CARBOHYDRATE POLYMERS
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2025
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IF 12.5
Meiting Liu,Hongbin Pu,Da-Wen Sun
Microplastics that eventually convert into nanoplastics are emerging global pollutants and the development of efficient adsorbents for their removal is urgently needed. For sustainability and eco-friendliness, in the current study, a polysaccharide aerogel (LPA) was prepared with lily bulbs as the raw material by following water bath extraction, purification and freeze-drying processes. The prepared porous LPA was then applied as a packing material in a mini adsorption column for removing polystyrene (PS) microplastics and nanoplastics. Results revealed that LPA was over 90 kDa in size and consisted mainly of glucomannan and the removal efficiencies for microplastics and nanoplastics were 93.68 % and 96.98 %, respectively, mainly due to hydrogen bonding interactions and porous structure. The adsorption column was robust and maintained a remarkable removal efficiency (over 90 %) for 3 months. In addition, the effects of other extraction methods and pre-freezing conditions before the freeze-drying process were studied. Compared with water bath extraction, ultrasonic-assisted extraction and microwave-assisted extraction transformed the LPA structure, resulting in reduced adsorption ability, while the pre-freezing temperature could be used to adjust the specific surface area. Meanwhile, the effects of temperature and pH of adsorbates were also investigated. The LPA was heat sensitive and not stable under strongly acidic (pH 4) or strongly alkaline (pH 10) conditions, resulting in a sharp decline in removal efficiency. The adsorption behaviour of LPA was further described via adsorption kinetic models, showing that the microplastics and nanoplastics adsorptions could be fitted by pseudo-second-order and pseudo-first-order models, respectively. Moreover, the adsorption performance of LPA was compared with some other aerogels and had a better result. This research provides a promising, sustainable alternative for microplastic and nanoplastic removal that has potential for pollutant adsorption and sample purification as well as a low preparation cost.
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ORGANIC PROCESS RESEARCH & DEVELOPMENT
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2025
·
IF 3.5
Lei Li,Xinyu Ye,Huaixi Liu,Rongwen Lu,Bingtao Tang,Shufen Zhang
Integrating the diazotization and coupling reactions in solid–liquid heterogeneous systems to achieve large-scale, multistep continuous flow synthesis of water-soluble azo dyes remains a significant challenge. During the diazotization process of water-soluble azo dyes, considerable diazonium salt may precipitate, posing potential safety risks. In this study, we established a continuous dynamic tubular reaction system to achieve the multistep continuous heterogeneous synthesis of C.I. Reactive Red 195, a representative water-soluble azo dye. The optimal conditions for continuous diazotization and coupling reactions were determined, achieving a high throughput of 120 L/h and a yield of up to 736 kg/day. The purity of the synthesized dye increased by 20% compared to the commercial C.I. Reactive Red 195, with the K/S value rising from 19.07 to 22.16, indicating enhanced dyeing performance. Density functional theory (DFT) calculations and ab initio molecular dynamics (AIMD) simulations show that 2-naphthylamine-1,5-disulfonic acid diazonium salt (NADA-DS) spontaneously aggregates into stable clusters due to dispersion forces, which leads to precipitation. Furthermore, the thermal stability, impact sensitivity, explosive propagation, and decomposition activation energy of NADA-DS were investigated. The severity and possibility of thermal runaway during the continuous diazotization process are classified as level 1. The risk matrix indicates that the continuous diazotization process risk is acceptable, with the Stoessel criticality diagram categorizing the hazard level as grade 1, signifying a low level of risk. This study promotes safer, more efficient, and sustainable production of water-soluble azo dyes.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Jin Liu,Cong Hu,Xiaoyan Meng,Ying Sun,Bo Zhao,Zian Lin
Phenolic compounds are a kind of persistent organic pollutants (POPs), which are always a threat to human and environment due to their strong toxicity and low biodegradability. Therefore, developing a reliable method to simultaneously detect phenolic pollutants is of great importance to environmental safety and human health. Herein, we combined the advantages of metal organic frameworks (MOFs) and covalent organic frameworks (COFs) to prepare two cyclic trinuclear unit-based metal covalent organic framework (MCOFs, denoted as Cu 3 -TDH COF and Cu 3 -BDU COF) with large specific surface area, good stability and excellent laccase-like activity. Their oxidative degradation ability toward phenolic pollutants was verified, and a dual-channel nanozyme sensor array based on Cu 3 -TDH COF and Cu 3 -BDU COF was constructed for the identification of six phenolic pollutants. Notably, the sensor array can accurately distinguish between different concentrations of phenolic pollutants and different types of phenolic pollutants at the same concentration, even at levels as low as 1 μM. Moreover, three real water samples (rainwater, tap water and wastewater) and 18 unknown samples were also distinguished and differentiated by the sensor array. This study opens up a potential avenue for the design of MCOFs-based nanozyme sensor arrays to simultaneously realize identification and detection of multiple phenolic pollutants.
