MICROCHEMICAL JOURNAL
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2023
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IF 4.8
Zhefei Hu,Yanhao Jiang,Panpan Cao,Yanjuan Liu,Yuefei Zhang,Wei Chen,Sheng Tang
In this work, 2-undecylimidazole (UI) and propyl methacrylate (PMA) dual-functionalized silica gel was prepared and applied as a mixed-mode chromatographic stationary phase. Successful preparation of this stationary phase (SiO 2 -UI-PMA) was proved through a range of characterization techniques. The chromatographic performance of the obtained SiO 2 -UI-PMA was investigated for the separation of environmental endocrine disruptors (phthalates, steroid hormones, bisphenols and alkylphenols), sulfonamides and food-borne stimulants in reversed-phase chromatography, as well as for the separation of inorganic anions in anion-exchange chromatography. The effect of column temperature, acetonitrile content, salt concentration and mobile phase pH on retention was studied to explore the separation mechanism, and the results indicated that this stationary phase provided multiple interactions with analytes. Compared with the commercial C18 column, the SiO 2 -UI-PMA demonstrated more preferable separation ability under the mobile phase conditions with a low content of acetonitrile, thereby acting as a good alternative candidate for the conventional reversed-phase stationary phase in chromatographic analysis. Furthermore, the SiO 2 -UI-PMA stationary phase exhibited high column efficiency (45 860 plates m −1 for progesterone) even though it was prepared from the non-serviceable silica based chromatographic packing materials.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Yu-Ning Hu,Jin-Tao Zhan,Pei-Rong Bai,Na An,Jun-Jie Tan,Yan-Zhen Wang,Quan-Fei Zhu,Yu-Qi Feng
Di(2-ethylhexyl) phthalate (DEHP), the most widely used plasticizers in the world, has been regarded as an endocrine disrupting chemical with serious adverse health outcomes. Accumulating evidence strongly suggests that the undesirable biological effects of DEHP are meditated by its metabolites rather than itself. However, the metabolic footprints of DEHP in vivo are still unclear. Here we developed a click chemistry-assisted mass spectrometry (CC-MS) strategy for in-depth profiling DEHP metabolites in rats. An alkyne-modified DEHP analogue (alkyne-DEHP) was synthesized as a tracer for in vivo tracing, and a pair of MS probes (4-azido-nphenylbenzamide, 4-ANPA, and its deuterated reagent d 5 -4-ANPA) were prepared to specifically label the alkyne-DEHP metabolites, and prominently improve their detection sensitivity and selectivity . Using the CC-MS strategy, we successfully screened 247 alkyne-DEHP metabolites from rat urine, feces, and serum, including many unrevealed metabolites, such as oxidized phthalate diester metabolites and glucuronides of phthalate monoester metabolites. The discovery of new DEHP metabolites provides additional insights for understanding the metabolism of DEHP, which may be beneficial in exploring the mechanism underlying DEHP induced-toxicity in the future.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2023
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IF 6.8
Bingru Zhang,Shaowei Wang,Yunbing Tang,Zhiyan Hu,Lei Shi,Jialin Lu,Huitao Li,Yiyan Wang,Yang Zhu,Han Lin,Ren-shan Ge
Bisphenols (BPs) as endocrine-disrupting compounds have drawn attention to their health hazards. Whether a BP interferes with glucocorticoid metabolism remains unclear. 11β-Hydroxysteroid dehydrogenase 2 (11β-HSD2) is a key glucocorticoid-metabolizing enzyme that controls fetal glucocorticoid levels across the placental barrier and mineralocorticoid receptor specificity in the kidney. In this study, 11 BPs were tested to inhibit human placental and rat renal 11β-HSD2 and were analyzed for inhibitory potency, mode action, and docking parameters. BPs had inhibitory potency against human 11β-HSD2: BPFL>BPAP>BPZ>BPB>BPC>BPAF>BPA>TDP and the IC 10 values were 0.21, 0.55, 1.04, 2.04, 2.43, 2.57, 14.43, and 22.18 μM, respectively. All BPs are mixed inhibitors except BPAP, which is a competitive inhibitor for human 11β-HSD2. Some BPs also inhibited rat renal 11β-HSD2, with BPB (IC 50 , 27.74 ± 0.95) > BPZ (42.14 ± 0.59) > BPAF (54.87 ± 1.73) > BPA (77.32 ± 1.20) > other BPs (about 100 μM). Docking analysis showed that all BPs bound to the steroid-binding site, interacting with the catalytic residue Tyr232 of both enzymes and the most potent human 11β-HSD2 inhibitor BPFL acts possibly due to its large fluorene ring that has hydrophobic interaction with residues Glu172 and Val270 and π-stacking interaction with catalytic residue Tyr232. The increase in the size of substituted alkanes and halogenated groups in the methane moiety of the bridge of BPs increases its inhibitory potency. Regressions of the lowest binding energy with inhibition constant indicated that there was an inverse regression. These results indicated that BPs significantly inhibited human and rat 11β-HSD2 activity and that there were species-dependent differences.