ChemPlusChem
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2023
·Vol. 88
·期 7
·e202300247
·
IF 3.4
Libao Han,Minghuo Wu,Yufeng Hu
Graphical A colorimetric detection method based on Fe 3 O 4 /SnS 2 composites was established for the detection and discrimination of ten phenols for the first time. The incorporation of the photo catalyst SnS 2 significantly improved the peroxidase-like activity of Fe 3 O 4 , leading to an enhancing efficiency of the colorimetric detection method. The developed method could rapidly determine the total phenols in real water samples. Phenols pose a great threat to human and environment due to their high toxicity and low bio-degradability. Therefore, the development of a rapid and sensitive detection method for multiple phenols is of great importance. Here, a colorimetric detection method based on Fe 3 O 4 /SnS 2 composites was established for the detection and discrimination of ten phenols for the first time. The results demonstrated that the incorporation of the photo catalyst SnS 2 significantly improved the peroxidase-like activity of Fe 3 O 4 , leading to an enhancing efficiency of the colorimetric detection method. The developed method was capable of detecting phenol within a concentration range of 0.5–2000 μM, with detection limit as low as 0.06 μM. This method was successfully applied to detect total phenols in samples obtained from two sewage treatment plants and seawater. Furthermore, by employing principal component analysis, the established colorimetric method enabled the simultaneous discrimination of all ten phenols. The performance was further evaluated by accurately identifying binary or ternary mixtures of phenols, and even identifying the type of phenol in 10 unknown samples containing one of the ten phenols. These findings highlight the potential of the Fe 3 O 4 /SnS 2 composite as a promising candidate for the simultaneous detection of multiple phenols in liquid samples.
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CHEMOSPHERE
·
2023
·
IF 8.8
Hao Li,Canyuan Lin,Ruhui Ma,Yuancai Chen
In this study, the selective adsorption of aromatic compounds on mesoporous MIL-53(Al) was investigated, and followed the order: Biphenyl (Biph) > Triclosan (TCS) > Bisphenol A (BPA) > Pyrogallol (Pyro) > Catechol (Cate) > Phenol (Phen), and exhibited high selectivity toward TCS in binary compounds. In addition to hydrophobicity and hydrogen bonding, π–π interaction/stacking predominated, and more evidently with double benzene rings. TCS-containing halogens could increase π interaction on the benzene rings via forming Cl–π stacking with MIL-53(Al). Moreover, site energy distribution confirmed that complementary adsorption mainly occurred in the Phen/TCS system, as evidenced by Δ Q pri (the decreased solid-phase TCS concentration of the primary adsorbate) < Q sec (the solid-phase concentrations of the competitor (Phen)) . In contrast , competitive sorption occurred in the BPA/TCS and Biph/TCS systems within 30 min due to Δ Q pri = Q sec , followed by substitution adsorption in the BPA/TCS system, but not for the Biph/TCS system, likely attributed to the magnitude of energy gaps (E g ) and bond energy of TCS (1.80 eV, 362 kJ/mol) fallen between BPA (1.74 eV, 332 kJ/mol) and Biph (1.99 eV, 518 kJ/mol) according to the density-functional theory of Gaussian models. Biph with a more stable electronic homeostasis than TCS lead to the occurrence of substitution adsorption in the TCS/BPA system, but not in the TCS/Biph system. This study provides insight into the mechanisms of different aromatic compounds on MIL-53(Al).