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APPLIED SURFACE SCIENCE
·
2024
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IF 6.3
Shengyu Shao,Xingting Liu,Renshu Wang,Yuanyuan He,Changhao Bian,Pengfei Sun,Xiaoping Dong
Photocatalysis technology is a promising green route to eliminate antibiotic residues, but current performance still cannot satisfy the practicality. Herein, an EDTA-2Na mediated supramolecular self-assembly strategy was employed to modulate the morphology and microstructure of graphitic carbon nitride (GCN). The obtained EDTA-2Na mediated supermolecule-based GCN (ESGCN) was proved to possess ultrathin flake-like morphology with developed porous structure and Na/O dopants to enhance visible light harvesting. Compared to the pristine GCN and the supermolecule-based GCN (SGCN) without the EDTA-2Na mediation, the ESGCN has more photogenerated charges, decreased charge recombination and accelerated transport/transfer rate, which thus greatly improved photocatalytic activity for degrading tetracycline hydrochloride (TC) and the apparent rate constant is 37.3 and 6.0 times higher than those of the GCN and the SGCN. Additionally, it exhibits excellent universality in degrading various tetracycline antibiotics with a wide pH range and good stability/durability. A possible mechanism of photocatalytic degradation of TC by the ESGCN was elaborated. And the toxicity assessments and mung bean germination experiments also indicate the photocatalytic process can effectively decrease the toxicity and the potential risk of TC to the environment. This work provides a feasible and effective approach to enhance photocatalytic activity of graphitic carbon nitride, which has prominent potentials for elimination of antibiotic residues in environment.
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ADVANCED FUNCTIONAL MATERIALS
·
2024
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IF 18.5
Ran Wang,Li Shi,Elena Yu. Konysheva,Xiaoxiang Xu
Photocatalytic conversion of benzyl alcohol (BA) is a promising means to coproduce H 2 with value-added chemicals. However, there is a lack of an efficient strategy to regulate the selectivity of the BA conversion products. Here, by a simple cocatalyst engineering technique, the selective conversion of BA over Zn 2 In 2 S 5 nanosheets (ZIS) is maneuvered. Two types of cocatalysts, i.e., Pt and Cd, are photo-deposited onto ZIS that can shift the selectivity to diverse products, namely, Pt to benzaldehyde (BAD) and Cd to the carbon-carbon (C─C) coupling compounds. Mechanistic studies indicate that Cd has a high reducing capacity to convert BAD back to the ketyl radical (C
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ENVIRONMENTAL RESEARCH
·
2025
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IF 7.7
Kai Wu,Wenlong Wang,Shubing Yang,Xu Zhang,Peizeng Yang,Yuefei Ji,Jing Chen,Junhe Lu
As global warming intensifies freeze-thaw cycles, the understanding of environmental chemistry processes in ice and their potential impact on global water quality becomes increasingly important. This study investigated the transformation of 1-naphthol in the presence of nitrite (NO 2 - ) under slightly acidic conditions in ice, focusing on the formation of nitro-naphthol. Results demonstrated that increasing NO 2 - concentration enhanced the conversion of 1-naphthol and the formation of nitrated products. This transformation of 1-naphthol was attributed to the freeze-concentration effect, which led to the accumulation of H + , NO 2 - , and 1-naphthol in the liquid-like grain boundary layer amid ice crystals. In this brine, NO 2 - underwent protonation to form reactive nitrous acid (HNO 2 ) and nitrosonium ions (NO + ), which facilitated the nitration, nitrosation, and oxidative coupling reactions, respectively. The pH was shown to influence nitro products formation by altering the HNO 2 to NO + ratio. Toxicity assessment revealed increased toxicity of the NO 2 - /1-naphthol solution after freezing treatment, likely due to the formation of nitrated products, whereas natural organic matter (NOM) reduced this toxicity by suppressing the generation of nitrated products. The findings of this study advance the understanding of NO 2 - chemistry and the behavior of hydroxylated polycyclic aromatic hydrocarbons in cold environments.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-9
·
IF 15.7
Jia Ming-Yang,Zhou Yue-Wen,Yang Jun-Lei,Liu Qinlei,Cai Zhen-Feng
Ullmann-type coupling reactions are one of the most important transformations in organic synthesis. Achieving catalyst-free Ullmann couplings under mild conditions is crucial to extending the scope of traditional carbon-carbon and carbon-heteroatom couplings. Herein, we show that Ullmann couplings can be effectively achieved at room temperature without the need for metal catalysts in MeOH/H 2 O microdroplets. Mechanistic investigations reveal that the Ullmann reaction in microdroplets is driven by •OH radicals and involves a single-electron transfer pathway via nitrogen-centered radicals. This work not only provides fundamental insights into the •OH radical-mediated coupling reactions in microdroplets but also offers a new strategy for catalyst-free Ullmann couplings.
