Latest ArticlesThe external stimulus response strategy has been evolved rapidly in the field of olefin polymerization. In this work, we modularly synthesized three types of double stimulus responsive α-diimine palladium catalysts, combining redox regulation and other regulation together, such as light, Lewis acid and alkali cations. The catalytic activities and the molecular weight of polyethylene products can be regulated for 4 times in ethylene polymerization. These palladium complexes were also used for the copolymerization reaction of ethylene and polar monomers, such as methyl 10-undecylenate and methyl acrylate, effectively regulating the catalytic activities, the molecular weight and polar monomer incorporation of the prepared copolymers. The research on these dual-regulated palladium complexes makes full use of prepared catalysts and provides new inspirations for regulating olefin polymerization.
Lithium-sulfur batteries (LSBs) boasting remarkable energy density have garnered significant attention within academic and industrial spheres. Nevertheless, the progression of LSBs remains constrained by the languid redox kinetics intrinsic to sulfur and the pronounced shuttle effect induced by lithium polysulfides (LiPSs), which seriously affecting the energy density, cycling life and rate capacity. The conceptualization and implementation of catalytic materials stand acknowledged as a propitious stratagem for orchestrating kinetic modulation, particularly in excavating the conversion of LiPSs and has evolved into a focal point for disposing. Among them, chalcogenide catalytic materials (CCMs) have shown satisfactory catalytic effects ascribe to the unique physicochemical properties, and have been extensively developed in recent years. Considering the lack of systematic summary regarding the development of CCMs and corresponding performance optimization strategies, herein, we initiate a comprehensive review regarding the recent progress of CCMs for effective collaborative immobilization and accelerated transformation kinetics of LiPSs. Following that, the modulation strategies to improve the catalytic activity of CCMs are summarized, including structural engineering (morphology engineering, surface/interface engineering, crystal engineering) and electronic engineering (doping and vacancy, etc.). Finally, the application prospect of CCMs in LSBs is clarified, and some enlightenment is provided for the reasonable design of CCMs serving practical LSBs.
The development of large-scale cell cultivation and non-invasive cell harvesting is highly desired in various fields, including biological regeneration and pharmaceutical research. When using traditional microcarriers for cell culture, trypsinization is often necessary during cell collection, leading to partial cells damage. In this work, we developed a thermoresponsive glass microcarrier modified with poly(γ-propargyl-ʟ-glutamate) (PPLG) and poly(N-isopropylacrylamide) (PNIPAM). We utilized these microcarriers for three-dimensional cell culture and enzyme-free cell harvesting, and the results indicated that the prepared microcarriers exhibited excellent non-invasive cell culture performance.
Developing efficient and long wavelength sensitive unimolecular photoinitiators (PIs) is still facing a great challenge. In this work, a series of thioxanthone-based N-hydroxyphthalimide esters (TX-NHPIEs) were synthesized by installing NHPIEs along the TX backbone and characterized. The investigated TX-NHPIEs have a 60 nm redshift and demonstrate sterling initiating efficiency for free radical photopolymerization (FRP) under LED@450 nm light irradiation compared with the commercialized isopropylthioxanthone (ITX). Real-time 1Hnuclear magnetic resonance (1H NMR), electron spin resonance (ESR), decarboxylation and gas chromatograph-mass spectrometer (GC–MS) experiments and density functional theory (DFT) reveal that TX-NHPIEs can generate one alkyl radical and one N-centered iminyl radical, which can initiate FRP directly and indirectly, respectively. In other words, TX-NHPIEs absorb one photon and can generate two active radicals, which break through the limitations of common PIs. TX-NHPIE-Cpe demonstrates the highest initiating efficiency, and its application in coatings and 3D printing was also studied, indicating TX-NHPIEs have broad potential applications in photopolymerization processes.
The photocatalytic conversion of biomass into high-value chemicals, coupled with simultaneous hydrogen (H2) evolution, leveraging the electrons and holes generated by solar energy, holds great promise for addressing energy demands. In this study, we constructed a dual functional photocatalytic system formed by NiS loaded on Ni doped two-dimensional (2D) CdS nanosheet (NiS/Ni-CdSNS) heterostructure for visible-light-driven H2 evolution and ethanol oxidation to acetaldehyde. Remarkably, the 2D NiS/Ni-CdSNS exhibited significant activity and selectivity in both photocatalytic H2 evolution and ethanol oxidation, achieving yields of 7.98 mmol g−1 h−1 for H2 and 7.33 mmol g−1 h−1 for acetaldehyde. The heterogeneous interface of the composite facilitated efficient charge separation, while NiS provided abundant sites for proton reduction, thereby promoting the overall dual-functional photocatalytic activity. Density functional theory calculations further reveal that both Ni doping and NiS loading can reduce the reaction energy barrier of ethanol oxidation of free radicals, and NiS/Ni-CdSNS composite materials exhibit stronger ethanol C-H activation ability to generate key intermediate •CH(OH)CH3 on the surface. This work serves as a valuable guide for the rational design of efficient dual functional photocatalytic systems that combine H2 evolution with the selective conversion of organic compounds into high-value chemicals.
