CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Qilin Xu,Huachun Fan,Hongmiao Yao,Duoheng Wang,Hangwei Yu,Bingbing Chen,Zhiqun Yu,Weike Su
Monoacylated symmetrical diamines are building blocks or intermediates of several well-established drugs. However, for the symmetrical diamines, the two amine groups located in a similar chemical environment make the selective monoacylation rather difficult and no kinetics study has ever been reported before. To comprehend this kind of reaction more deeply, a continuous flow microfluidic system was developed to evaluate the reaction kinetics of m -phenylenediamine and benzoic anhydride. At first, the reaction order of each reactant, pre-exponential factors and activation energies were determined in turn. The possible reaction mechanism was postulated from the reaction order. Then, a series of validation experiments were designed to show the accuracy and the applied range (concentration and temperature) of the kinetic model. Next, to obtain a controlled selectivity, the effects of initial concentration, reaction temperature and molar ratio on the selectivity were investigated through the model simulation. In the end, under the conditions optimized by the kinetic model, 96.9% selectivity and 92.5% yield were obtained in the microreactor.
研究领域:
有机化学
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药物化学
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化学工程
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高影响因子
Chemical Science
·
2024
·Vol. 15
·期 28
·10882-10891
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IF 7.6
Lizhen Zhong,Xuefeng Feng,Qingyun Zhang,Xianqing Xie,Feng Luo
Uranium extraction from seawater represents an effective way to solve the difficulty of the insufficient uranium supply chain. However, this route is still restricted by the low extraction efficiency of reported adsorbents. Here, we find that reversing the donor–acceptor in imidazole-based COFs (covalent-organic frameworks) would be effective for enhancing the extraction efficiency of uranium. As a result, the TI-COF is found to enable a uranium extraction efficiency up to 8.8 mg g−1 day−1 from seawater under visible light irradiation, exceeding all established adsorbents for such use, and an unprecedented uranium extraction efficiency up to 6.9 mg g−1 day−1 from seawater under natural sunlight.
研究领域:
材料科学
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环境科学
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能源研究
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2025
·
IF 2.5
Shuanglong Lu,Kunpeng Zhang,Yu Wu,Fang Duan,Mingliang Du
The indiscriminate use of organic dyes without adequate wastewater treatment can result in severe water pollution and pose significant threats to biological health. This underscores the urgent need for the development of advanced materials capable of selectively removing contaminant organic dyes from water systems. In this study, highly crystalline covalent organic framework (COF) materials with pyridine structures were synthesized via a molten polymerization method, employing a Knoevenagel condensation reaction between 2,4,6-trimethylpyridine and 1,4-phthalaldehyde. Following modification with hydrochloric acid, cationic COF materials (S-iCOF) were obtained. These positively charged COF exhibited excellent crystallinity and a high specific surface area of up to 354.1 m2 g−1. They demonstrated exceptional efficiency in adsorbing anionic dyes, with maximum adsorption capacities of 481.7 mg g−1 for methyl orange (MO) and 460.4 mg g−1 for orange II (O II). The adsorption behavior adhered to a pseudo-second-order kinetic model. Furthermore, due to the difference in charge, S-iCOF exhibited significantly lower adsorption capacities for cationic dyes such as methylene blue (MB) and crystal violet (CV), enabling its use as a selective adsorbent for separating dyes with different ionic properties. By changing the 1,4-phthalaldehyde to 4,4′-biphenyldicarbaldehyde, the pore size of the COFs could be precisely expanded. It was demonstrated that large-pore cationic COFs (L-iCOF) are more advantageous for the removal of medium- to large-sized dyes. The molten polymerization method used for the synthesis of iCOF is both cost-effective and efficient. This study highlights the immense potential of cationic COFs for removing and separating organic dye pollutants from wastewater, offering promising applications in the remediation of organic contamination.