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Pharmaceutics
·
2023
·Vol. 15
·期 8
·2135
·
IF 5.4
Jia Liu,Peng Sun,Xiaole Qi
Clinically, indobufen is widely used for the treatment of antiplatelet aggregation and anticoagulation. Prior studies have discovered that abnormal platelet function can be promptly restored to normal when the drug is stopped. Herein, through the study of the enzyme reaction kinetics, we demonstrated that the inhibitory effect of indobufen on cyclooxygenase-1 (COX-1) was reversible and non-competitive. Specifically, the cyclooxygenase inhibition experiment showed that the level of 6-keto-PGF1α in the gastric mucosa of the indobufen-treated groups was significantly higher than that of the aspirin group (###p< 0.001), indicating a higher level of PGI2in and a better physiological state of the gastric mucosa. Moreover, the rat gastric ulcer index and mucosal section experiments further confirmed the relief of gastrointestinal irritation and the adverse reaction rate of the indobufen-treated group compared to those of the aspirin group. Furthermore, indobufen was verified to exert reversible inhibitory activity on the heme group of COX-1 and thus reversibly inhibit COX-1 activity. In general, compared with aspirin, the long-term oral administration of indobufen yields a lower risk of gastrointestinal symptoms, such as ulcers.Keywords:indobufen;anticoagulant effect;antiplatelet effect;adverse reaction;COX-1
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Zhuangzhuang Zhang,Haiqian Zhao,Zhonghua Wang,Zhipei Hu,Qingshu Wang,Erlin Meng,Shiwei Lai,Jiaxin Ying,Hongguang Li,Chuanyan Wu
The use of the electro-Fenton process to continuously generate H 2 O 2 and efficiently degrade organic pollutants is considered a promising technology . The ratio of generation of H 2 O 2 is usually regarded as the critical step; however, how the H 2 O 2 is utilized is also of particular importance. Herein, activated carbon was activated at different temperatures and used to explore the effect of nitrogen doping on the production and utilization of H 2 O 2 in the electro-Fenton-based degradation of organic pollutants. The experimental results indicate that nitrogen-doped activated carbon simultaneously promotes the generation and utilization of H 2 O 2 , which is attributed to the regulation of the competition between phenol and O 2 adsorption by the doped nitrogen. Nitrogen doping not only improves 2e − ORR selectivity but also aggregates phenol near the cathode to balance the concentrations of phenol and ·OH. Density functional theory (DFT) calculations further confirmed that pyrrole-N as a dopant promoted the adsorption of phenol , while pyridine-N was more favorable for O 2 adsorption. The unique balance of nitrogen types possessed by modified activated carbon NAC-750 permits the efficient synergistic generation and utilization of H 2 O 2 in a balanced manner during the degradation of phenol. This work provides a new direction for the rational nitrogen-doping modification of activated carbon for the electro-Fenton-based degradation of organic pollutants.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Haiqing Zhang,Richard Lee Smith,Haixin Guo,Xinhua Qi
Ordered mesoporous carbons (OMCs) functionalized with catalytically-active metals have many potential applications in sulfate radical-based advanced oxidation processes for degrading antibiotics. Cobalt cross-linked ordered mesoporous carbon materials (OMC-Co-Tx) were synthesized through evaporation-induced self-assembly, calcinated at (600 to 800) o C. The OMC-Co-Tx materials were then employed as peroxymonosulfate (PMS) activators for removal of sulfamethoxazole (SMX) from aqueous solutions. OMC-Co-T800 prepared by calcination at 800 °C had a large specific surface area (449 m 2 /g), uniform pore structure (∼4.5 nm) and showed the best performance for activation of PMS. With a dosage of 0.1 g/L OMC-Co-T800 and 0.4 g/L PMS, the functionalized OMC material allowed SMX (10 mg/L) removal of up to 99% in 30 min. The increase of calcination temperature promoted the reduction of cobalt in OMC materials and increased the defects in their structure, resulting in better catalyst behavior. Quenching experiments and electron paramagnetic resonance analyses showed that reactive species of sulfamethoxazole degradation involved in the OMC-T800/PMS system were SO 4 •− , OH, O 2 •− and 1 O 2 . HPLC-MS analyses of degradation intermediates formed in the OMC-Co-T800/PMS system allowed elucidation of four transformation pathways for SMX degradation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Zhipeng Luo,Yao Xu,Diyong Tang,Li Lu,Yuanfang Li,Mengmeng Zhang,Jie Sun
