JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Mengfan Luo,Heng Zhang,Peng Zhou,Jiali Peng,Ye Du,Zhaokun Xiong,Bo Lai
The sluggish oxidation kinetics of ferrate (Fe(VI)) at neutral and slightly alkaline pH impedes its rapid abatement of micropollutants in practical application. This work discovers that graphite (GP), a metal-free carbonaceous material , can be a promising material to improve the reactivity of Fe(VI) in the pH range of 7.0 − 9.0. The performance of the GP/Fe(VI) process for sulfamethoxazole (SMX) removal was further evaluated via altering the dosages of Fe(VI), GP, and SMX. Probe analysis and quenching experiments identified Fe(IV) and Fe(V) as the primary active species responsible for the removal of organic compounds in the GP/Fe(VI) system. The detailed activation mechanism of GP is discussed via analyzing the surface chemical changes of GP exposed to Fe(VI). It is found that the carbonyl groups on GP surface execute a critical role in Fe(VI) activation. The GP/Fe(VI) system shows powerful anti-interference ability to environmental background substances. Therefore, the new oxidation process proposed in this work holds a great application prospect for contamination remediation. Finally, we discuss the underlying degradation pathways of SMX by the GP/Fe(VI) system. This study not only develops a promising system for the removal of micropollutants but also provides an in-depth insight into the activation mechanism of metal-free carbonaceous material in Fe(VI) oxidation process.
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高影响因子
MOLECULES
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2022
·Vol. 27
·期 7
·2353
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IF 4.927
Yuping Zhang,Ning Wang,Zhenyu Lu,Na Chen,Chengxing Cui,Xinxin Chen
Evaluation of the hydrophobic/hydrophilic interaction individually between the sorbent and target compounds in sample pretreatment is a big challenge. Herein, a smart titanium substrate with switchable surface wettability was fabricated and selected as the sorbent for the solution. The titanium wires and meshes were fabricated by simple hydrothermal etching and chemical modification so as to construct the superhydrophilic and superhydrophobic surfaces. The micro/nano hierarchical structures of the formed TiO2nanoparticles in situ on the surface of Ti substrates exhibited the switchable surface wettability. After UV irradiation for about 15.5 h, the superhydrophobic substrates became superhydrophilic. The morphologies and element composition of the wires were observed by SEM, EDS, and XRD, and their surface wettabilities were measured using the Ti mesh by contact angle goniometer. The pristine hydrophilic wire, the resulting superhydrophilic wire, superhydrophobic wire, and the UV-irradiated superhydrophilic wire were filled into a stainless tube as the sorbent instead of the sample loop of a six-port valve for on-line in-tube solid-phase microextraction. When employed in conjunction with HPLC, four kinds of wires were comparatively applied to extract six estrogens in water samples. The optimal conditions for the preconcentration and separation of target compounds were obtained with a sample volume of 60 mL, an injection rate of 2 mL/min, a desorption time of 2 min, and a mobile phase of acetonile/water (47/53,v/v). The results showed that both the superhydrophilic wire and UV-irradiated wire had the highest extraction efficiency for the polar compounds of estrogens with the enrichment factors in the range of 20–177, while the superhydrophobic wire exhibited the highest extraction efficiency for the non-polar compounds of five polycyclic aromatic hydrocarbons (PAHs). They demonstrated that extraction efficiency was mainly dependent on the surface wettability of the sorbent and the polarity of the target compounds, which was in accordance with the molecular theory of like dissolves like.Keywords:titanium wire;superhydrophobic;superhydrophilic;in-tube solid-phase microextraction;high-performance liquid chromatography
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CHEMOSPHERE
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2022
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IF 8.943
Ting Chen,Zhiliang Zhu,Yue Wang,Hua Zhang,Yanling Qiu,Daqiang Yin
Facilitating reactive oxygen species (ROS) generation is an effective way to promote the heterogeneous catalytic efficiency for organics removal. However, the metal leaching in metal-based catalysts and the low activity of non-metallic materials restrict ROS production. In this work, the purpose was achieved by loading a small amount of spinel CuFe 2 O 4 onto porous carbon nitride substrate. The synthesized CuFe 2 O 4 @O–CN composite first to activate peroxymonosulfate (PMS), which produce a plenty of ROS (•OH, SO 4 • − and 1 O 2 ) for organics removal, leading to highly oxidation for diverse organics. Through the comparative analysis of the surface composition before and after reaction, we found that the interface multi-electron transfer routs, including surface Cu(II)/Cu(I), Fe(III)/Fe(II) and their cross interaction, participated in the redox cycle, giving rise to the rapid and massive production of ROS, so that DMPO and TEMP were instantly oxidized in electron paramagnetic resonance (ESR) detection. Importantly, the carrier of porous O–CN, which acted as the electron transfer mediator, not only favors PMS adsorption via surface –OH, but also facilitates the conversion between different metal species. As a result, the CuFe 2 O 4 @O–CN/PMS system can remove 99.1% BPA and achieve 52.6% mineralization under optimized conditions. Thus, this study not only sheds light on the tailored design of heterogeneous catalyst for organics removal and elucidates the interfacial catalytic mechanisms for PMS activation .
