COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
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2023
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IF 8.7
Ronghua Yu,Xin Wen,Yue Zhu,Shenghui Lou,Yongjiang Li,Shengda Wang,Jie Liu,Tao Tang
The application of polymer materials has provided the convenience and also bring fire risk and hazard due to intrinsic flammable property of polymers. Here we demonstrate a novel strategy using boron-doped copper phenylphosphate (BCuPP) nanosheets with temperature-response characteristics as only flame retardant for creating high fire-safety polycarbonate (PC) nanocomposites with excellent comprehensive performances. PC/BCuPP nanocomposites presents a good mechanical performance at room temperature due to the strong interfacial interaction between PC matrix and BCuPP nanosheets. Furthermore, BCuPP exhibits unique temperature-response behavior driven by fire, where fully molten boron oxide flows freely, followed by in-situ formed BPO 4 to repair the defects to form a complete and continuous protective layer. So the temperature-response behavior endows PC/BCuPP nanocomposites excellent fire-safety performance with dramatical decrease in both heat release rate and total smoke production. This study offers a novel route only incorporating nanoparticles as flame retardant to create high fire-safety polymer nanocomposites.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Dingxiang Wang,Yongqiang Yu,Jiahao He,Jun Ma,Jing Zhang,Timothy J. Strathmann
Most previous studies examined permanganate or ferrate oxidation using various emerging pollutants (EPs) spiked in ultrapure water with concentrations of orders-of-magnitude higher than those in natural waters. In present study, we assessed the efficiency of permanganate and ferrate (with ozone as a comparison) at mg L −1 level to remove selected EPs at μg L −1 level in complex water matrices. The efficiency of permanganate and ferrate is more easily affected by the humic acid in synthetic water or dissolved organic matter (DOM) in natural river water compared to ozone. Experiment results revealed that humic acid or DOM were not mineralized by oxidants, but changed in compositional nature, including decreases in the aromaticity, electron-donating capacity, and average molecular weight . At molecular level, condensed aromatic, lignin-like, and tannin-like components in humic acid and DOM are the critical sites being attacked by permanganate or ferrate, the alkene groups and aromatic structures were oxidized predominantly to carboxylic acids . Overall, the present study provided insights into the performance of permanganate and ferrate used for EPs treatment under realistic conditions, as well as alternations of DOM that can be expected following exposure to these oxidants.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2023
·Vol. 24
·期 19
·14708
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IF 5.6
Xianheng Li,Huan Li,Keqiang Lai,Junjian Miao
The interaction mechanism of hemoglobin (Hb) with bisphenol A (BPA) in diabetic patients and the difference with healthy people have been studied using spectroscopic and molecular docking techniques at several glucose (Glc) concentration, with bovine hemoglobin (BHb) instead of Hb. It is found that Glc can interact with BHb–BPA and affect its molecular structure, resulting in an altered microenvironment for tyrosine (Tyr) and tryptophan (Trp) in BHb–BPA. It is also found that Glc can bind to BHb alone, and its effect on the molecular structure of BHb is weaker than that on the structure of BHb in BHb–BPA complex. The results of circular dichroism (CD) and Fourier transform infrared spectroscopy (FTIR) indicate that Glc causes an increase in the content of the α-helix and a decrease in that of the β-sheet of BHb–BPA by 1.5–1.9% and 3.1%, respectively. The results of molecular docking show that Glc binds to BHb–BPA through hydrogen and hydrophobic bonds, and the position of binding differs from that of Glc binding to BHb alone, which may be attributed to the fact that BPA affects the protein molecular structure of BHb and has an effect on the binding of BHb to Glc. This study provides some theoretical basis for the mechanism of BPA toxicity in vivo for people with different blood glucose levels.Keywords:glucose;bisphenol A;bovine hemoglobin;spectroscopic techniques;molecular docking
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
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IF 9.8
Feilong Dong,Chuyun Fu,Zhu Meng,Qiufeng Lin,Jinzhe Li,Tao Zeng,Da Wang,Juntao Tang,Shuang Song
Ferrate (Fe(VI)) has been extensively studied as a green oxidant to treat wastewater. But Fe(VI) oxidation still faces several challenges for application, such as the sensitivity of Fe(VI) to pH and the restrictions on the Fe(VI) utilization efficiency for pollutant elimination at low concentration levels. This study proposed a two-stage Fe(VI) oxidation process to enhance the bisphenol A (BPA) removal for potential applicability, consisting of the adsorption by CNTs of stage I and the degradation by Fe(VI) of stage II. The Fe(VI) utilization efficiency in the two-stage process (0.848) was higher than that in one-stage processes (0.727) and Fe(VI) alone system (0.504) at pH 9. In stage I, the adsorption process had good compliance with the Langmuir isotherm model and pseudo-second-order kinetic model. In stage II, the effective utilization of low-concentration Fe(VI) was 2.45 times more than Fe(VI) alone, and the reduction of reaction volume was beneficial to further enhance utilization. The probe experiments (sulfoxide) and the degradation experiments of other electron-donating/withdrawing pollutants (e.g., atrazine, benzoic acid) demonstrated that Fe(IV) and Fe(V) were major oxidizing species in the two-stage process. The regeneration experiments showed that CNTs still had acceptable adsorption and catalytic capabilities after five cycles. Finally, the intermediate products in the two-stage process were detected and four possible degradation pathways of BPA were proposed. These findings were meaningful for the practical application of Fe(VI) oxidation to overcome the conditional limitation and improve the utilization.
