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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Generation of dichloroacetonitrile with the co-presence of g-C3N4 and chloride in peroxymonosulfate/Vis system: Impacts and mechanism

Zhiwei Zhao,Yu Li,Fei Wang,Zhitao Xu,Sai Zhang,Li Li,Junyu Fan,Jie Liu

Monitoring and regulating the formation of toxic byproducts in advanced oxidation processes (AOPs) is of great significance for their practical application in water treatment. In this work, we found that dichloroacetonitrile (DCAN), a common N-containing byproduct in chloramination disinfection, can be formed with the co-presence of g-C 3 N 4 and chloride in a peroxymonosulfate (PMS) system. The measured value was 12.01 μM within 12 h under the given conditions. Structure analysis of raw and used g-C 3 N 4 demonstrated that g-C 3 N 4 decomposition indeed occurred, and C = N bonds acted as primary active sites, releasing N resources for subsequent DCAN formation. Additionally, multiple parameters, including the reactant (i.e., g-C 3 N 4 , PMS, Cl - , phenol) dose and solution pH, were observed to remarkably affect the yield of DCAN. Phenol was identified as the organic precursor of DCAN and may cooperate with inorganic chloramine to promote DCAN formation via the decarboxylation pathway. This study highlights the generation of DCAN in N-involved catalyst-based AOPs and improves understanding of the DCAN formation mechanism.

研究领域: 环境科学 · 化学工程
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY · 2024 · IF 6.2

Insight into the role of stress response and toxic mechanism induced by Chloro-haloacetonitrile in vitro

Dong Li,Wen Cheng,Xiaoping Zhou,Xing Zheng,Jiehui Ren,Ting Meng

Chloro-haloacetonitrile (Cl-HAN), belongs to a group of nitrogenous disinfection by-products (N-DBPs) found in surface water, and are known to pose a major risk to the safety of human drinking water. However, the exact biological toxicity mechanism and the extent of the stress response caused by Cl-HAN remain unclear, resulting in a lack of effective measures to control its presence. Thus, the quantitative toxicological genomics and bioinformatics methods were applied to explore the effects of three chloro-haloacetonitriles (Cl-HANs) on the transcription of fusion genes under varying concentrations of stress in E. coli over 2-hour period. The initial stress response and their toxic mechanism were analyzed. The study also identified the molecular toxicity endpoint, and the core genes that are responsible for the specific toxicity of different Cl-HANs. Cl-HANs exhibited concentration-dependent characteristics of toxic effects, and caused changes in gene expression related oxidative and membrane stress. The stress response results showed that dichloroacetonitrile (dCAN) still caused significant DNA damage under the lowest concentration stress. Chloroacetonitrile (CAN) and trichloroacetonitrile (tCAN) exhibited lower genetic toxicity levels at 513 μg/L and 10.7 μg/L, respectively. The toxic effects of tCAN were widespread. And there was a good correlation between the molecular endpoint (EC-TELI 1.5 ) and the phenotypic endpoint (LD50) with r p =-0.8634 ( P =0.0593). In all concentrations of stress in CAN, dCAN, and tCAN, the number of overexpressed genes shared was 15, 2, and 14, respectively. Furthermore, bioinformatics analysis demonstrated that Cl-HANs affected genes associated with general stress pathways, such as cell biochemistry and physical homeostasis, resulting in changes in biological processes. And for CAN-induced DNA damage, polA played a dominant role, while katG , oxyR , and ahpC were the core genes involved in oxidative stress induced by dCAN and tCAN, respectively. These findings provide valuable data for the toxic effect of Cl-HANs.