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MARINE POLLUTION BULLETIN
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2022
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IF 7.001
Wang Li,Bo Zu,Qingwei Yang,Junwen An,Jiawen Li
Nanoplastics (NPs) are widely found in the environment and can act as a vector for various toxic substances and promote their diffusion and bioenrichment, but the underlying mechanisms are largely unknown. Here, the adsorption characteristics of bisphenol A (BPA) onto NPs were explored. The results show that the adsorption of BPA on NPs was dominated by saturated single-layer adsorption and affected by both intra-particle diffusion and liquid film diffusion. Electrostatic interaction, π–π interaction, and hydrophobic effects played key roles in adsorption. In addition, the introduction of electrolytes inhibited the adsorption of BPA onto NPs. Interestingly, the introduction of suspended sediment promoted the formation of heterogeneous aggregates of NPs-SS, thereby reducing the adsorption capacity, indicating that aggregation may play an important role in the adsorption behavior of NPs. Overall, our results provide new insights into the adsorption behavior of BPA on NPs and the underlying mechanisms under different environmental conditions.
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JOURNAL OF CHROMATOGRAPHY A
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2022
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IF 4.601
Yang Feng,Min Sun,Mingxia Sun,Jiaqing Feng,Haili Sun,Juanjuan Feng
Polyamidoamine dendrimers with different generations (G1-G5) were synthesized in situ on silica progressively via Michael addition and amidation reactions. A sequence of materials was characterized by elemental analysis and Brunauer-Emmett-Teller test, the content of each element (C, H and N) was increased but the surface area was reduced gradually from G1 to G5. These materials were separately packed in a stainless steel column (10 × 4.0 mm, i.d.) for SPE . These SPE columns were combined with high performance liquid chromatography (HPLC) to establish an online SPE-HPLC analysis. According to the chemical structures of materials, polycyclic aromatic hydrocarbons (PAHs) and bisphenols as model analytes were selected to investigate the extraction performance and the extraction mechanism, so as to reveal the extraction performance-structure relationship of G1-G5. The extraction performance was improved with the increase of functional groups from G1 to G4 or G5, the hydrophobic effect played main role accompanied with possible weak hydrophilic, hydrogen-bonding and electrostatic interactions in extraction mechanism. The adsorption capacity, enrichment factor, partition coefficient and extraction efficiency for PAHs and bisphenols reached to 17.52 µg g −1 and 2.70 µg g −1 , 5353 and 3002, 5066 and 1197, and 90.09% and 60.05% respectively. Compared with commercial SPE materials, these dendrimer-grafted silica materials were inferior to C18, but better than silica. Furthermore, the G4 and G5 were separately selected to develop two online SPE-HPLC analytical methods for determining trace PAHs and bisphenols in real water samples, and satisfactory results were obtained.