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Xian Jiang,Bing Liu,Qinghong Zeng,Fuchao Yang,Zhiguang Guo
To alleviate the economic and environmental damage caused by industrial discharges of oily wastewater, materials applied for efficient oil/water separation are receiving significant attention from researchers and engineers. Among others, switchable wettable materials for bidirectional oil/water separation show great potential for practical applications. Inspired by mussels, we utilized a simple immersion method to construct a polydopamine (PDA) coating on a peony-like copper phosphate surface. Then, TiO2 was deposited on the PDA coating surface to build a micro–nano hierarchical structure, which was modified with octadecanethiol (ODT) to obtain a switchable wettable peony-like superhydrophobic surface. The water contact angle of the obtained superhydrophobic surface reached 153.5°, and the separation efficiency was as high as 99.84% with a flux greater than 15,100 L/(m2·h) after 10 separation cycles for a variety of heavy oil/water mixtures. Notably, the modified membranes have a unique photoresponsiveness, transforming to superhydrophilic upon ultraviolet irradiation, achieving separation efficiencies of up to 99.83% and separation fluxes greater than 32,200 L/(m2·h) after 10 separation cycles for a variety of light oil/water mixtures. More importantly, this switch behavior is reversible, and the high hydrophobicity can be restored after heating to achieve efficient separation of heavy oil/water mixtures. In addition, the prepared membranes can maintain high hydrophobicity under acid–base conditions and after 30 sandpaper abrasion cycles, and damaged membranes can be restored to superhydrophobicity after a brief modification in the ODT solution. This simple-to-prepare, easy-to-repair, robust membrane with switchable wettability shows great potential in the field of oil/water separation.
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Nano Research
·
2023
·
IF 9.9
Yang Limin,Qu Linjiao,Zhang Xiaolong,Li Mingming,Liu Zhen
Enzyme-inorganic hybrid nanoflowers (HNFs) have shown excellent sensing capabilities due to their large specific surface area as well as the simplicity and mildness of the preparation process. However, coupling HNFs to electrodes to fabricate a uniform and controllable enzymatic electrochemical sensing interface remains a challenge. Here, we proposed an aptamer-induced in-situ fabrication strategy for preparing an HNF-based electrochemical sensor with ideal performance. Central to this strategy is the introduction of acetylcholinesterase (AChE)-specific binding aptamer (Apt), which induces the in-situ growth of AChE-copper phosphate (Cu 3 (PO 4 ) 2 ) HNFs on the surface of carbon paper (CP). In addition, a dense gold nanoparticle (AuNP) layer was electrodeposited on the CP for anchoring Apt and further extending the electroactive surface area. The prepared AChE-Cu 3 (PO 4 ) 2 HNF/Apt/AuNP/CP biosensor exhibited a wide detection range from 1 to 10 7 pM for the four organophosphorus inhibitors, including isocarbophos, dichlorvos, methamidophos, and parathion, with detection limits down to 0.016, 0.028, 0.071, and 0.113 pM, respectively. With the reactivation of pralidoxime chloride, the electrode can still recover 98.1% of the response after five times of repeated use. In real sample detection, the biosensor achieved high recoveries from 96.45% to 100.13%. The detection target may be extendable to other AChE inhibitors (e.g., drugs for Alzheimer’s disease). This study demonstrates for the first time the feasibility of using aptamers as an inducer to fabricate an electrochemical enzyme sensing interface in-situ . This strategy can be used to fabricate other enzyme-based biosensors and therefore has broader applications.
