Latest ArticlesIt has been challenging for Fe(Ⅲ) regeneration in Fe-based photocatalysts for continuous peroxydisulfate (PDS) activation due to the lower ability to reduce Fe(Ⅲ). In this work, Fe-doped ultrathin VO2 (Fe-VO2) nanobelts were synthesized for purifying metronidazole (MNZ) via PDS activation. As an efficient Fenton-like catalyst for PDS activation, 2 wt% Fe-doped VO2 can remove 98% of MNZ within 40 min and exhibits impressive recyclability. The synergistic effect of Fe-VO2 and Fe(Ⅲ) activated PDS boosted the photocatalytic performance. Moreover, SO4•−, h+, O2•−, 1O2, and •OH were the main reactive radicals. The effects of initial MNZ concentration, Fe-VO2, PDS dosage, and various anions/cations on MNZ removal by the Fe-VO2/PDS/Vis system were studied. The intermediates of MNZ degradation and possible pathways were determined by density function theory (DFT) calculations and HPLC-MS. This study provided a sustainable technology using Fe-doped ultrathin VO2 nanobelts for photocatalytic PDS activation and decontamination of pharmaceutical wastewater.
Pyrrole is a heterocycle with four carbon atoms and a nitrogen atom, which is extensively used in the pesticide and pharmaceutical industries. In addition, it has a series of analogs such as pyrrolidine, pyrroline, and pyrrolidone. Pesticides containing pyrrole and its analogs have been formally marketed as fungicides, including fenpiclonil, fludioxonil, the insecticide chlorfenapyr, and the herbicide fluorochloridone. In this paper, we analyze the structure-activity relationships (SARs) of pesticides containing these structures. We summarize the characteristics possessed by the most highly active pyrrole and its analogs and provide an overview of research on pyrrole compounds with insecticidal, antimicrobial, herbicidal, and antiviral properties in the past 20 years. It is hoped to provide ideas for the development and design of this type compounds in pesticides and to assist researchers in this area.
In contrast to research on active sites in nanomaterials, lithium tantalate single crystals, known for their exceptional optical properties and long-range ordered lattice structure, present a promising avenue for in-depth exploration of photocatalytic reaction systems with fewer constraints imposed by surface chemistry. Typically, the isotropy of a specific facet provides a perfect support for studying heteroatom doping. Herein, this work delves into the intrinsic catalytic sites for photocatalytic nitrogen fixation in iron-doped lithium tantalate single crystals. The presence of iron not only modifies the electronic structure of lithium tantalate, improving its light absorption capacity, but also functions as an active site for the nitrogen adsorption and activation. The photocatalytic ammonia production rate of the iron-doped lithium tantalate in pure water is maximum 26.95 µg cm−2 h−1, which is three times higher than that of undoped lithium tantalate. The combination of first-principles simulations with in situ characterizations confirms that iron doping promotes the rate-determining step and changes the pathway of hydrogenation to associative alternating. This study provides a new perspective on in-depth investigation of intrinsic catalytic active sites in photocatalysis and other catalytic processes.
The imbalance of nitric oxide (NO) homeostasis in the brain is closely related to the occurrence of Parkinson’s disease (PD). Therefore, revealing the fluctuation of NO in brain is crucial for understanding the pathophysiological processes. However, currently developed NO probes are unsuitable for this purpose due to their poor blood-brain barrier permeability. Herein, a fluorescent probe (PO-NH) with blood-brain barrier crossing capability and high selectivity for NO was developed. Under the NO mediation, the photo-induced electron transfer (PET) process of the probe was blocked, giving an intensive fluorescence enhancement (F/F0 = 15). Moreover, PO-NH can be used to effectively monitor changes in intracellular NO levels. Significantly, due to excellent blood-brain barrier crossing ability and near-infrared (NIR) emission, PO-NH is suitable for in vivo imaging of NO in the brain and illustrating with the deterioration of PD, the level of NO gradually increased in the brain of PD mice. We believe that PO-NH may provide a beneficial tool for understanding the biological function of NO in the brain and revealing the complex connection between NO and PD.