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Additive Manufacturing
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2022
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IF 11.632
Qinfei Xu,Wenhan Xu,Yang Yang,Xin Yin,Chenyi Zhou,Jinxuan Han,Xuefeng Li,Yingshuang Shang,Haibo Zhang
3D printed poly (ether ether ketone) (PEEK) parts have attracted considerable attention in the automotive, medical, and aerospace fields in the past two decades. However, the major obstacle to its further application is weak interlayer strength and severe mechanical anisotropy. Herein, amorphous poly (aryl ether ketone) (aPAEK) was designed as an interlayer reinforcement modifier to strengthen the interlayer strength and reduce mechanical anisotropy of 3D printed PEEK parts. By introducing 7 wt% aPAEK in PEEK filaments, the interlayer strength in 3D printed parts increased 130% from pristine PEEK to aPAEK/PEEK blends. The mechanical anisotropy in the XY plane was reduced to 1.1%, and its X-axis and Y-axis tensile strength still reached 89.2 ± 3.3 MPa and 88.1 ± 4.1 MPa, respectively. We demonstrate that these performance enhancements were due to the diffusion and entanglement of aPAEK between the layers. These remarkable results significantly improve the comprehensive mechanical properties of 3D printed PEEK parts, and expand its high-performance applications. This work also yields new insight into the development strategy of additive manufacturing materials by blending.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Menghan Sun,Liangzhi Zou,Pengcheng Wang,Xinfei Fan,Zonglin Pan,Yanming Liu,Chengwen Song
Fenton , a conventional technology , has been widely employed for wastewater purification, but it still suffers from the unsatisfactory capability for pollutants degradation . Herein, a membrane-based Fenton process was proposed by immobilizing nano zero valent iron (NZVI) in a CNT membrane (Fe 0 -CNT catalytic membrane) for accelerating pollutants degradation efficiency. It realizes a promotion on·OH generation rate from H 2 O 2 catalyzed by NZVI catalyst owing to the cycle of between ferrous and ferric ions during the Fenton process. Meanwhile, mass transfer improvement can be achieved due to the liquid convection in the membrane pore via the flow-through process. As a result, the Fe 0 -CNT catalytic membrane presented a high removal efficiency of 98% for bisphenol A (BPA) under an optimum operation condition. Also, the prepared Fe 0 -CNT catalytic membrane showed excellent degradation efficiency for other organic contaminants , such as phenol (80.6%), sulfamethoxazole (SMX, 95.5%) and paracetamol (ACM, 84.1%). Furthermore, the environmental factors (various of anion ions, such as Cl - , HCO 3 - and NO 3 - and natural organic matter) presented negligible influences on organic pollutants degradation via Fe 0 -CNT catalytic membrane, suggesting a good potential for factual wastewater treatment application. Based on the results, this work introduces a novel insight into the design of highly efficient Fenton process using membrane-based catalyst for pollution abatement .
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 17
·8203-8214
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IF 3.925
Lingli Zhang,Han Tao,Chun Ji,Qiaoling Wu,Xiao Wang,Yuangeng Wu
As an alternative to bisphenol A (BPA), bisphenol S (BPS) is widely used in many consumer goods and industrial products. However, BPS has similar genotoxic, reproductive and endocrine disrupting effects to BPA and can enter the body through the food chain or by dermal absorption to endanger human health. This paper presents a rapid and direct electrochemical sensing technique for ultra-trace BPS determination on the basis of the signal amplification of the 1T phase & 2H phase hybrid MoS2 nanosheets (1T&2H-MoS2) and amino-functionalized carbon nanotube (CNTs-NH2) composites. The cooperative electrocatalytic effect and high-electrically active surface area of 1T&2H-MoS2/CNTs-NH2 composites not only facilitated the electron transfer between BPS and the electrode, but also promoted the adsorption of BPS on the electrode. Hence, the 1T&2H-MoS2/CNTs-NH2 modified electrode exhibited excellent electrocatalytic activity with a lower oxidation potential and higher peak current for BPS. Under the optimized conditions, the peak current response of BPS showed a good dose-dependent relationship with its concentration in the range of 0.02–1.0 μM and 1.0–70.0 μM, while the detection limit was as low as 8.6 nM. The proposed method was used to determine BPS in the mineral water bottle and orange juice samples with satisfactory spiked recoveries between 92.31% and 104.20%, demonstrating its reliability and practicality in real sample analysis. Furthermore, the sensing method has the characteristics of facile electrode fabrication, fast response (<4 min) and good reproducibility.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Chuangjian Su,Ruhong Li,Chaolin Li,Wenhui Wang
