Latest ArticlesDegradation of nitrobenzene (NB) via Fenton-like reaction is considered as an efficient approach for contaminated groundwater remediation. However, the poor stability of H2O2 limits the application of traditional Fenton reactions in soil and groundwater due to the transportation risks of H2O2. In this study, we synthesized a controlled release nano calcium peroxide (nCP) by coating it with polydopamine (PDA) as a solid H2O2 to construct a Fe(Ⅱ)/PDA@nCP Fenton-like system for contaminants degradation. The phenol-quinone transformations of catechol groups on the PDA surface facilitated the Fe(Ⅱ)/Fe(Ⅲ) cycle, resulting in enhanced generation of hydroxyl radicals (HO) and effective long-term degradation of NB. Moreover, the PDA shell modulated the nCP decomposition rate and inhibited sharp pH fluctuations, and the NB removal efficiency was achieved up to 96.8% at pH ranging from 3.0 to 9.0. This study demonstrated the promising application potential of PDA@nCP as a solid-controlled release H2O2 source in Fenton-like system for groundwater contamination remediation.
Advanced oxidation processes (AOPs) governed by peroxide activation to produce highly oxidative active species have been extensively explored for environmental remediation. Nevertheless, the low diffusion rates, inadequate interactions of the reactants, and limited active site exposure hinder treatment efficiency. Porous carbocatalysts with high specific surface area, tunable pore size, and programmable active sites demonstrate outstanding performance in activating diverse types of peroxides to generate active species for treatment of aqueous organic pollutants. The pore-rich structures enhance reaction kinetics for peroxide activation by facilitating diffusion of the reactants and their interactions. Additionally, the structural flexibility of porous structures favors the accommodation of highly dispersed metal species and allows for precise tuning of the microenvironment around the active sites, which further enhances the catalytic activity. This review critically summarizes the recent research progress in the applications of engineered porous carbocatalysts for peroxide activation and outlines the prevailing pore construction methods in carbocatalysts. Moreover, engineering strategies to regulate the mass transfer efficiency and fine-tune the microenvironment around the active sites are systematically addressed to enhance their catalytic peroxide activation performances. Challenges and future research opportunities pertaining to the design, optimization, mechanistic investigation, and practical application of porous carbocatalysts in peroxide activation are also proposed.
Pure organic materials with ultralong room-temperature phosphorescence (RTP) and persistent luminescence in broad color gamut exhibit tremendous potential and broad application prospects due to their unique optical properties. This article proposes a simple strategy, polyatomic synergistic effect, to endow persistent luminescent materials with ultralong lifetime and broad color-tunability through polyatomic synergistic effect and non-traditional phosphorescence resonance energy transfer (PRET). By leveraging the polyatomic synergistic effect to enhance the intersystem crossing (ISC) in bibenzimidazole (BBI) derivatives and suppress the non-radiative transition process, ultralong persistent room-temperature phosphorescence has been successfully achieved after incorporating BBI-Cl-M into poly(methyl methacrylate) (PMMA) to form a rigid matrix(BBI-Cl-M@PMMA). Specifically, the ester functionalized bibenzimidazole with modified chlorine on molecular skeleton (BBI-Cl-M) demonstrates a remarkable phosphorescent lifetime (τp) of up to 256.4 ms. In addition, the behaviors and mechanism of RTP via polyatomic synergistic effect have been further understood by theoretical calculation and single crystal analysis. Subsequently, utilizing BBI-Cl-M as the energy donor and Rhodamine B (RB) as the energy acceptor, persistent and multicolor organic afterglow covering from green to red has been realized successfully by simply regulating the doping composition and concentration of PRET systems. These RTP materials have also been applied in underwater afterglow emission and multilevel anti-counterfeiting technology successfully.
Intracellular bacteria (ICB), cloaked by the protective barriers of host cells, pose a formidable challenge to selective and efficient eradication. The employment of activatable photosensitizers based antibacterial photodynamic therapy (aPDT) holds significant potential for selective imaging and photo-inactivation of ICB while minimizing side effects on normal cells. Drawing inspiration from the elevated hypochlorous acid (HClO) levels in ICB infected phagocytes, herein we firstly designed and synthesized a series of HClO-responsive dinuclear Ru(Ⅱ) complexes (Ru1-Ru3) to achieve such a goal. Initially, the luminescence, 1O2 generation and aPDT activity of these Ru(Ⅱ) complexes were suppressed due to the quenching effect of the azo group, but were recovered after reaction with HClO in solutions or within ICB infected phagocytes. The detailed results revealed that Ru1 and Ru3 could not only selectively visualize ICB, but also demonstrated remarkable aPDT activity against ICB, surpassing vancomycin both in vitro and in vivo.
The asymmetric conjugate additions of aryl Grignard reagents to trisubstituted enones by chiral P, N ligand L6 with low catalyst loading (0.25–1.0 mol%) are disclosed. Chiral 2-ester chromanone and its analogs bearing a quaternary stereogenic centers at C2 position were produced in high to excellent yields, enantioselectivities and high turnover number. The notable features of this reaction include its broad substrate scope, complete 1, 4-addition regioselectivities, applicability to both batch and flow for large scale synthesis. This report develops an efficient strategy to apply aryl Grignard reagents in asymmetric 1, 4-conjugation reactions and provides a direct method to incorporate quaternary chiral centers toward the synthesis of biologically relevant chromanone derivatives.