Colon-targeted oral drug delivery systems are one of the most promising therapeutic strategies for alleviating and curing inflammatory bowel disease (IBD), but they still face challenges in successfully passing through the harsh gastrointestinal environment and intestinal mucus barrier. To overcome the gastrointestinal barriers for oral drug delivery mentioned above, a "spore-like" oral nanodrug delivery platform (Cur/COS/SC NPs) has been developed. Firstly, chitooligosaccharides (COS) are encapsulated on the surface of Curcumin nanoparticles (Cur NPs) to form carrier-free nanoparticles (Cur/COS NPs). Subsequently, inspired by the natural high resistance of spore coat (SC), SC is chosen as the "protective umbrella" to encapsulate Cur/COS NPs for precision targeted therapy of IBD. After oral administration, SC can effectively protect NPs through the rugged gastrointestinal environment and exhibit excellent intestinal mucus penetration characteristics. Moreover, the negatively-charged Cur/COS/SC NPs specifically target positively-charged inflamed colon via electrostatic interactions. It is demonstrated that Cur/COS/SC NPs can promote the expression of tight junction proteins, inhibit aberrant activation of the Toll-like receptor 4/myeloid differentiation primary response gene 88/nuclear factor-κB (TLR4/MyD88/NF-κB) signaling pathway, and downregulate the levels of pro-inflammatory factors, exhibiting excellent anti-inflammatory effects. Notably, it is found that Cur/COS/SC NPs can significantly increase the richness and diversity of gut microbiota, and restore the homeostasis of gut microbiota by inhibiting pathogenic bacteria and promoting probiotics. Hence, Cur/COS/SC NPs provide a safe, efficient, and feasible new strategy for IBD treatment.
The alkaline hydrogen evolution reaction (HER) is a crucial process for sustainable hydrogen production, yet it requires efficient and stable electrocatalysts to overcome the high activation energy barrier. The article discusses a novel strategy for enhancing the performance of Ni-Fe layered double hydroxide (Ni-Fe LDH) in the alkaline HER by modifying it with a frustrated Lewis acid-base pair (FLP) constructed through vacancy engineering. The study found that the modified Ni-Fe LDH exhibited improved alkaline HER performance. Density functional theory (DFT) calculations demonstrate that the introduction of FLP can activate water and protons more efficiently than monometallic sites, thus reducing the alkaline HER energy barrier and overpotential. In HER under alkaline conditions, the Volmer step involves an additional hydrolysis dissociation compared to acidic conditions, which is one of the factors contributing to the slow reaction kinetics. This paper demonstrates that FLPs can alter the rate-determining step in alkaline HER from the Volmer step to a step with a lower energy barrier, more suitable for hydrogen desorption. The work provides new insights into the role of FLPs in regulating the mechanism and kinetics of HER and opens a new direction for the design and optimization of LDH-based and other electrocatalysts.
Gliomas are the most common intracranial tumors with poor survival and high mortality. Furthermore, the clinical efficacy of current drugs is still not ideal; despite the development of several therapeutic drugs over the past decades and tumor progression or recurrence is inevitable in many patients. RNAi-based therapy presents a novel disease-related gene targeting therapy, including otherwise undruggable genes, and generates therapeutic options. However, the therapeutic effect of siRNA is hindered by multiple biological barriers, primarily the blood-brain barrier (BBB). A glycoprotein-derived peptide-mediated delivery system is the preferred option to resolve this phenomenon. RDP, a polypeptide composed of 15 amino acids derived from rabies virus glycoprotein (RVG), possesses an N-type acetylcholine receptor (nAChR)-binding efficiency similar to that of RVG29. Given its lower cost and small particle size when used as a ligand, RDP should be extensively evaluated. First, we verified the brain-targeting efficacyy of RDP at the cellular and animal levels and further explored the possibility of using the RDP-oligoarginine peptide (designated RDP-5R) as a bio-safe vehicle to deliver therapeutic siRNA into glioma cells in vitro and in vivo. The polypeptide carrier possesses a diblock design composed of oligoarginine for binding siRNA through electrostatic interactions and RDP for cascade BBB- and glioma cell-targeting. The results indicated that RDP-R5/siRNA nanoparticles exhibited stable and suitable physicochemical properties for in vivo application, desirable glioma-targeting effects, and therapeutic efficiency. As a novel and efficient polypeptide carrier, RDP-based polypeptides hold great promise as a noninvasive, safe, and efficient treatment for various brain diseases.