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CARBOHYDRATE POLYMERS
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2023
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IF 11.2
Wenwen Bie,Shuzhao Zhang,Lin Zhang,Hengye Li,Xiaoyu Sun,Tianpei Cai,Zhongxia Wang,Fenying Kong,Wei Wang
Herein, a thioether-functionalized porous β-cyclodextrin polymer (P(Bn-S-CD)) was prepared for efficient removal of heavy metal ions and organic micropollutants (OMPs) from water. P(Bn-S-CD) showed a surface area of 763 m 2 /g and a sulfur content 5.83 wt%. Based on screening studies, Hg 2+ and diclofenac sodium (DS) were selected as model pollutants. P(Bn-S-CD) could adsorb Hg 2+ and DS simultaneously, while the adsorbed Hg 2+ afforded positive charges to the primary rims of CDs, greatly enhancing the adsorption rate and adsorption capacity of DS. Although the adsorbed DS showed no obvious effect on Hg 2+ adsorption, it improved the affinity of Hg 2+ upon P(Bn-S-CD). Adsorption mechanism studies confirmed the essential role of electrostatic interactions for these results. P(Bn-S-CD) also showed good selectivity towards heavy metal ions, excellent adsorption performance in real water at environmental levels and good reusability, implying great promise for water treatment.
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MATERIALS RESEARCH BULLETIN
·
2023
·
IF 5.4
Junge Zhang,Yuan Ding,Xianggang Ma,Yingliang Liu,Li Zhang,Kunlun Wang,Shaokui Cao,Shengang Xu
The rapid recombination of photogenerated carriers and the narrow absorption range of visible light greatly limit the photocatalytic activity of graphite carbon nitride (g-C 3 N 4 ). Herein, g-C 3 N 4 was jointly modified by carbon dots (CDs) and copolymerization via in situ co-calcining of three precursors (urea, glucose and 2-amino-5-iodo-benzonitrile (I-ABN)), and named as I-ABN x -C 3 N 4 @CDs y . Then, solid-state Z-scheme photocatalysts PC1–PC9 with CDs as the electron mediators were prepared via in situ growth of BiOI on the surface of I-ABN x -C 3 N 4 @CDs y through solvothermal method. The optimal proportion of each component was explored through orthogonal experiments. The existence of CDs act as an electron transport medium to accelerate the transportation rate of photogenerated carriers, improve the light absorption capacity. The copolymerization with I-ABN introduce benzene rings and I − to g-C 3 N 4 , which enhance the light absorption capacity and photoelectric efficiency. The Z-scheme heterojunction effectively suppresses the recombination of photogenerated electron–hole pairs. Therefore, PC1–PC9 presented excellent performance for the degradation of BPA due to the synergistic effects of the above three points. Among them, PC6 showed the best photocatalytic activity, which completely degraded BPA (15 mg/L) within 40 min, and whose rate constant (0.091 min −1 ) was 22.8 times that of bulk g-C 3 N 4 . The active radical trapping experiment determined •O 2 − and h + were the main active radicals. Finally, the BPA degradation mechanism by PC6 was proposed. This study provides new insights for the combination of heterojunction, carbon dots, and copolymerization to rationally design efficient photocatalysts to restore the environment.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Jinming Feng,Jincheng Mu,Qiong Peng,Yang Xiao,Baojun Liu
Cobalt-based oxides have attracted extensive attention in heterogeneous catalytic peroxymonosulfate (PMS) activation towards emerging pollutants degradation, while the improvement of their catalytic performance is still a severe challenge. Herein, a CoO x ultrathin nanosheet composed of in situ interfacial Co 3 O 4 and CoO (CoO x -Ar-350) was synthesized and employed in PMS activation for micro-contaminates removal. The catalyst shows 100 % bisphenol A (BPA) conversion within 2 min ([BPA] = 20 mg/L, [Catalyst] = 20 mg/L, [PMS] = 200 mg/L) with a remarkable reaction rate of 2.69 min −1 , which is 3.84 and 2.66 times of pure Co 3 O 4 and CoO, respectively. Characterization and theoretical calculation results indicates that the interfacial synergy between Co 3 O 4 and CoO could modulate the adsorption behavior and enhance the electron acceptance of PMS, which boosts the breaking of O-O bonds and the generation of reactive oxygen species (ROS) and thereby the pollutant removal efficiency. The ROS quenching and capture experiments demonstrate that the enhanced OH and 1 O 2 play significant contribution during the degradation process. This work provides a novel in situ interfacial engineering for the development of highly efficient catalyst and reveals the activity enhancement mechanism for PMS activation.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Mei-Mei Wang,Yun-Ke Cui,Jia-Tai Wen,Yan-Shan Wang,Meng-Hui Jia,Shu-Zhen He,Wei-Kang Wang,Juan Xu
