Latest ArticlesSulfidation of zero-valent iron (ZVI) has attracted broad attention in recent years for improving the sequestration of contaminants from water. However, sulfidated ZVI (S-ZVI) is mostly synthesized in the aqueous phase, which usually causes the formation of a thick iron oxide layer on the ZVI surface and hinders the efficient electron transfer to the contaminants. In this study, an alcohothermal strategy was employed for S-ZVI synthesis by the one-step reaction of iron powder with elemental sulfur. It is found that ferrous sulfide (FeS) with high purity and fine crystallization was formed on the ZVI surface, which is extremely favorable for electron transfer. Cr(Ⅵ) removal experiments confirm that the rate constant of S-ZVI synthesized by the alcohothermal method was 267.1- and 5.4-fold higher than those of un-sulfidated ZVI and aqueous-phase synthesized S-ZVI, respectively. Systematic characterizations proved that Cr(Ⅵ) was reduced and co-precipitated on S-ZVI in the form of a Fe(Ⅲ)/Cr(Ⅲ)/Cr(Ⅵ) composite, suggesting its environmental benignancy.
Anode free lithium metal batteries (AF-LMBs) have conspicuous advantages both in energy density and the compatibility of battery manufacturing process. However, the limited cycle life of AF-LMBs is a crucial factor hindering its practical application. Fluorinated or nitride artificial inorganic solid electrolyte interphase (SEI) has been found as an effective method to prolong the lifespan of AF-LMBs. Herein, by investigating the impact of nano-sized inorganic gradient layers (LiF or Li3N) on initial Li deposition behavior, we notice that the Li+ diffusion barrier and the deposition morphology are highly depended on the thickness of inorganic layers. Thicker protective layers cause larger overpotential as well as more aggregated Li+ distribution. This study reveals that the ideal SEI should be synthesized thin and uniformly enough and uncontrollable artificial SEI can cause damage to the lifespan of AF-LMBs.
Chemodynamic therapy (CDT) combined with dual phototherapy (photothermal therapy (PTT) and photodynamic therapy (PDT)) is an efficient way to synergistically improve anti-tumor efficacy. However, the combination of multiple modes often makes the composition of the system more complex, which is not conducive to clinical application. In this study, a dual phototherapy ligand carboxyl-modified Aza-BODIPY (BOD-COOH) and metal active center Cu2+ were used to construct multiple-modes metal-photosensitizer nanoparticles (BOD-Cu NPs) via one-step coordination self-assembly for combination therapy of CDT/PDT/PTT. In order to improve delivery efficiency, the targeted hydrophilic molecule pyridine-modified glucose derivative (G-Py) was synthesized and coated onto the BOD-Cu NPs to form a glycosylated nano metal-photosensitizer BOD-Cu@G by electrostatic interaction. The Cu2+ in BOD-Cu@G could not only be used as a coordination node for metal-driven self-assembly but also consume intracellular glutathione (GSH), and then catalyze Fenton-like reaction to generate hydroxyl radical (·OH) for CDT. In vitro and in vivo studies revealed that BOD-Cu@G could achieve excellent anti-tumor efficiency by CDT-enhanced dual phototherapy.
Improving the highly selective and sensitive binding of chemosensor to target guest is always very challenging. In order to solve this issue, herein, the enrichment effect was introduced into the design of chemosensor molecule. A novel bi-fused-macrocyclic host molecule BPN1 was synthesized by bridging a pillar[5]arene and a naphthalene diimide (NDI) group through hydrogen-bond-rich chain. In the BPN1, the naphthalimide side ring is outside the cavity of the pillar[5]arene. In addition, Cr(Ⅵ) greatly threat human health and the environment due to its severe toxicity, and it is very important to develop effective chemosensor for sensitive and selective detection of Cr2O72− or its ion pairs. In this paper, the novel bi-fused-macrocyclic host molecule BPN1 can recognize Cr2O72− with high selectivity and sensitivity. The mechanism of BPN1 recognition of Cr2O72− was studied through experiments and density functional theory (DFT), the results show that BPN1 could supply enrichment effect to bind Cr2O72− through multiple weak interactions such as hydrogen bonds and anion-π, and achieve highly sensitive and selective detection of Cr2O72−. It is a significant and feasible strategy for improve high selectivity and sensitivity of host to specific objects by using the enrichment effect of fused bi-macrocyclic.
Transition-metal-catalyzed cross-electrophile coupling has emerged as a reliable method for constructing carbon–carbon bonds. Herein, we report a general method, cobalt-catalyzed reductive alkynylation, to construct C(sp)-C(sp3) and C(sp)-C(sp2) bonds. This presented reaction has a broad substrate scope, enabling the efficient cross-electrophile coupling between alkynyl bromides with alkyl halides and aryl or alkenyl (pseudo)halides. This presented reaction is conducted under mild conditions, tolerating many functional groups, thus suitable for the modification and synthesis of biologically active molecules.
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.
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.
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).
Herein, we report the NHC-Ru catalyst system that realizes the chemo-selective transformation of ketones with methanol. By simply changing the base, a broad range of structurally diverse ketones, could be selectively and efficiently converted to the corresponding β-methylated secondary alcohols or secondary alcohols. Remarkably, this catalytic system was very effective for the synthesis of bio-related molecules and deuterated alcohols, as well as the three-component coupling between methyl ketones, primary alcohols, and methanol. The reaction mechanism was further revealed by experiment and DFT mechanistic investigations.
A highly efficient and concise bromocyclization has been successfully achieved, in which tryptamine/tryptophol derivates can be transformed to valuable HPI/TFI scaffolds with economic and green manners. Moreover, a controllable cascade transformation of bromocyclization and aromatic bromination has also been smoothly achieved to form dibrominated HPIs and TFIs. Production could be successfully scaled up under both the batch process and a continuous flow fashion. The most remarkable peculiarity of our process over all previous methods is that the generated water is the major waste. Notably, successful application of this new protocol has been demonstrated by the pharmaceutical and natural products syntheses.
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