The application of promising persulfate-based advanced oxidation processes (AOPs) for environment remediation is limited by the poor charge separation and the sluggish kinetic for active centers regeneration of the catalysts. Piezocatalytic activation has been proposed to solve the above concern recently, but little is known on its mechanism. Herein, novel piezocatalyst Bi 2 Fe 4 O 9 nanosheets (BFO NSs) are demonstrated to significantly improve peroxydisulfate (PDS) activation efficiency via piezocatalysis, resulting SO 4 •− and •OH as the dominant active species for organic pollutants degradation. Further DFT calculations and experimental investigations confirm that the Fe 2+ in BFO NSs as active sites donate electrons for PDS to generate SO 4 •− , and simultaneously that the piezo-electrons can accelerate the regeneration of Fe 2+ , thus leading to the superior catalytic activity. This work provides atomic-scale insights of catalytic sites and mechanisms of piezocatalytic PDS activation and may inspire the development of more efficient piezocatalysts and AOPs.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Yuanxi Huang,Lingjun Bu,Yangtao Wu,Shumin Zhu,Shiqing Zhou,Zhou Shi,Dionysios D. Dionysiou
UV/sodium percarbonate (UV/SPC) advanced oxidation process is an efficient and green technology to remove contaminants of emerging concern (CECs), with the simultaneous formation of hydroxyl radical ( • OH) and carbonate radical (CO 3 •− ). This study investigated the degradation of eight CECs in UV/SPC process, including phenol, atrazine, bisphenol A, ibuprofen, sulfadiazine, acetaminophen, carbamazepine, and diuron. A model was established to simulate the experimental results, which shows that both • OH and CO 3 •− played crucial roles in UV/SPC process, and the steady-state concentrations of CO 3 •− were much higher than that of • OH. The higher concentration compensates for the low reactivity of CO 3 •− with CECs and the loss of • OH depleting by CO 3 •− . Also, the Hammett constants decreased linearly with increasing natural logarithms of rate constants, indicating the selectivity of CO 3 •− with electron-donating substituents. In real water, CEC degradation was significantly inhibited due to the competition for light absorption from background compounds and scavenging of free radicals, especially CO 3 •− , by water matrix. Further, demethylation, decarbonylation, hydroxylation, amino oxidation, and quinonization were proposed as the main reactions for CEC degradation in UV/SPC process. The minimum electrical energy per order (EE/O) was calculated as 0.152 kWh m −3 , with SPC dose of 0.138 mM and UV intensity of 2.02 × 10 -7 Einstein L −1 s −1 .
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Wenchao Jia,Xiangying Jin,Yuhua Wu,Danping Xie,Wenhua Yin,Bo Zhao,Zhonghui Huang,Lijun Liu,Yanyan Yang,Tonghui Cao,Xidan Feng,Sheng Chang
Here, we report a novel aptasensor based on decahedral silver nanoparticles (Ag 10 NPs) enhanced fluorescence polarization (FP) for detecting PCB-77. Using aptamer modified Ag 10 NPs hybridized with DNA sequence labeled fluorescent group as an analytical probe, polychlorinated biphenyls (PCB-77) could be detected with high sensitivity and selectivity. The linear range of determination was 0.02 ng/L to 390 ng/L and the limit of detection was 5 pg/L. In addition, through the optimization of the experiment condition and signal probe DNA (pDNA), we found that the maximum FP signal could be generated when the distance between fluorescein and the surface of Ag 10 NPs was 3 nm. When the aptamer was immobilized on the surface of Ag 10 NPs could be strengthened the anti-interference performance of aptamer nanoprobe and further improved the detection ability. At the same time, we also compared the detection performance of the traditional FP signal enhancer streptavidin (SA) analysis system. The fluorescence polarization aptasensor could detect PCB-77 samples efficiently in complex environmental water, which shows a good application prospect.
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Wenjun Zhu,Sylvestre Ndayiragije,Xiaohua Zuo,Xiaofei Zhang,Guanghui Wang,Xiaobo Wang
Single-atom Cu and N co-coordinated porous carbon (Cu-N-C) was synthesized by hydrothermal-calcination using zinc zeolite imidazole frameworks (ZIF-8) as the precursor. The catalyst showed excellent adsorption and catalytic ability due to the ideally-dispersed single atomic copper sites and the unique nitrogen-doped porous carbon. The complete removal of sulfamethoxazole (SMX, 18 mg/L) could be achieved within 40 min of pre-adsorption and 25 min of oxidative degradation in the present of peroxymonosulfate (PMS). The adsorption capacity of Cu-N-C (0.2 g/L) was evaluated to be 58.69 mg/g. The apparent degradation rate constant ( k ) of SMX on Cu-N-C was 0.155 min -1 , which was 14.1 times faster than that on N-C (0.011 min -1 ). From the activation mechanism, it was found that CuN units acted as the main active sites in Cu-N-C for PMS activation . EPR analysis and quenching experiments verified that the reactive oxygen species (ROSs) of SO 4 · - and 1 O 2 were involved in the decomposition and mineralization of SMX. This work provides a new perspective for the development of Fenton-like single-atom catalysts.
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