CAS / MDL: 3018-12-0
研究领域: 环境科学 · 分子生物学 · 毒理学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2020 · IF 5.774

Fate of typical organic halogen compounds during electrodialysis process and improvement of their recoveries

Jie Yang,Yulin Zhang,Yinan Bu,Baiyang Chen,Juan Li

According to an earlier study, electrodialysis (ED) can efficiently separate most organic halogenated micropollutants from inorganic halogens (i.e., halides and oxyhalides) in water, with only a few micropollutants being poorly-recovered. To optimize the ED process and to gain in-depth knowledge of the mechanisms responsible for their low recoveries, this study designed some experiments to examine the fates and transports of three hard-to-separate organic halogen compounds. Results show that the dominant mechanism responsible for the loss of trichlorophenol (TCP) is migration and retention in the ion exchange membrane (IEM), the dominant mechanism for the loss of trichloroacetic acid (TCAA) is ion exchange with the IEM, and the dominant mechanism for the loss of trichloroacetonitrile (TCAN) is volatilization and chemical decomposition during the ED process. Optimizing specific operating conditions (e.g., sealing, voltage, and membrane type, etc.) can improve recovery of these micropollutants to 70.4–95.8% while maintaining 90.4–99.5% removal of chloride. Even though TCAN underwent hydrolysis, we recovered 82.0% chlorine from TCAN and its hydrolytic products. These results may help not only better understand the fates and transports of organic micropollutants during the ED process, but also help facilitate application of electrodialysis technique for measuring total organic halogen.

研究领域: 环境科学 · 水处理技术
✓ 已验证 DOI 高影响因子
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Journal of Energy Chemistry · 2024 · IF 14

Regulating the non-effective carriers transport for high-performance lithium metal batteries

Simeng Wang,Youchun Yu,Shaotong Fu,Hongtao Li,Jiajia Huang

The absence of control over carriers transport during electrochemical cycling, accompanied by the deterioration of the solid electrolyte interphase (SEI) and the growth of lithium dendrites, has hindered the development of lithium metal batteries. Herein, a separator complexion consisting of polyacrylonitrile (PAN) nanofiber and MIL-101(Cr) particles prepared by electrospinning is proposed to bind the anions from the electrolyte utilizing abundant effective open metal sites in the MIL-101(Cr) particles to modulate the transport of non-effective carriers. The binding effect of the PANM separator promotes uniform lithium metal deposition and enhances the stability of the SEI layer and long cycling stability of ultra-high nickel layered oxide cathodes. Taking PANM as the Li || NCM96 separator enables high-voltage cycling stability, maintaining 72% capacity retention after 800 cycles at a charging and discharging rate of 0.2 C at a cut-off voltage of 4.5 V and 0 °C. Meanwhile, the excellent high-rate performance delivers a specific capacity of 156.3 mA h g −1 at 10 C. In addition, outstanding cycling performance is realized from −20 to 60 °C. The separator engineering facilitates the electrochemical performance of lithium metal batteries and enlightens a facile and promising strategy to develop fast charge/discharge over a wide range of temperatures.

研究领域: 材料科学 · 电化学 · 能源存储
✓ 已验证 DOI 高影响因子
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HIGH PERFORMANCE POLYMERS · 2024 · IF 1.8

Preparation of phthalonitrile resin/calcium sulfate whisker composites with enhanced wear and heat resistance

Dengke Li,Han Zhao,Zhiyi Jia,Dianqiu Jia,Jianxin Rong,Huaijie Yan,Xiaoyan Yu,Qingxin Zhang