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FUEL
·
2023
·
IF 7.4
Qihuang Huo,Yahui Wang,Huijun Chen,Yu Feng,Lina Han,Weiren Bao,Liping Chang,Jiancheng Wang,Kechang Xie
It is a win–win strategy to prepare mercury sorbents from low-cost high-sulfur raw materials. In part 1, mercury sorbents with excellent performance were prepared from high inorganic sulfur coal through KOH activation. However, this method does not work for high organic sulfur coal. In this work, a two-step preparation method is developed to prepare mercury sorbents from high organic sulfur coal. The first step is the co-pyrolysis/carbonization of Fe 2 O 3 and coal, during which organic sulfur in coal is converted into FeS x . XPS shows that the percentage of S x 2– /S on the surface of the carbonized samples gradually increases from 5.4% to 22.2% with the m(Fe):m(S o ) ratio from 0:4 to 5:4. The second step is KOH activation, and it converts FeS x into various S species, including C-S, S 0 , S 2 2− and S 2− . Among the prepared mercury sorbents, LF+3Fe/4S-A (m(Fe):m(S o ) = 3:4) shows the best mercury removal performance, and its mercury removal efficiency remains above 84% for 120 min under N 2 +O 2 at 120 °C. The Hg-TPDD and XPS results indicate that S*, including C-S, S 0 and S 2 2− , are the major active sites for mercury removal rather than Fe element, and HgS is the main existing form of mercury on the used sorbents. Besides LF coal, this two-step process is also applicable to other high organic sulfur coals (such as LL coal, WJZ coal, and SY coal) and high-sulfur petroleum coke.
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COMBUSTION AND FLAME
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2023
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IF 4.4
Jinhu Liang,Ruining He,Shashank S. Nagaraja,A. Abd El-Sabor Mohamed,Haitao Lu,Yousef M. Almarzooq,Xiaorui Dong,Olivier Mathieu,William H. Green,Eric L. Petersen,S. Mani Sarathy,Henry J. Curran
2,3-Dimethyl-2-butene (TME) is a potential fuel additive with high research octane number (RON) and octane sensitivity ( S ), which can improve internal combustion engine performance and efficiency. However, the combustion characteristics of TME have not been comprehensively investigated. Thus, it is essential to study the combustion characteristics of TME and construct a detailed chemical kinetic model to describe its combustion. In this paper, two high-pressure shock tubes and a constant-volume reactor are used to measure ignition delay times and laminar flame speeds of TME oxidation . The ignition delay times were measured at equivalence ratios of 0.5, 1.0, and 2.0 in “air”, at pressures of 5 and 10 bar, in the temperature range of 950 – 1500 K. Flame speeds of the TME/ “air” mixtures were measured at atmospheric pressure, at a temperature of 325 K, for equivalence ratios ranging from 0.78 to 1.31. Two detailed kinetic mechanisms were constructed independently using different methodologies; the KAUST TME mechanism was constructed based on NUIGMech1.1, and the MIT TME mechanism was built using the Reaction Mechanism Generator (RMG). Both mechanisms were used to simulate the experimental results using Chemkin Pro. In the present work, reaction flux and sensitivity analyses were performed using the KAUST mechanism to determine the critical reactions controlling TME oxidation at the conditions studied.