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MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Xingyun Zhao,Chengxiao Zhao,Hao Jia,Yifan Niu,Jiangyan Jin,Xiaojian Liu,Zhenyu Li,Xuemei Qin,Ke Li
Hydrothermal carbon (HTC) and modified hydrothermal carbon coated silica microspheres were optimized and applied for the separation of phenolic acids, standard saccharides and natural oligosaccharides in the extract of Traditional Chinese Herbal Medicine (TCM). The materials obtained were characterized by scanning electron microscope (SEM), Fourier-transform infrared spectroscopy (FT-IR), the BET surface area analysis and the zeta potential. The investigation of the synthesized materials and the purchased amide modified silica stationary phases column was performed with a set of test solutes. Both the synthesized HTC coated silica gel (silica@HTC) and the modified silica@HTC column exhibit excellent hydrophilicity. Notably, the poly(ethyleneimine) (PEI) modified silica@HTC column demonstrates superior chromatographic performance in the separation of saccharides. This work showed significant potential in the modification of novel hydrothermal carbon stationary phases for application in separating polar oligosaccharide compositions from TCM extracts and similar sources.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Tingan Yao,Guohui Dong,Ying Gao,Dongfeng Sun,Hehua Zeng
This study successfully constructed a g-C₃N₄/FeOOH S-scheme heterojunction photocatalyst with lotus-leaf structural effects, addressing the challenges of insufficient oxygen and water adsorption sites and high photocurrent recombination rates in g-C₃N₄ photocatalysts. The optimized photocatalyst exhibits outstanding performance, generating hydroxyl radicals via dual pathways under visible light (generation rate: 2.8 μmol/(L·min)). The lotus-leaf effect in the composite was confirmed through morphology analysis, static water contact angle measurements, and oxygen adsorption/desorption experiments, demonstrating an 18.9-fold enhancement in oxygen capacity. In situ XPS, built-in electric field intensity measurements, and theoretical calculations confirm that the built-in electric field at the interface, directed from g-C₃N₄ toward FeOOH, drives an S-scheme charge transport pathway. This not only achieves efficient spatial separation of photogenerated carriers but also uniquely preserves the system's strongest redox capability, significantly enhancing photocatalytic efficiency. Furthermore, in situ infrared spectroscopy and electron paramagnetic resonance studies confirm the composite material's dual-channel mechanism for hydroxyl radical generation via oxygen reduction and water oxidation. This work provides robust experimental and theoretical foundations for understanding and designing S-scheme heterojunctions for dual-channel hydroxyl radical generation in photocatalysis.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Yonghao Wang,Shanshan Lei,Miao Liu,Ming Zhou,Zhiwei Zou,Youmei Liu,Xiaomei Zheng
Electrocatalytic reduction of nitrate (NO 3 RR) to ammonia is considered as a promising strategy for nitrogen resource recovery from nitrate-contaminated water. However, conventional Cu-based catalysts often suffer from poor selectivity, with toxic nitrite accumulation and sluggish reduction kinetics. This work reports a Cu Co co-loaded carbon catalyst (CuCo-C) that leverages electron-deficient Cu sites in synergy with Co to significantly enhance the NO 3 RR activity and ammonia selectivity. The optimized CuCo-C discloses a nitrate removal rate of 94 %, an ammonia selectivity of 99 % and multi-turn stability. The combination of comprehensive surface analysis and experimental techniques reveals that the high NO 3 − -to-NH 4 + performance results from Co-induced electronic modulation of Cu sites. This synergistic effect not only kinetically facilitate the adsorption and activation of NO 3 − but also enhance the selectivity of key intermediate (NO 2 − ) towards NH 4 + formation. Density Functional Theory (DFT) calculations and synchrotron radiation-based XAFS measurements further reveal the presence of Co promotes the adsorption of NO 3 − (forming *NO 3 ), lowers the energy barrier for *NO 3 to *NO 2 deoxygenation and simultaneously suppresses the competing H 2 evolution reaction. Importantly, the presence of Co promotes the conduction of the electron reduction path by CuCo-C to generate NH 4 + . This work provides valuable insights for the rational design of high-performance Cu-based electrocatalysts for sustainable nitrate remediation and ammonia synthesis.