Composites based on high-performance resin matrix have excellent high temperature resistance, chemical stability, and excellent processability, and exhibit a wide range of applications in many fields. At present, there are no reports on the application of calcium sulfate whiskers (CSW) in phthalonitrile resins. In this study, KH560 was used to modify CSW, through FT-IR, TGA, XRD and XPS methods, KH560 was successfully grafted onto CSW, and the modified CSW was filled with phthalonitrile resin containing fluorine elements. SEM shows that the modified CSW is uniformly dispersed in the resin. The storage modulus of composites increased from 2.6 GPa to 3.8 GPa. Under air and nitrogen atmospheres, the T5% of the composites increased by about 10°C. When the addition amount of CSW is 10%, the friction coefficient of the material is reduced from 0.68 to 0.58, the depth of wear marks decreased from 49.1 μm to 27.9 μm, the wear rate of AFPN-10 (the addition amount of CSW is 10%) decreases from 3.59 × 10−4 mm3/(N·m) to 2.70 × 10−4 mm3/(N·m), the wear resistance performance was significantly improved. With the increase of CSW in composites, the hardness, reduced modulus and elastic recovery rate are also gradually increasing, the highest reduced modulus and hardness are 2434 MPa and 597 MPa respectively. The addition of CSW can improve the mechanical properties and thermal properties of the phthalonitrile resin, as well as enhance its anti-friction ability. Phthalonitrile resin-based composites have potential application values in the fields of aerospace, electronic instruments and lightweight components.

研究领域: 材料科学 · 航空航天 · 化学工程
✓ 已验证 DOI 高影响因子
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2021 ·Vol. 168 ·期 6 ·066514 · IF 4.316

High Electrosorption Capacity of Uranium (VI) by Carboxylic Acid Functionaliszed N, P Co-Doped Carbon Materials

Xiaopeng Liu,Yan Liu,Yun Wang,Dingzhong Yuan,Jinbiao Liu,zuqing Zhu

Polyphosphazene, as a precursor, was synthesized by ultrasonication using 4,4-diaminodiphenyl ether and hexachlorocyclotriphosphazene (HCCP). It was carbonized and functionalized at high temperature to obtain carboxylic acid functionalized N, P co-doped carbon materials (denoted as NPCs-COOH). The structure of NPCs-COOH was characterized by Fourier Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffractometry (XRD), Raman spectrometry (Raman), Thermogravimetric analysis (TG) and N2 adsorption-desorption isotherm (BET). The electrosorption properties were explored under different pH values, applied potentials, initial concentrations and contact time. The optimal pH for electrosorption was 5.0 while the equilibrium time was 30 min. The maximum electrosorption capacity from the experiments towards U(VI) was about 551.46 mg g−1 under the most suitable applied potential of 0.9 V, which was much higher than other carbon materials. Meanwhile, it also showed excellent recyclability with a 23.3% reduction of electrosorption capacity after six cycles. A plausible mechanism of electrosorption was presented using XPS analysis. The results showed the N, P co-doped NPCs-COOH can be used in the electrosorption field to remove U(VI) effectively in solution.

研究领域: 材料科学 · 环境科学
✓ 已验证 DOI 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2016 · IF 5.31

Comparison of THMs and HANs formation potential from the chlorination of free and combined histidine and glycine

Changjun Li,Naiyun Gao,Wenhai Chu,Tom Bond,Xingya Wei

Trihalomethane (THMs) and haloacetonitriles (HANs) are typical and frequently detected carbonaceous (C–) and nitrogenous (N–) disinfection by-products (DBPs) in water treatment , and amine acids (AAs) are important precursors of DBPs. However, previous researches mainly focused on free AAs and few investigations evaluated the DBPs formation potential of combined AAs, especially combined histidine . The formation of THMs and HANs from free and combined histidine and glycine during chlorination was firstly examined and compared in this study with an emphasis on their differences. The impacts of chlorine dose, pH, ammonia nitrogen and bromide were evaluated and mechanistic formation pathways were proposed. In comparison with free AAs, combined AAs generated more chloroform (CF, 125%–671%) but less dichloroacetonitrile (DCAN, 4.66%–87.5%) at all chlorine doses. The effect of solution pH on combined AAs was slighter than that on free AAs. During chloramination, both free AAs and combined AAs generated much smaller amounts of DBPs, especially DCAN (<9.01%), compared with chlorination. At any bromide dose, there was more bromine merging into THMs than DHANs, especially for combined AAs. At the beginning of chlorination, the combined AAs decomposed in three different ways: hydrolysis, decarboxylation and scission , leading to differing amounts of CF and DCAN compared with the free AAs.