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MICROCHIMICA ACTA
·
2023
·Vol. 190
·期 3
·1-10
·
IF 5.7
Liu Yuyao,Deng Yuan,Liao Dongyun,Han Yujie,Wang Qiang,Guo Yujing,Bai Hongcun,Dong Chuan,Fan Lifang
A label-free and efficient electrochemical (EC) sensing platform for di-2-ethylhexyl phthalate (DEHP) was developed based on in situ probe nickel hexacyanoferrate nanoparticle (NiHCF NP)-decorated three-dimensional reduced graphene oxide (3D rGO) composites. NiHCF NPs in the composites as an in situ probe show a pair of well-defined peaks with good reversibility and stability. Coupling 3D rGO with NiHCF NPs not only improved the electron transfer capability of NiHCF NPs but also provided more sites for aptamer immobilization. The synthesized NiHCF NP-decorated 3D rGO composites were used to act as a substrate for the immobilization of anti-DEHP aptamer by the covalent bonding method. The designed EC sensing platform displays excellent sensing performance for DEHP with a low detection limit of 3.64 pg/L, and a linear working range of 0.01 − 1000 ng/L. The application of the sensing platform to actual environmental samples was studied and satisfactory results were obtained. Thus, the proposed EC sensing platform would provide a potential tool for efficient detection of pollutants in the environment. Graphical abstract
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JOURNAL OF THE SCIENCE OF FOOD AND AGRICULTURE
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2023
·Vol. 103
·期 7
·3628-3637
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IF 4.1
Yuanyuan Xue,Youwu Liao,Haiqiao Wang,Shuang Li,Zhengqing Gu,Michael Adu-Frimpong,Jiangnan Yu,Ximing Xu,Hugh D. C Smyth,Yuan Zhu
BACKGROUND Astaxanthin is a type of food-derived active ingredient with antioxidant, antidiabetic and non-toxicity functions, but its poor solubility and low bioavailability hinder further application in food industry. In the present study, through inclusion technologies, micellar solubilization and electrospray techniques, we prepared astaxanthin nanoparticles before optimizing the formulation to regulate the physical and chemical properties of micelles. We accomplished the preparation of astaxanthin nanoparticle delivery system based on single needle electrospray technology through use of 2-hydroxypropyl-β-cyclodextrin and Soluplus® to improveme the release behavior of the nanocarrier. RESULTS Through this experiment, we successfully prepared astaxanthin nanoparticles with a particle size of approximately 80 nm, which was further verified with scanning electron microscopy and transmission electron microscopy. Furthermore, the encapsulation of astaxanthin molecules into the carrier nanoparticles was verified via the results of attenuated total reflectance intensity and X-ray powder diffraction techniques. The in vitro release behavior of astaxanthin nanoparticles was different in media that contained 0.5% Tween 80 (pH 1.2, 4.5 and 6.8) buffer solution and distilled water. Also, we carried out a pharmacokinetic study of astaxanthin nanoparticles, in which it was observed that astaxanthin nanoparticle showed an effect of immediate release and significant improved bioavailability. CONCLUSION 2-hydroxypropyl-β-cyclodextrin and Soluplus® were used in the present study as a hydrophilic nanocarrier that could provide a simple way of encapsulating natural function food with repsect to improving the solubility and bioavailability of poorly water-soluble ingredients. © 2023 Society of Chemical Industry.