Radical and nonradical dominated persulfate activation processes have pros and cons in the degradation of pollutants. It is challenging to flexibly tune the contribution ratios of radicals and nonradicals in a persulfate activation process for improved pollutant degradation. Herein, we successfully synthesize copper oxide catalysts derived from metal-organic frameworks. By varying the annealing temperature, valence states of copper can be regulated in the catalyst, thereby enabling the switching between radical and nonradical mechanisms for persulfate activation. Copper oxides annealed at 300 °C (CuBTC-300) demonstrate high performance in peroxydisulfate (PDS) activation for the degradation of bisphenol A (BPA), with the synergy of radical and nonradical mechanisms. The surface activated PDS-catalyst complex and OH are identified as the reactive oxidative species involved in this process. On one hand, PDS undergoes a one-electron transfer reaction with Cu(I) sites in Cu 2 O, generating SO 4 − , which subsequently converts into OH for BPA degradation. On the other hand, the combination of PDS molecules with CuO forms surface-activated complexes, depriving electrons from BPA. The increased content of Cu(II) in the catalyst gradually directs PDS activation towards the nonradical pathway. As the annealing temperature increases from 300 °C to 500 °C, the contribution of nonradical oxidation to BPA degradation increases from 58.65 % to 100 %. This work provides new insights into flexibly regulating persulfate activation mechanisms via rational catalysts design.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
·
2023
·
IF 7.8
Zezheng Lin,Yang Guo,Xiaoxuan Qu,Yuying Xiang,Shuwen Shen,Xin Zhu
Widely diffused pollution of endocrine disrupting chemicals (EDCs) has indeed threatened the safety of ecological environment and human health. A hydrangea-like Fe doped BiOBr (Fe-BiOBr) microsphere was synthesized and used to enhance the performance of UV/persulfate (PS) system using bisphenol A (BPA) as the targeted contaminant. The photochemical characterization of Fe-BiOBr showed that Fe doping markedly improved the separation efficiency of photoelectron and hole, and enhanced the utility rate of luminous energy of BiOBr. Degradation test demonstrated that with the assistance of Fe-BiOBr, the efficiency of UV/PS system was increased by 1.8 times, while 85.7% of BPA can be degraded within 10 min. Through scavenging experiments, sulfate radical (SO 4 •− ), superoxide radical (O 2 •− ), and hole were demonstrated as the dominate reactive species (RSs) in UV/Fe-BiOBr/PS system. Then, the role and mutual transformation of RSs was further clarified by radicals steady-state concentrations estimation and X-ray photoelectron spectroscopy (XPS) analysis. Based on the results, the produced O 2 •− can be subdivided into confined O 2 •− and free O 2 •− from the UV induced oxygen vacancy and photoelectron, respectively. Of which, SO 4 •− and confined O 2 •− were symbiotic via the redox cycle of Fe species. Significantly, only 2.6% of TOC can be simultaneously removed within 10 min treatment time, suggesting the incomplete degradation of BPA. For this, 16 organics was detected using LC-MS and the degradation route of BPA was also determined based on the intermediates analysis. Finally, the application possibility of the system was evaluated from the perspective of ecotoxicity by ECOSAR and T.E.S.T. softwares. This study investigates the dual effect of transition metal doped semiconductor on coupling system, and provides new insights into the role of O 2 •− .