研究领域:
环境科学
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材料科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Yonghao Zhu,Xia Zhao,Xiaoping Guo,Donald Terry Greenfield,Jizhou Duan,Shan Lin,Baorong Hou
A Covalent Organic Frameworks with superhydrophobic nanofluidic channels was assembled. • The coating synergistically combined self-healing corrosion protection and anti-icing abilities. • The anti-corrosion performance was verified through localized electrochemical testing. • The mechanism of anti-icing performance was simulated by Finite Element Analysis. Covalent organic frameworks (COFs) with nanofluidic channels have shown great potential in self-healing anticorrosion coatings for metals. In this paper, a strategy was reported to fabricate a superhydrophobic nanofluidic-channel coating (SCOF coating) that concurrently delivered anti-icing, and self-healing protection. The specific surface area of the produced COF reaches 1714.1 m 2 ·g −1 , which can achieve a BTA loading of 31% and increase the photothermal efficiency to 39.21%.The SCOF coating achieved a superhydrophobic contact angle of 154° and maintained this non-wetting behavior even after enduring 800 abrasion cycles under a 100 g load, 300 consecutive tape peeling cycles, and 30 min of high-impact water jet impingement. Electrochemical evaluations revealed that the intact coating provided an exceptional initial |Z| 0.01 Hz of 3.7 × 10 10 Ω·cm 2 . Upon localized damage, the pH-responsive controller releases corrosion inhibitor and restores the barrier. Furthermore, the robust Cassie structure and photothermal conversion synergistically reduced the ice adhesion strength to 18 kPa, extended the freezing delay time by 340%, and enabled complete ice melting within 383 s. This facile yet efficient strategy opened new avenues for practical coatings in cold environments. Download: Download high-res image (166KB) Download: Download full-size image
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高影响因子
Catalysts
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2025
·Vol. 15
·期 5
·459
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IF 4
Dan Wang,Yanan Liu,Kun Wan,Danning Feng,Yan Pei,Minghua Qiao,Xiaoxin Zhang,Baoning Zong
The electrocatalytic reduction of O2via two-electron reaction (2e-ORR) to H2O2represents a promising alternative to the current anthraquinone process, since it is advantageous in the sustainable and decentralized production of H2O2. Herein, we report the development of oxygen and nitrogen-rich few-layered graphene-like materials (ms-dcda) by the one-step carbonization of biomass-sourced monosaccharides (D-glucose, D-fructose, D-galactose, D-ribose, D-xylose, L-arabinose, and D-mannose) with the aid of dicyandiamide for electrochemical O2reduction to H2O2. The ms-dcdamaterials were porous and possessed wrinkled morphology typical of graphene nanosheets. In H2O2production via 2e-ORR in an acidic electrolyte, these ms-dcdamaterials were all active and stable catalysts, among which glu-dcdaderived from D-glucose and dicyandiamide displayed the lowest onset potential of 0.553 V and the highest selectivity of up to 91.6%. The catalyst was also highly stable in chronoamperometric tests. Selective chemical titration of the C–OH and C=O groups revealed that the latter is far more active and selective than the former in 2e-ORR. Moreover, a positive correlation between the contents of C=O and pyrrolic N and the H2O2partial current suggests that the pyrrolic N group also contributes to 2e-ORR. This work affords a facile strategy for the sustainable fabrication of metal-free carbon-based catalysts efficient for H2O2electrosynthesis.