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WATER RESEARCH
·
2023
·
IF 12.8
Wei-Ran Han,Wen-Long Wang,Tie-Jun Qiao,Wei Wang,Hang Su,Chen-Xin Xu,Qian-Yuan Wu
Micro-bubble aeration is an efficient way to promote ozonation performance, but the technology is challenged by extensive energy cost. Here, a ceramic ultrafiltration membrane was used to achieve ozone micro-bubble (0–80 µm) aeration in a simple way at gaseous pressures of 0.14–0.19 MPa. Compared with milli-bubble aeration, micro-bubble aeration increased the equilibrium aquatic O 3 concentrations by 1.53–3.25 times and apparent O 3 transfer rates by 3.12–3.35 times at pH 5.0–8.0. Consequently, the • OH yield was 2.67–3.54 times via faster O 3 transfer to the aquatic solution followed by decomposition rather than interfacial reaction. Ozone micro-bubble aeration outperformed milli-bubble aeration, with the degradation kinetics of 2,4-D being 3.08–4.36 times higher. Both O 3 -oxidation and • OH oxidation were important to the promotion with the contributions being 35.8%-45.9% and 54.1%-64.2%, respectively. The operational and water matric conditions influenced the oxidation performance via both O 3 oxidation and • OH oxidation, which is reported for the first time. In general, the ceramic membrane offered a low-energy approach of ozone micro-bubble aeration for efficient pollutant degradation. The O 3 oxidation and • OH oxidation were proportionally promoted by ozone micro-bubble due to O 3 transfer enhancement. Thus, the promotive mechanism can be interpreted as the synchronous enchantment on ozone exposure and • OH exposure for the first time.
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BIOMEDICAL AND ENVIRONMENTAL SCIENCES
·
2023
·
IF 3.5
Hao CHEN,Zhi Yuan HOU,Die CHEN,Ting LI,Yi Ming WANG,Marcelo Andrade DE LIMA,Ying YANG,Zhen Zhong GUO
Objective Late 2019 witnessed the outbreak and widespread transmission of coronavirus disease 2019 (COVID-19), a new, highly contagious disease caused by novel severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). Consequently, considerable attention has been paid to the development of new diagnostic tools for the early detection of SARS-CoV-2. Methods In this study, a new poly-N-isopropylacrylamide microgel-based electrochemical sensor was explored to detect the SARS-CoV-2 spike protein (S protein) in human saliva. The microgel was composed of a copolymer of N-isopropylacrylamide and acrylic acid, and gold nanoparticles were encapsulated within the microgel through facile and economical fabrication. The electrochemical performance of the sensor was evaluated through differential pulse voltammetry. Results Under optimal experimental conditions, the linear range of the sensor was 10 −13 –10 −9 mg/mL, whereas the detection limit was 9.55 fg/mL. Furthermore, the S protein was instilled in artificial saliva as the infected human saliva model, and the sensing platform showed satisfactory detection capability. Conclusion The sensing platform exhibited excellent specificity and sensitivity in detecting spike protein, indicating its potential application for the time-saving and inexpensive detection of SARS-CoV-2.
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TALANTA
·
2023
·
IF 6.1
Tao Peng,Lianhua Dong,Xiaoli Feng,Yi Yang,Xia Wang,Chunyan Niu,Zhanwei Liang,Wang Qu,Qingcui Zou,Xinhua Dai,Minghua Li,Xiang Fang
More than forty antigen testing kits have been approved to response the prevalence of SARS-CoV-2 and its variant strains. However, the approved antigen testing kits are not capable of quantitative detection. Here, we successfully developed a lateral flow immunoassay based on colloidal gold nanoparticles (CGNP-based LFIA) for nucleocapsid (N) protein of SARS-CoV-2 quantitative detection. Delta strain (NMDC60042793) of SARS-CoV-2 have been cultured and analyzed by our developed digital PCR and LFIA methods to explore the relationship between N protein amount and N gene level. It indicated that the linear relationship (y = 47 ×) between N protein molecule number and N gene copy number exhibited very well (R 2 = 0.995), the virus titers and N protein amount can be roughly estimated according to nucleic acid testing. Additionally, detection limits (LODs) of nine approved antigen testing kits also have been evaluated according to the Guidelines for the registration review of 2019-nCoV antigen testing reagents. Only three antigen testing kits had LODs as stated in the instructions, the LODs of Kits have been converted into the N gene and N protein levels, according to the established relationships among virus titer vers. N gene and antigen. Results demonstrated that the sensitivity of nucleic acid testing is at least 1835 times higher than that of antigen testing. We expect that the relationship investigation and testing kits evaluation have the important directive significance to precise epidemic prevention.
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危险品化学品经营许可证（带存储）