrane (OM) of Gram-negative bacteria (GNB) and then compromise the inner membrane. We hypothesise that different AMPs impose different structural disruptions, with direct implications to their antimicrobial efficacies. Experiments: The antimicrobial activities of three typical AMPs, including the designed short AMP, G3, and two natural AMPs, melittin and LL37, against E. coli and their haemolytic activities were studied. Lipopolysaccharide (LPS) and anionic di-palmitoyl phosphatidyl glycerol (DPPG) monolayer models were constructed to mimic the outer membrane and inner membrane leaflets of Gram-negative bacteria. The binding and penetration of AMPs to the model lipid monolayers were systematically studied by neutron reflection via multiple H/D contrast variations. Finding: G3 has relatively high antimicrobial activity, low cytotoxicity, and high proteolytic stability, whilst melittin has significant haemolysis and LL37 has weaker antimicrobial activity. G3 could rapidly lyse LPS and DPPG monolayers within 10-20 min. In contrast, melittin was highly active against the LPS membrane, but the dynamic process lasted up to 80 min, with excessive stacking in the OM. LL37 caused rather weak destruction to LPS and DPPG monolayers, leading to massive adsorption on the membrane surface without penetrating the lipid tail region. These findings demonstrate that the rationally designed AMP G3 was well optimised to impose most effective destruction to bacterial membranes, con-sistent with its highest bactericidal activity. These different interfacial structural features associated with AMP binding shed light on the future development of active and biocompatible AMPs for infection and wound treatments. (c) 2023 The Authors. Published by Elsevier Inc. This is an open access article under the CC BY license (http:// creativecommons.org/licenses/by/4.0/)