研究领域:
材料科学
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电化学
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催化
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高影响因子
Journal of Energy Chemistry
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2025
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IF 14.9
Jinli Liu,Mo Zhang,Ling Tang,Simin Zhang,Jiayong Lu,Xu Yang,Yangming Lin
Hydrogen peroxide (H 2 O 2 ) is an important chemical that can be sustainably produced through a two-electron pathway in the electrocatalytic oxygen reduction reaction (ORR). However, the high cost and low reaction efficiency of catalysts currently limit the widespread application of this technology. Developing high-selectivity and scalable catalysts and accurately identifying the reaction active sites remain challenges. In this work, we have developed a promising nanodiamond (ND) catalyst to achieve high-selectivity H 2 O 2 production by oxygen reduction. Through surface carbon hybridization regulation to identify specific oxygen-containing functional groups combined with titration, model catalysis and DFT methods, it is found that the presence of carbonyl groups inducing the surrounding carbon atoms exhibit an optimal *OOH adsorption strength, thus promoting the two-electron pathway in ORR. Specifically, dynamic evolution processes of carbonyl groups and key adsorbed intermediate products including O 2 (ads), superoxide anion *O 2 − , and *OOH are monitored in situ spectroscopy. In the flow-cell device, ND catalyst realizes the high H 2 O 2 Faradaic efficiency around 92% with a rate activity up to 105 mol g C=O −1 h −1 , surpassing among reported non-metallic catalysts. The total H 2 O 2 yield reaches to 23.79 mM after a ten-hour test, which is 2.56 times higher than that of carbonyl-passivated ND, demonstrating its potential in scale-up application. Both titration and model catalytic processes proposed in this study further offer methods of designing efficient electrocatalysts for H 2 O 2 production.
研究领域:
材料科学
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电化学
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催化科学
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高影响因子
ENVIRONMENT INTERNATIONAL
·
2025
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IF 9.7
Jiaqi Shi,Yan Li,Qi Wei,Xin Zhu,Shaohua Cao,Wenyi Xie,Yang Guo,Jing Wei,Zekai Li,Tao Long
The widely used rubber antioxidant N-(1,3-Dimethylbutyl)-N’-phenyl-p-phenylenediamine (6PPD) and its ozonated product, 6PPD-quinone (6PPD-Q), are highly toxic to aquatic life, yet understanding on their environmental behaviors is limited. This study comprehensively investigated their adsorption and transformation processes on natural Fe-Mn nodules (NFMN), which commonly exist in sediments and soils through a combination of diverse experimental and computational methods. The maximum adsorption capacity of 6PPD-Q (719.2 μg·g −1 ) is significantly higher than that of 6PPD (133.8 μg·g −1 ) at 293 K, and it is more difficult to desorb. They follow different kinetic and isothermal adsorption models, and environmental conditions (including temperature, pH, and anions) exert distinct influences on the adsorption of the two substances. Adsorption mechanisms involving electrostatic attraction, charge transfer, hydrogen bonding, and Lewis acid-base complexation were unveiled. For 6PPD, electrostatic adsorption and Lewis acid-base complexation contribute significantly to its adsorption. Conversely, for 6PPD-Q, the contribution of Lewis acid-base complexation outweighs that of hydrogen bonding, while the effect of electrostatic adsorption is relatively negligible. The stronger electrostatic attraction, more efficient charge transfer, and a greater number of binding sites for hydrogen bonding and Lewis acid-base complexation with NFMN results in more robust adsorption of 6PPD-Q. Furthermore, 6PPD can transform into 6PPD-Q on NFMN, facilitated by dissolved Mn(III). This study advances understanding of the adsorption behavior and mechanism of 6PPD and 6PPD-Q, and highlights a new pathway for 6PPD-Q formation, which provides valuable reference for assessing the water body exposure risks and formulating environmental remediation strategies for such pollutants. Environmental Implication This study offers the first comprehensive insight into the interactions between 6PPD/6PPD-Q and NFMN, illuminating their environmental behavior in water and soil systems. It reveals the adsorption discrepancy between 6PPD and 6PPD-Q, and elucidates the mechanisms underlying the difference in adsorption. Additionally, it uncovers a novel pathway for 6PPD-Q formation, offering valuable implications for risk assessment and environmental remediation strategies.