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Xiaohuan Zang,Qingyun Chang,Fangyuan Hou,Shuaihua Zhang,Chun Wang,Zhi Wang,Jianzhong Xu
Endocrine disruption chemicals (EDCs) in food can seriously harm human health. In this study, a hydroxyl and carboxyl group functionalized conjugated microporous nanomaterial (CMP) was prepared by Friedel-Crafts reaction and used as solid-phase extraction (SPE) adsorbent. A functionalized CMP based SPE combined with high performance liquid chromatography-diode array detection was built for the determination of phenolic EDCs from nine fish samples. The extraction conditions were optimized by both single factor and response surface methodology (Box-Behnken Design). The established method performed well in terms of the response linearity (in the range of 0.50–100 ng g −1 with coefficient of determination larger than 0.9942), limits of detection (0.15–0.30 ng g −1 , S/N of 3), limits of quantification (0.50–1.00 ng g −1 , S/N = 10), method recoveries (78.4–121 %) and repeatability (relative standard deviation < 11 %). It can be used as an efficient method to detect trace phenolic EDCs in real fish samples.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Gang Chu,Wangmin Wang,Yang Dou,Wenxiu Qin,Da Tian,Youbin Si
Phosphorus (P)-rich chars produced by phosphoric-acid-assisted pyrolysis are promising carbonaceous remediation agents for soil pollution. Nevertheless, the potential of P species dissolution from P-rich chars has been ignored, and the impact of P dissolution on the sorption of hydrophobic compounds remains greatly unaddressed to date. Herein, the P species dissolution from wood-, cellulose-, and lignin-derived P-rich chars at 200–650 °C were investigated. P release capacity ranged from 0.2 to 0.3 mg·g −1 through cyclic dissolution and the maximum release capacity was 1.6 mg·g −1 through continuous dissolution. Enhanced P dissolution in soil experiment implies that P-rich char can be a potential P source. After P species dissolution, bisphenol A (BPA) sorption increased and carbamazepine (CBZ) sorption decreased onto P-rich chars. The enhanced π-π interaction facilitated BPA sorption, while the declined double charge-assisted H-bond ((±)CAHB) weakened CBZ sorption. Combined with DFT calculations, the binding energy (ΔE) supported the contrasting interfacial sorption processes. Apart from micropore-filling, the contribution of sorption mechanisms followed the sequence of (±)CAHB > π-π interaction > H-bonding. This work not only reveals that P-rich char can serve as a promising phosphatic fertilizer for soil improvement but also casts new light on the sorption mechanisms for hydrophobic compounds.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Junjie Xu,Yanchi Yao,Chao Zhu,Lun Lu,Qile Fang,Zhiqiao He,Shuang Song,Baoliang Chen,Yi Shen
The electron transfer pathway activated by peroxymonosulfate (PMS) has garnered significant attention for the removal of emerging organic pollutants from water. However, overcoming the two-step energy barriers involved in electron transport across reaction interfaces presents a formidable challenge. To surmount the two-step energy barriers of pollutant-catalyst and catalyst-PMS, a catalyst with nano-island structure was developed, forming efficient ternary catalytic interfaces with PMS and pollutants. The presence of atomic pairs within the catalyst punched through the electron transport channels, resulting in a pseudo-first-order kinetic rate of 2.06 min −1 for bisphenol A, which was 5.1 times higher than that of the control sample. The electronic coupling of atomic pairs exerted a profound impact on the splitting of d -orbitals, effectively elevating the d -orbital unoccupancy and reducing the two-step energy barriers encountered by electrons from pollutants to catalysts, and subsequently to PMS, which promoted efficient degradation of pollutants. Furthermore, through the association of two-step energy barrier, the feasibility of utilizing the orbital interaction as a descriptor of the degradation rate by electron-mediated PMS activation was demonstrated. Additionally, the intermediates generated through electron transfer pathway exhibited a lower risk of bioaccumulation. This work inspires insights into the electron-mediated mechanism of multinary catalytic interface reactions.
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