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PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
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2025
·
IF 4
Yan Sun,Tayyab Shaheen,Jiali Guo,Bingjie Shi,Miaohan Li,Xiaoyan Li,Yongqiang Li,Gunghui Tang
The cotton aphid, Aphis gossypii Glover, one of the most economically destructive pests, causes a significant threat to various crops and has evolved with varying levels of resistance to various types of chemical insecticides. Flonicamid, a novel systemic insecticide, is commonly employed to control sucking insect pests owing to its high efficacy and relatively non-hazardous nature. In this study, the A. gossypii population (F 40 ) exhibited a resistance ratio of 19.68 to flonicamid, with a realized heritability ( h 2 ) of 0.09. F 40 displayed a negative cross-resistance (CR) between flonicamid and several insecticides, such as pirimicarb, acetamiprid and thiamethoxam, while demonstrating minimal CR with lambda-cyhalothrin and bifenthrin. Analysis of the fitness characteristics indicates that the F 40 exhibits a relatively lower fitness of 0.83 and a reduced net reproductive rate when compared to the F 0 strain. The enzyme activity assays suggest that the F 40 strain has a significant increase in activities of cytochrome P450 monooxygenase (P450s) and UDP-glycosyltransferases (UGTs). Furthermore, the F 40 strain exhibits a higher nicotinamidase (NAMase) enzymes activity (1.48-fold) and a significant upregulation of the nicotinamidase gene ( Naam ) expression (2.92-fold) compared to the F 0 strain. Taken together, our results suggest that A. gossypii shows a low propensity for developing resistance to flonicamid and little cross-resistance to typical insecticides. The sustained efficacy of this insecticide could be achieved through strategic rotation or temporary cessation of its use in conjunction with other insecticides. The enhanced activity of P450s, UGTs and NAMase in the F 40 strain may co-contribute to the flonicamid resistance in A. gossypii .
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JOURNAL OF SEPARATION SCIENCE
·
2019
·Vol. 42
·期 7
·1332-1340
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IF 2.516
Yan Wang,Shujuan Ma,Luwei Zhang,Na Zhang,Yanan Li,Junjie Ou,Yehua Shen,Mingliang Ye
Three monomers, octakis (3-mercaptopropyl) octasilsesquioxane, 1,2,4-trivinylcyclohexane and isophytol were employed to synthesize a novel monolithic stationary phase via photo-initiated thiol-ene click polymerization for reversed-phase liquid chromatography. Several factors such as porogenic system, reaction time and the molar ratio of functional groups were investigated in detail. The resulting poly(POSS- co -TVCH- co -isophytol) monolithic column exhibited suitable permeability for fast separation and outstanding thermal stability. Five alkylbenzenes were employed to evaluate the ability of chromatographic separation of the resulting monolithic columns at different flow rates, and showed the highest column efficiencies of 90,200–93,100 N/m (corresponding to 10.4–10.6 μm of plate height) at a velocity of 0.41 mm/s. The baseline separations of five anilines and eight phenols further proved the applicability of poly(POSS- co -TVCH- co -isophytol) monolithic column in the separation of small molecules.
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