2, 6-Diisopropylaniline reacts with an open-cage fullerene derivative with a 11-membered orifice and forms an open-cage derivative containing one imino group on the rim of the expanded orifice. Further treatment with Lewis acids leads to open-cage fullerenes with an 18-membered orifice. Instead of the direct addition process observed before for less bulky anilines, an electron transfer process takes place in the initial step in the present reaction with bulky 2, 6-diisopropylaniline. As a result, the chemo-selectivity is completely different affording the mono imino open-cage derivative selectively.
Photoredox-mediated reversible-deactivation radical polymerization (RDRP) is an effective approach to synthesize polymers with defined composition and architecture. Current photoinduced RDRP primarily depends on outer-sphere electron transfer or homolysis mechanisms. Herein, we describe an example of iodine-mediated RDRP facilitated by photoinduced charge transfer complex (CTC) catalysis. The approach uses cheap and easily accessible N-heterocyclic nitrenium salt (NHN+···I-) as the photoactive CTC. Upon the irradiation of visible light, NHN+···I- undergoes single electron transfer to generate NHN• and I• radicals. The NHN• radical activates dormant Pn-I polymers via inner-sphere single electron transfer, leading to the propagating Pn• radical for chain growth and the I- anion for recovering the CTC, and the I• radical deactivates the polymerization via coupling with Pn•.
Halide solid-state electrolytes (HSSEs) with excellent ionic conductivity and high voltage stability are promising for all-solid-state Li-ion batteries (ASSLBs). However, they suffer from poor processability, mechanical durability and humidity stability, hindering their large-scale applications. Here, we introduce a dry-processing fibrillation strategy using hydrophobic polytetrafluoroethylene (PTFE) binder to encapsulate Li3InCl6 (LIC) particles (the most representative HSSE). By manipulating the fibrillating process, only 0.5 wt% PTFE is sufficient to prepare free-standing LIC-PTFE (LIC-P) HSSEs. Additionally, LIC-P demonstrates excellent mechanical durability and humidity resistance. They can maintain their shapes after being exposed to humid atmosphere for 30 min, meanwhile still exhibit high ionic conductivity of > 0.2 mS/cm at 25 ℃. Consequently, the LIC-P-based ASSLBs deliver a high specific capacity of 126.6 mAh/g at 0.1 C and long cyclability of 200 cycles at 0.2 C. More importantly, the ASSLBs using moisture-exposed LIC-P can still operate properly by exhibiting a high capacity-retention of 87.7% after 100 cycles under 0.2 C. Furthermore, for the first time, we unravel the LIC interfacial morphology evolution upon cycling because the good mechanical durability enables a facile separation of LIC-P from ASSLBs after testing.
Electrochemical water splitting presents a promising, environmentally friendly alternative to fossil fuels for hydrogen production. However, the efficiency is constrained by the sluggish kinetics and high overpotentials associated with the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). While noble metal catalysts, such as Pt for HER and Ir for OER, currently offer superior performance, their widespread adoption is hindered by high cost and scarcity. This has spurred research into cost-effective alternatives, with a focus on understanding the underlying electrocatalytic mechanisms. MXenes, a class of two-dimensional materials, have emerged as promising candidates for electrocatalytic water splitting due to their unique physical and chemical properties. However, research in this field remains largely experimental, lacking a comprehensive understanding of fundamental mechanisms. This knowledge gap impedes the development of high-efficiency electrocatalysts and necessitates further investigation. This review systematically examines recent advancements in MXene-based nanohybrids for electrocatalytic water splitting, covering synthetic methods, structure-property relationships, and performance enhancement strategies. It encompasses both precious and non-noble metal-based systems for HER, OER, and overall water splitting applications. Additionally, this review addresses current challenges, opportunities, and future research directions for MXene-based nanohybrids. By providing comprehensive insights into the development of high-performance MXene-based electrocatalysts, this review aims to accelerate progress in the field of electrochemical water splitting. It serves as a valuable resource for researchers and engineers working towards more efficient and sustainable hydrogen production technologies, potentially contributing to the broader goal of transitioning away from fossil fuels towards cleaner energy sources.
Chemotherapy is the cornerstone of cancer treatment, and paclitaxel (PTX), as a first-line broad-spectrum chemotherapy drug, is widely used in the treatment of multiple tumors in the clinic. However, unsatisfactory efficacy and drug resistance of single chemotherapy have severely hampered the clinical progress of PTX. Herein, three-in-one naringenin (NAR)-loaded PTX polymer prodrug micelles were constructed for efficient and synergistic antitumor therapy. Firstly, the polymer prodrug micelles could simultaneously act as nanoreservoirs for two hydrophobic drugs, PTX and NAR. Secondly, the polymer prodrug micelles enabled dual-responsive intelligent release of PTX and NAR triggered by reduction and acid. Finally, released PTX and NAR exerted synergistic antitumor effects for reversing tumor resistance, while NAR enhanced the immune and anti-inflammatory functions of polymer prodrug micelles. Due to the cascade-enhanced chemotherapeutic augmentation, the intelligent-responsive nanoreservoir proved to be an excellent antitumor therapeutic platform. This work was of great interest for designing superior chemotherapeutic augmentation regimens.
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