研究领域: 环境科学 · 水处理工程 · 化学
✓ 已验证 DOI 高影响因子
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ELECTROCHIMICA ACTA · 2016 · IF 4.803

Electrochemical effect and mechanism of adiponitrile additive for high-voltage electrolyte

Shiyou Li,Dongni Zhao,Peng Wang,Xiaoling Cui,Fengjuan Tang

To satisfy the need of 5   V high-voltage cathode materials, lithium difluoro(oxalato)borate (LiDFOB) with excellent film-forming property has been chosen as lithium salt , and adiponitrile (ADN) with stable electrochemical performance has been evaluated as functional additive. An electrochemical investigation of this novel electrolyte solution shows a wide electrochemical oxidation window of nearly 6.0   V vs Li + /Li. Due to the positive effect of ADN on the cathode/electrolyte interface, LiNi 0.5 Mn 1.5 O 4 /Li half-cell with ADN-adding electrolyte exhibits prominent rate capability and cyclability. It is believed that the improvement of electrochemical performances has benefitted greatly from interfacial impedance reducing. Two modeling hypotheses have been used to explain interfacial interaction between ADN and LiNi 0.5 Mn 1.5 O 4 , by the means of analysis of X-ray photoelectron spectroscopy and theoretical calculation. Results show that ADN can enrich the surface of cathode material to hinder the further decomposition of the electrolyte, and contribute to the formation of a cathode-electrolyte interface passivation film with protective and conductive properties.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY · 2012 ·Vol. 51 ·期 2 ·340-346 · IF 3.919

Living radical polymerization of acrylonitrile catalyzed by copper with a high concentration of radical initiator and its application in removal of Ag(I) after modification

Delong Liu,Hou Chen,Naiyi Ji,Zhi Tan

In this study, we reported the synthesis of polyacrylonitrile (PAN) via living radical polymerization in N, N -dimethylformamide using carbon tetrachloride as initiator, copper(II) chloride (CuCl 2 )/hexamethylenetetramine as catalyst system, and 2,2-azobisisobutyronitrile as a high concentration of thermal radical initiator. The polymerization proceeded in controlled/living manner as indicated by first-order kinetics of the polymerization with respect to the monomer concentration, linear increase of the molecular weight with monomer conversion and narrow polydispersity. Higher polymerization rate and narrower molecular weight distributions were observed with CuCl 2 less than 50 ppm. The rate of polymerization showed a trend of increase along with temperature. The modified PAN containing amidoxime group was used for extraction of Ag(I) ions from aqueous solutions. The adsorption kinetics data indicated that the adsorption process followed pseudo-second-order rate model. The isotherm adsorption process could be described by the Freundlich isotherm model. © 2012 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2013

CAS / MDL: 100-97-0
研究领域: 高分子化学 · 环境科学
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Membranes · 2024 ·Vol. 14 ·期 5 ·97 · IF 3.3

Enrichment of Nutmeg Essential Oil from Oil-in-Water Emulsions with PAN-Based Membranes

Huilan Yin,Haoyu Zhang,Jiaoyang Cui,Qianlian Wu,Linlin Huang,Jiaoyue Qiu,Xin Zhang,Yanyu Xiang,Bo Li,Hongbo Liu,Zhishu Tang,Yue Zhang,Huaxu Zhu

This study used polyacrylonitrile (PAN) and heat-treated polyacrylonitrile (H-PAN) membranes to enrich nutmeg essential oils, which have more complex compositions compared with common oils. The oil rejection rate of the H-PAN membrane was higher than that of the PAN membrane for different oil concentrations of nutmeg essential oil-in-water emulsions. After heat treatment, the H-PAN membrane showed a smaller pore size, narrower pore size distribution, a rougher surface, higher hydrophilicity, and higher oleophobicity. According to the GC-MS results, the similarities of the essential oils enriched by the PAN and H-PAN membranes to those obtained by steam distillation (SD) were 0.988 and 0.990, respectively. In addition, these two membranes also exhibited higher essential oil rejection for Bupleuri Radix, Magnolia Officinalis Cortex, Caryophylli Flos, and Cinnamomi Cortex essential oil-in-water emulsions. This work could provide a reference for membrane technology for the non-destructive separation of oil with complex components from oil-in-water emulsions.