For persulfate-based advanced oxidation process, the non-radical pathway is an important route due to the selective oxidation of pollutants and its strong tolerance to complex water bodies. However, the selective oxidation mechanism of organic pollutants needs further elaboration. Herein, we demonstrate a facile hydrothermal pretreatment and high-temperature carbonization route to synthesize the nitrogen-doped porous biochar (NHBC-1). Owing to the well-developed hierarchical porous structure, the created internal active defects, and tailored nitrogen dopants, the NHBC-1 catalyst exhibited excellent catalytic activity for peroxydisulfate (PDS) activation. The results show that pyridinic N facilitated the adsorption of PDS on NHBC-1 to form the highly active NHBC-PDS* complex. Meanwhile, graphitic N and the defective structures promoted the electron-transfer process, thus allowing the efficient catalytic performance of the NHBC/PDS system for phenol oxidation via an electron-transfer dominated pathway. In addition, the system exhibited versatile applicability for the remediation of various organic pollutants in different actual water matrices with wide pH adaptability and satisfactory mineralization efficiency. More importantly, the selective oxidation mechanism of organic contaminants was revealed. Specifically, only the pollutant with oxidation potential lower than that of the NHBC-PDS* complex (0.91 V) can be effectively eliminated. This study not only provides a facile route for the rational designing of a cost-affordable biochar catalyst for PDS activation, but also offers valuable insights into the understanding of selective oxidation of organic contaminants via an electron-transfer dominated pathway.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xin Lv,Chenying Zhou,Zhichao Shen,Yuchen Zhang,Chuanshu He,Ye Du,Zhaokun Xiong,Rongfu Huang,Peng Zhou,Bo Lai
The acceleration of Fe(III)/Fe(II) conversion in Fenton systems is the critical route to achieve the long-lasting generation of reactive oxygen species towards the oxidation of refractory contaminants. Here, we found that waste leather derived porous carbon materials (LPC), as a simple and readily available metal-free biochar material, can promote the Fe(III)/H 2 O 2 system to generate hydroxyl radicals ( • OH) for oxidizing a broad spectrum of contaminants. Results of characterizations, theoretical calculations, and electrochemical tests show that the surface carbonyl groups of LPC can provide electron for direct Fe(III) reduction. More importantly, the graphitic-N on surface of LPC can enhance the reactivity of Fe(III) for accelerating H 2 O 2 induced Fe(III) reduction. The presence of LPC accelerates the Fe(III)/Fe(II) redox cycle in the Fe(III)/H 2 O 2 system, sustainable Fenton chain reactions is thus initiated for long-lasting generation of hydroxyl radicals without adding Fe(II). The continuous flow mode that couples in-situ Fenton-like oxidation and LPC with excellent adsorption catalytic properties, anti-coexisting substances interference and reusability performance enables efficient, green and sustainable degradation of trace organic pollutants . Therefore, the application of metal-free carbon materials in Fenton-like system can solve its rate-limiting problem, reduce the production of iron sludge , achieve green Fenton chemistry , and facilitate the actual engineering application of economic and ecological methods to efficiently remove trace organic contaminants from actual water sources.
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CORROSION SCIENCE
·
2023
·
IF 8.3
Jinke Wang,Lingwei Ma,Zhibin Chen,Yue Wang,Chenhao Ren,Tong Liu,Li Ma,Cunguo Lin,Dawei Zhang
A high-throughput method was proposed to screen coating fillers with both good corrosion-sensing and inhibition performances. SiO 2 nanoparticles loaded with different percentages of phenanthroline (Phen) and 1-hexadecyl-3-methylimidazolium chloride (HDMIC) were prepared (Ph-HD@SN) using a multi-channel synthesis instrument. The corrosion-sensing ability of different Ph-HD@SN to detect Fe 2+ ions can be determined by spectrophotometric method within 30 s. The corrosion inhibition effect of Ph-HD@SN was evaluated by visual assessment and quantification of iron dissolution from carbon steel in NaCl solutions containing different nanoparticles . The optimized Ph-HD@SN was incorporated into epoxy coating to achieve the corrosion-sensing and self-healing properties.