Formic acid (FA), which is obtainable through CO2 hydrogenation with green hydrogen or biomass conversion, has been used as a prospective liquid organic hydrogen carrier (LOHC) because of the abundant advantages of renewability, wide availability, stability, and high volumetric capacity (53 g H2/L). The development of highly efficient catalytic systems to achieve enhanced catalytic activity is attractive but still challenging. Herein, ultrafine and highly dispersed PdAu nanoclusters (NCs) anchored on amino-modified reduced graphene oxide (ArGO) were successfully synthesized via a facile impregnation-reduction method and applied as a catalyst toward formic acid dehydrogenation (FAD). Benefiting from the promoting effect of amino groups, the strain and ligand effect in the alloy, and the Mott–Schottky effect between PdAu NCs and ArGO, the resultant PdAu/ArGO affords an ultrahigh activity under visible light irradiation with an exceptional turnover frequency value of 10, 699.5 h−1 at 298 K without any additives, more than 2.6 times improvement than that under dark, which is the highest among all reported catalysts under the same conditions. This study provides a green and convenient strategy for developing more efficient and sustainable FAD catalysts and promotes the effective utilization of FA as a prospective renewable LOHC.
Disgusting deposits (e.g., scale and crude oil) in daily life and industrial production are always serious problems, posing great threats to the safety and economic development. However, most of developed coatings can only conquer one part of these deposits such as superhydrophobic coatings possess anti-scaling capacity but would adhere crude oil. To integrate scale resistance with oil repellence, we herein report a robust superamphiphobic (SAB) coating simultaneously reducing pollution of scale and oil for extended period of time (two weeks with over 98% reduction). Compared with single role of superhydrophobic and amphiphilic surfaces, the SAB coating can not only inhibit interfacial nucleation of scale but also reduce the adhesion of formed scale and polluted oil. The durability of the SAB coating is evaluated via mechanical tests (sandpaper abrasion, tape stripping and sand falling) and chemical corrosion (corrosive liquid immersing), revealed by sustainable high contact angles and low contact angle hysteresis of water and oil. The universality of this strategy can be further confirmed by adding different particles like kaolin, Al2O3, and SiO2, resisting multiple types of scale (i.e., CaSO4, BaSO4 and MgCO3) and oil (i.e., glycerol, glycol, and mineral oil). Therefore, this study provides an ideal avenue for resisting scale and oil, which may be used for conquering the complexity of application environments (e.g., oil production and transportation).
Fe-based Fenton agents can generate highly reactive and toxic hydroxyl radicals (·OH) in the tumor microenvironment (TME) for chemodynamic therapy (CDT) with high specificity. However, the low pH environment and insufficient endogenous hydrogen peroxide (H2O2) of the highly efficient Fenton reaction limits its practical application in clinic. Here, a Cu(Ⅱ)-doped mesoporous silica nanoagent (Cu-MSN) with excellent dispersity was successfully developed. After loaded with doxorubicin (DOX) and ascorbate (AA), Cu-MSN@DA was coated with active targeting ligand folic acid (FA), dimethyl maleic an-hydride (DMMA) and carboxymethyl chitosan (CMC) to obtain an active transporting nanoagent (FCDC@Cu-MSN@DA) with tunable charge-reversal property, which is more adaptable to the pH value of TME than Fe-based Fenton agents, and can self-supply exogenous H2O2 by ascorbate to produce more toxic ·OH to trigger the apoptosis of cancer cells. Meanwhile, the high level of glutathione (GSH) in TME can reduce Cu(Ⅱ) to Cu(Ⅰ) by Fenton-like reaction, increasing the generation rate of ·OH and relieving tumor antioxidant ability. The supply of exogenous H2O2 significantly enhanced the synergistic effect of CDT by oxidative damage. Together with DOX-induced cell apoptosis, this novel nanoagent FCDC@Cu-MSN@DA can achieve maximum therapeutic efficacy, creating a new model of safe and effective tumor treatment with high specificity.
A solid electrolyte interphase (SEI) with a robust mechanical property and a high ionic conductivity is imperative for high-performance zinc metal batteries. However, it is difficult to form such a SEI directly from an electrolyte. In this work, a molecular crowding effect is based on the introduction of Zn(OTF)2 and Zn(ClO4)2 to 2 mol/L ZnSO4 electrolytes. Simulations and experiments indicate that the Zn(OTF)2 and Zn(ClO4)2 not only create a molecularly crowded electrolyte environment to promote the interaction of Zn2+and OTF−, but also participate in the reduction to construct a robust and high ionic-conductive SEI, thus promoting metal zinc deposition to the (002) crystal surface. With this molecular crowding electrolyte, a high current density of 1 mA/cm2 can be obtained by assembling symmetric batteries with Zn as the anode for over 1000 h. And in a temperature environment of −10 ℃, a current density of 1 mA/cm2 can be obtained by assembling symmetric batteries with Zn for over 200 h. Zn//Bi2S3/VS4@C cells achieve a CE rate of up to 99.81% over 1000 cycles. Hence, the utilization of a molecular crowding electrolyte is deemed a highly effective approach to fabricating a sophisticated SEI for a zinc anode.
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