CAS / MDL: 75-11-6 141-78-6
研究领域: 食品科学 · 分离技术
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING · 2025 · IF 8.9

Enhancing the heat resistance, dielectric properties, and flame retardancy of self-curing silicon-based phthalonitrile/quartz composites for a rapid hot-melt prepreg process

Yabin Zhang,Jiaming Wang,Xuedong Wu,Linyan Zhu,Wenguang Zhang,Lishuai Zong,Jinyan Wang,Xigao Jian

The robust operation of electromagnetic waves in communication systems with extreme temperatures relies on high-temperature resistant wave-transparent composites, with organic resin matrix being a pivotal constituent. Enhancing the heat resistance of resins while maintaining excellent processability poses a significant challenge. Herein, a novel “rigid-in-flexible” self-curing silicon-based   silicon-based   phthalonitrile monomer containing phenylacetylene backbone (Si-ALK-PN) was designed. The silazane component disrupts the crystallinity in Si-ALK-PN, resulting in a characteristic of low viscosity (0.3 Pa·s) and extended processing window (>3h). After curing at 450 °C, the resin, namely Si-ALK-PN-450 °C, demonstrated exceptional thermal stability ( T 5%  = 631 °C) and thermo-oxidative stability ( T 5%  = 560 °C). Their quartz fiber-infused composites (Si-ALK-PNs/QF) were manufactured through a straightforward melt processing approach. Upon post-curing at 450 °C, Si-ALK-PN-450 °C/QF exhibited elevated glass transition temperature, flexural strength, and consistent dielectric properties across a wide temperature ranging from 25 °C to 600 °C. Especially, it exhibited excellent flame retardancy as well, stemming from release of eco-friendlyeco-friendly inert gases (NH 3 ) and the high thermal stability of N-enriched all-aromatic PN resin. The design concept of “rigid-in-flexible”, along with the multi-functional group co-curing strategy, offers a promising solution for addressing the trade-off between processing and heat resistance in resins, extending beyond PN resins.

研究领域: 材料科学 · 化学工程
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Soft Matter · 2015 ·Vol. 11 ·期 31 ·6266-6274 · IF 4.029

Self-assembly and morphological transitions of random amphiphilic poly(β-D-glucose-co-1-octyl) phosphazenes

Chen Chen,Yue-Cheng Qian,Chuan-bin Sun,Xiao-Jun Huang

The amphiphilic random copolymer poly(β-D-glucose-co-1-octyl)phosphazene (PGOP) can undergo continuous morphological transitions in DMF–water mixed solvents. In this study, the ratio of glucose moieties to octyl moieties was controlled via a two-step thiol–ene reaction. As a result, polyphosphazenes with glycosyl functionalization degrees of 58.1% (PGOP-1), 74.1% (PGOP-2) and 87.0% (PGOP-3) were obtained. These amphiphilic polyphosphazenes self-assemble in both water and water–DMF mixtures. Several self-assembled morphologies including spheres, rods and vesicles were formed though careful control of the water content (WC) in the DMF solvent as well as of the hydrophilicity or hydrophobicity of the copolymers. We also found that an increase in the hydrophobic proportion led to faster morphological transitions at a constant WC. The thermodynamics of micellization were also studied by Isothermal Titration Calorimetry (ITC), and the strong hydrophobic interactions in PGOP-1 were demonstrated by their highly exothermic nature. These self-assemblies have potential applications in biosensing, lectin adsorption and drug loading with controlled release.

研究领域: 材料科学 · 生物医学工程 · 化学
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