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Journal of Materials Chemistry A
·
2023
·
IF 11.9
Han-Yue Yang,Kai-Yue He,Xuan Ai,Xue Liu,Yun Yang,Shi-Bin Yin,Pu-Jun Jin,Yu Chen
The nitrate electroreduction reaction (NO3RR) serves as an environmentally friendly method for ammonia (NH3) synthesis and effectively mitigates nitrate pollution in natural water bodies. The chemical functionalization of noble metal nanostructures can effectively enhance their activity and selectivity in electrocatalytic reactions. In this study, we successfully synthesized pyridine (Py) functionalized silver (Ag) nanosheets (Py–Ag NSs) as an electrocatalyst for NO3RR. Density functional theory calculation results revealed that the adsorbed pyridine modulated the electronic structure of Ag atoms, thereby facilitating the adsorption of nitrate ions and the following reduction steps. Consequently, Py–Ag NSs revealed significantly improved activity for NO3RR compared to pure Ag catalysts. Notably, at a potential of −0.53 V, Py–Ag NSs exhibited a faradaic efficiency and production rate of NH3 reaching 96.6% and 72.664 mg h−1 mgcat−1, respectively. This work provides valuable insights into the modulation of electronic structures using a chemical functionalization strategy, thus guiding the rational design of noble metal-based electrocatalysts.
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JOURNAL OF ETHNOPHARMACOLOGY
·
2023
·
IF 5.4
Mengqi Shi,Tianshi Li,Yan Zhao,Zhongmei He,Ying Zong,Weijia Chen,Rui Du
Ethnopharmacological relevance Antler glue is a classic medicinal to enhance sexual function in traditional Chinese medicine (TCM), which was first recorded in Shen Nong Ben Cao Jing (Shennong′s Classic of the Materia Medica) . Vinegar-processing is a classic method of processing traditional Chinese medicine. The method of preparing antler glue by boiling antlers in vinegar and then concentrating them is recorded in Lei Gong Pao Zhi Lun (Master Lei′s Discourse on Medicinal Processing) . In modern times, the typical processing method of antler glue is water extraction and concentration. However, it is not clear whether there is a difference in the effect of these two processing methods on the chemical composition and pharmacological activity of antler glue. Aim of the study The Chinese Pharmacopoeia (2020) records that the processing method of antler glue is water extraction and concentration. But Lei Gong Pao Zhi Lun differs in Chinese Pharmacopoeia (2020) , which records the processing method of vinegar extraction and concentration. The effect of the two processing methods on antler glue's chemical composition and pharmacological activity is unknown. So this study aimed to elucidate the difference between different processing methods on the chemical composition and the treatment effect on oligoasthenospermia of antler glue. Materials and methods So the automatic amino acid analyzer is used to determine the amino acid content of two different processing methods of antler glue. Proteomics was performed to detect the protein components of two different processing methods of antler glue and analyze them. Cyclophosphamide-induced mice models of oligoasthenospermia were used to study the different pharmacological effects of antler glue in two different processing methods. An automatic sperm analyzer observed the quantity and quality of sperm in mice epididymis. Serum sex hormone testosterone (T), luteinizing hormone (LH) and follicle stimulating hormone (FSH) levels in mice were tested using the enzyme-linked immunosorbent assay (ELISA) kits. Hematoxylin-eosin (H&E) staining was used to analyze pathological alterations in mouse testicular tissue. The transcriptome has been used to reveal the potential mechanism of antler glue in treating oligoasthenospermia. Mitochondrial complex activity assay kits were used to assay the activity of mitochondrial respiratory chain complex I–V in mouse testicular tissue. Western blot was used to determine the expression of related proteins in mouse testicular tissue. Results Vinegar-processing can increase the alanine , proline , and glycine content in antler glue, reduce the length of protein peptides in antler glue, and produce a variety of unique proteins. Vinegar-processed antler glue (VAG) increased sperm density, sperm survival, sperm viability, and serum sex hormone levels in oligozoospermic mice. It reversed testicular damage caused by cyclophosphamide, and the effects were differently superior to those of water-processed antler glue (WAG). In addition, transcriptomics and related experiments have shown that VAG can increase the expression of Ndufa2, Uqcr11, Cox6b1, and Atp5i genes and proteins in mouse testis, thus promoting adenosine diphosphate (ATP) synthesis by increasing the activity of mitochondrial respiratory chain complexes I, III, IV and V. By promoting the oxidative phosphorylation process to produce more ATP, VAG can achieve the therapeutic effect of oligoasthenospermia. Conclusion Vinegar-processing method can increase the content of active ingredients in antler glue. VAG increases ATP levels in the testes by promoting the process of oxidative phosphorylation to treat oligozoospermia.