研究领域:
环境科学
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化学
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PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Jing Hu,Penghui Zhang,Pengfei Wang,Lingxiao Zhang,Xiwang Zhang
Membranes capable of efficient ion transport are highly demanded for separation and energy conversion and storage, such as flow batteries and fuel cells. Beyond the primary benefits of high ion selectivity and conductivity, the ideal membrane must also exhibit robust chemical and physical stability for industrial applications. Herein, we develop a composite membrane (COFs-M) incorporating designed olefin-linked ultramicroporous COF nanosheets (pore size 0.6 nm) with selective ion transport ability and outstanding chemical stability under highly alkaline conditions (6 M NaOH). The COFs-M membrane demonstrates exceptional hydroxide ion transport efficiency, achieving an area resistance of 0.82 Ω cm 2 and facilitating the operation of an alkaline zinc-based flow battery at a remarkable current density of 320 mA cm −2 , achieving a voltage efficiency of 81.56 %. Additionally, the membrane allows the battery to maintain long-cycle stability over 350 cycles with a dendrite-free zinc morphology at a current density of 200 mA cm −2 .
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高影响因子
ANALYTICAL CHEMISTRY
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2025
·
IF 6.7
Jingtao Huang,Ying Ying Nie,Yu Meng Yang,Xin Ying Long,Yongpeng He,Lei Zhan,Cheng Zhi Huang
Acetylcholinesterase (AChE), one of nature’s most efficient enzymes, plays a crucial role in neural signal transduction and the restoration of tissue homeostasis with implications in the development of neurodegenerative diseases. Conventional methods for detecting AChE mainly rely on its catalytic activity. Herein, we present an approach for AChE detection based on its chiral binding with photoluminescent carbon dots (CDs) with rich chiral cysteine residues (L/D-CDs), synthesized via a general hydrothermal route. Interestingly, L-CDs, despite being synthesized under the same conditions as D-CDs, exhibited a stronger specific binding affinity for AChE than D-CDs through electrostatic interactions, attributed to the amphiphilic nature of AChE, leading to enhanced photoluminescence near the isoelectric point of AChE at 6.50. The enhanced photoluminescence intensity of L-CDs showed a linear correlation with AChE concentrations over the range of 200–4500 mU/mL with a detection limit of 20 mU/mL. Meanwhile, by leveraging the selective recognition of AChE by L-CDs, we applied the probe to distinguish between liver cancer tissues and adjacent nontumor tissues. The results demonstrated that, due to the reduced AChE content in liver cancer tissues, the fluorescence intensity was significantly lower than that in adjacent nontumor tissues. Our findings highlight the potential of CDs rich in chiral residuals as optical probes for biosensing and imaging applications based on biomolecular recognition.
研究领域:
分析化学
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生物化学
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纳米技术
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生物医学工程
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分子生物学
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PubMed
高影响因子
Journal of Water Process Engineering
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2026
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IF 6.7
Tianyuan Xu,Nanxi Zhu,Ruina Yuan,Yaowen Xing,Xiahui Gui
Carbon-driven persulfate (PS) activation is promising for antibiotic degradation, but conventional carbon catalysts often require thermal/acid-base modification or metal doping, suffering from low yields and high costs. Herein, we innovatively employed unmodified low-rank coals from Shengdong (LC SD ) and Sujiagou (LC SJG ) as cost-effective PS activators for sulfamethazine (SMZ) degradation. Characterizations including Raman, 13 C nuclear magnetic resonance, and electron paramagnetic resonance (EPR) revealed distinct structural-chemical features. LC SJG had more structural defects, –OH, and –COOH groups, while LC SD showed higher persistent free radical and C O group concentrations. LC SJG exhibited superior performance (99.3 % SMZ removal in 120 min) versus LC SD (84.2 %) and good tolerance to coexisting ions, indicating practical application potential. Possible degradation pathways of SMZ, as revealed by high-performance liquid chromatography-mass spectrometry, were proposed involving sulfonamide cleavage and pyrimidine ring opening. Mechanistic investigations via EPR, radical quenching, and electrochemical analysis revealed that 1 O 2 dominated SMZ degradation (59.3 %) in the LC SD /PS system via C O groups. Conversely, • OH and SO 4 •− contributed 62.7 % to degradation in the LC SJG /PS system through structural defects and –COOH groups. Overall, this study provides a novel strategy for developing low-cost, high-performance PS activators tailored for wastewater treatment.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Xiaoxia Zhang,Qinming Zhang,Xiaoqing Zhang,Jiwei Shen,Yinmao Wei,Chaozhan Wang