Aqueous zinc-based energy storage devices (ZESDs) have garnered considerable interest because of their high specific capacity, abundant zinc reserves, excellent safety, and environmental friendliness. In recent years, various types of boron, nitrogen co-doped carbon (BNC) materials have been developed to improve electrochemical performance of ZESDs. To promote the advancement of these technologies, we herein give a comprehensive review of the progress in BNC materials for ZESDs. The different synthetic methods employed in the preparation of BNC materials, including direct carbonization, template method, chemical vapor deposition, hydrothermal method, etc., are summarized. These methods play a vital role in tailoring the structure, composition, and properties of BNC materials to optimize their performance in energy storage applications. Furthermore, some key achievements of BNC materials in zinc-air batteries and zinc-ion hybrid supercapacitors are elaborated. Lastly, future challenges and development directions of BNC materials in ZESDs are prospected. This comprehensive review could serve as a valuable resource in the energy storage field, providing insights into the potential of BNC materials in zinc-based energy storage technologies.
CO2 electrolysis into formate is a promising technology with the potential to simultaneously alleviate energy shortages and global warming. However, the limited stability of the catalysts during long-term electrolysis hinders their widespread implementation. Herein, we show that a core-shell bimetallic BiAg catalyst with a multifaceted Janus structure at its core can achieve a stability of up to 300 h with a formate faradaic efficiency (FEformate) over 90% at −0.75 V vs. RHE (reversible hydrogen electrode) in an H-type cell. Our investigations reveal the important role of the Janus structure on the transfer of electrons, favoring their delocalization across the catalyst and enhancing their mobility. We propose that the compressive strain inclined to grain boundaries within this structure would lower the energy barrier for electrons transfer and promotes the cooperation between Ag and Bi. Indeed, Ag initiates the activation of CO2 through a series of cascade reactions and is subsequently hydrogenated on Bi. Additionally, our study suggests that Ag plays a crucial role in stabilizing the catalyst structure after long-term electrolysis. This work highlights a new strategy for tandem CO2 electrolysis, providing novel insights for the design of formate formation catalysts.
Introducing ligand into the surface of gold (Au)-based catalyst has been recognized as an efficient strategy to enhance the performance of catalyst in acetylene hydrochlorination reaction. However, due to the multifactorial deactivation, the usage of single type of ligand has limitations on the performance improvement. In this work, two types of ligands including a molecular 2-methylimidazole and an ionic cetrimonium are selected to protect Aun+ species. After kinetics analysis, advanced characterization, and density functional theory simulation, we demonstrate the optimal interaction model between two ligands and Au species: Two 2-methylimidazole molecules are coordinated with high-valent Au species while cetrimonium is interacted via electrostatic interaction. Except the synergistic effect in the decrease of Au species reduction and agglomeration, the existence of molecular ligand greatly increases the adsorption of hydrogen chloride while the ionic ligand significantly inhibits the deposition of coke. Due to the positive effect of dual-ligands, we achieved 97.1% of acetylene conversion and 0.29 h−1 of deactivation rate under high gas hourly space velocity of acetylene. This work establishes a foundation to explore the property-activity relationships in Au-based catalyst via ligand engineering.
No. 86 Xueyuan South Road, Haidian District, Beijing
010-62662699(Operation and Technical Support)
qkjq@cast.org.cn
Copyright © 2025 China Association for Science and Technology. All rights reserved. For all open access content, the relevant licensing terms apply.
Sponsored by the Office of the Leading Group for Cybersecurity and Informatization of CAST, and supported by Science and Technology Review Publishing House