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ACS Applied Polymer Materials
·
2023
·
IF 5
Jingkai Liu,Liyue Zhang,Xinbei Zhu,Qing Chen,Kan Zhang,Xiaoqing Liu
Phenolic derivatives capable of reducing the ring-opening temperature of benzoxazine resin have gradually emerged as valuable modules for benzoxazine chemistry, not to mention their good compatibility, coreactivity, and network modifiability. However, the previously reported unsatisfactory promotion effects, unclear reaction mechanisms, and unstable structure have severely limited the development of benzoxazine/phenol systems. Herein, a supramolecular hydrogen-bonded system consisting of resorcinol and 2-aminopyridine benzoxazine (PH-2a) was developed. The PH-2a/resorcinol mixture system with an equivalence ratio of 1:1 exhibited a dramatic reduction in ring-opening peak temperature (Tp) from 283 to 110 °C. Experimental combined with computational investigations supported its supramolecular H-bond behavior. Based on the cross-comparison of PH-2a analogues and other diphenols, the critical roles of H-bonding interactions both in activating reactants and inducing a directional reaction were revealed. These H-bonds with appropriate strengths can self-assembly form and close the distance between potential reaction sites, facilitating the direct production of an adduct. In addition, the application potential of the PH-2a/resorcinol system was also prospected, which can promise network tailoring and low-temperature cross-linking by the design flexibility of PH-2a and resorcinol derivatives, opening up possibilities for the preparation of advanced polybenzoxazine resins at low temperature.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Jing Zhu,Hongwei Jiang,Wenwu Wang
The high toxicity and low biodegradability of the phenolic pollutants destroyed the balance of the environment and influenced human health seriously. Here, we developed a three-dimensional coloremetric sensor array for discriminating and determinating phenolic pollutants basing on the distinct Cu/nucleotides MOFs . Firstly, three laccase-mimic Cu/MOFs (Cu/AMP, Cu/CMP, and Cu/GMP) were obtained by regulating the molar ratio of Cu 2+ and nucleotides. Then the Cu/MOFs as the recognition elements of the sensor array catalyzed the pollutants-4-AAP-H 2 O 2 system, obtaining the colored benzoquinone products. Subsequently, the data array obtaining from the combined training matrix (3 Cu/MOFs × 6 pollutants × 5 replicates) was projected into a new dimensional space to obtain the 3D canonical scores, and classified into individual clusters by introducing LDA method. No overlap in their respective LDA plots for the six phenolic pollutants with different concentrations suggested the prominent discriminating performance of the sensor array. Furthermore, the sensor array exhibited high selectivity compared to the “lock-and-key” sensors even other active matrices coexisting in water samples. Importantly, the most influential discrimination factor was used to monitor the levels of the six targets, evidencing the potential application in assessing water pollution and maintaining human health.
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