Per -and polyfluoroalkyl substances (PFASs) have become a pressing global concern for environmental and public health due to their extreme persistence and association with severe adverse effects, underscoring the urgent need for efficient and sustainable remediation technologies. In this study, we present a cost-effective, one-pot melt polymerization approach for the synthesis of an ionic covalent organic framework (COF) adsorbent, TMB-TPA-COF(Br − ), using 2,4,6-trimethylpyridine (TMB) and terephthalaldehyde (TPA) as inexpensive molecular building blocks. The material is subsequently functionalized via in-situ quaternization with bromoethane to introduce cationic sites that enable strong electrostatic interactions for selective PFAS capture. The resulting TMB-TPA-COF(Br − ) exhibits well performance in the removal of perfluorooctanoic acid (PFOA), achieving a maximum adsorption capacity of 411.5 mg/g and reaching adsorption equilibrium within 30 min. It maintains high removal efficiency for five perfluoroalkyl carboxylic acids (PFCAs) over a broad pH range (2–5), and the presence of humic acid induces only a marginal decrease (<10 %) in PFOA uptake, demonstrating remarkable resilience in complex environmental matrices. Notably, TMB-TPA-COF(Br − ) surpasses commercial activated carbon and conventional anion exchange resins in the simultaneous removal of 14 structurally diverse PFASs, achieving ≥75 % removal for 13 compounds, with the exception of perfluorobutanoic acid (PFBA). Moreover, the adsorbent exhibits excellent chemical stability, retaining over 88 % of its initial removal efficiency after five regeneration cycles, and consistently maintains high performance across seven real-world water samples, including groundwater, wastewater, and surface water, where it achieves >75 % removal of PFCAs. This study highlights the potential of TMB-TPA-COF(Br − ) as a high-performance and cost-effective adsorbent for PFASs remediation, offering a scalable and practical solution to address widespread PFASs contamination.
研究领域:
环境科学
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材料化学
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水处理技术
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吸附
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高分子化学
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高影响因子
ChemSusChem
·
2021
·Vol. 14
·期 9
·2067-2075
·
IF 8.928
Sen Jiang,Haihua Wu,Junying Yin,Zhihua Wei,Jiahao Wu,Lai Wei,Dunfeng Gao,Xin Xu,Yunfang Gao
Graphical Enhanced electrolyte : Ultralow-cost benzoic anhydride (BA), as a promising bifunctional electrolyte additive to capture hydrogen fluoride and H 2 O as well as to construct a robust cathode-electrolyte interface on the LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811) cathode surface, effectively improves the cycling performance and rate capability of high-voltage Li-ion batteries with LiPF 6 -based electrolyte. High-voltage LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)-based Li-ion batteries (LIBs) with enhanced performance can be achieved by properly tailoring the electrolyte systems. Benzoic anhydride (BA) was proposed here as a promising bifunctional electrolyte additive that can not only construct a robust cathode-electrolyte interface (CEI) film on the electrode surface but also capture HF/H 2 O in the electrolyte effectively. Compared to the cell without the BA additive, the capacity of Li/NCM811 half-cell with 1.0 wt % BA was increased from 128.5 to 149.6 mAh g −1 after 200 cycles at 1 C between 3.0 and 4.3 V. Even at a higher cut-off voltage of 4.5 V, the BA-containing Li/NCM811 half-cell delivered a capacity retention of 69 % after 200 cycles, much higher than that of the half-cell without the additive (56 %). Both theoretical calculation and experimental results verified that the BA additive could be preferentially oxidized to form a stable interface film with high conductivity that protected the NCM811 cathode and suppressed the decomposition of the electrolyte.
研究领域:
材料科学
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电化学
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PubMed
高影响因子
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