Journal of Cleaner Production
·
2023
·
IF 11.1
Hao Cheng,Xinyan Li,Chao Huang,Jian Zhu,Ping Wang,Heng Cao,Chongling Feng,Dingxun Ling,Hao Liu,Min Cheng
Commercial molybdenum carbide (Mo 2 C) and ferrous iron (Fe 2+ ) were investigated for the first time to co-catalyze the activation of H 2 O 2 for the treatment of organic contaminants . Compared with traditional Fenton process, the presence of Mo 2 C decomposed hydrogen peroxide (H 2 O 2 ) more effectively and accelerated the conversion of Fe 3+ /Fe 2+ . The Rhodamine B (RhB) degradation rate constant in Mo 2 C/Fe 2+ /H 2 O 2 reached appropriately three times that in Fe 2+ /H 2 O 2 , and the co-catalytic reactivity of Mo 2 C was significantly higher than that of MoS 2 . In addition, Mo 2 C/Fe 2+ /H 2 O 2 exhibited a board effective pH range of 2.8–8.8, and four-cycle experiments confirmed the stability and reusability of Mo 2 C. The results of X-ray photoelectron spectroscopy (XPS) indicated that Mo(Ⅱ) and Mo(IV) played major roles in Fe 3+ reduction. Electron Paramagnetic Resonance analysis and quenching experiments demonstrated that hydroxyl radical (·OH), superoxide anion radical (O 2 − ) and singlet oxygen radical ( 1 O 2 ) were all involved in Mo 2 C/Fe 2+ /H 2 O 2 . Particularly, Mo 2 C/Fe 2+ /H 2 O 2 significantly enhanced the generation of ·OH and 1 O 2 in comparison to Fe 2+ /H 2 O 2 . Moreover, toxicity assessment analysis by ECOSAR suggested that the toxicity of most degradation products of RhB decreased after treatment. Overall, this study offers a promising Mo 2 C co-catalyzed Fenton process for rapid and efficient abatement of organic contaminants.
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CHEMOSPHERE
·
2023
·
IF 8.8
Xiaojun Lai,Nuoyi Huang,Xiaohua Zhao,Yang Li,Yao He,Jiesen Li,Jinhuan Deng,Xun-an Ning
Aromatic amines (AAs), a characteristic pollutant with electron-donating groups in textile industry , having high reactivity with reactive chlorine free radicals, is probably the precursor of chlorinated aromatic products in advanced oxidation treatment . In this study, Fe2+/peroxydisulfate (PDS)/Cl- and Fe2+/H2O2/Cl-systems were used to treat four kinds of AAs (5-Nitro-o-toluidine (NT), 4-Aminoazobenzol (AAB), O-Aminoazotoluene (OAAT), 4,4′-Methylene-bis(2-chloroaniline) (MBCA)) in simulated wastewater, and the selectivity of various reactive species to AAs, the oxidation law and pathway of AAs were explored. The results showed that dichloride anion radical (Cl2·-) could effectively oxidize four AAs, and chlorine radical (·Cl) was strongly reactive to AAB and MBCA, especially MBCA. The largest f – (Fukui function) of MBCA is 0.0822, which is the lowest of the four AAs, so ·Cl might be more sensitive to electrophilic point than hydroxyl radical (·OH). The oxidation pathway of NT and MBCA showed that ·Cl mainly played the role of electron transfer to AAs instead of generating chlorinated products, but the addition of ·OH to –NH2 generated aromatic nitro compounds with higher toxicity than NT and MBCA. Therefore, the electron transfer of ·Cl and Cl2·- could not only improve the removal of AAs but also reduce the generation of toxic products. This study found that the reactivity of reactive chlorine free radicals was not necessarily related to chlorination, which provided a theoretical basis for the further studies into the formation mechanism of chlorination products.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Zhenyu Shen,Zhexin Zhu,Gangqiang Wang,Zhendong Wang,Wenxing Chen,Wangyang Lu
It is of great significance for improving the electron transmission performance of graphite phase carbon nitride (g-C 3 N 4 ) by an economical method. Herein, urea was mixed with tourmaline (TM) and calcined to obtain g-C 3 N 4 /TM composite photocatalyst . Under solar light, g-C 3 N 4 /TM activated peroxymonosulfate (PMS) to degrade carbamazepine (CBZ) entirely within 25 min. g-C 3 N 4 /TM had a superior photocatalytic oxidation performance under solar light than g-C 3 N 4 . Photogenerated electron-hole pairs of g-C 3 N 4 were efficaciously suppressed, originating from the more excellent electronic transfer to TM. Four active species, including SO 4 • - , •OH, 1 O 2 , and O 2 • - , were identified for the degradation of CBZ. Ten intermediates of CBZ and six intermediates of sulfaquinoxaline sodium (SQXNa) were determined by using ultra-performance liquid chromatography coupled with a high definition mass spectrometer (UPLC-HDMS), and a degradation pathway was proposed. As the reaction progressed, all aromatic nuclear intermediates were mineralized. The degradation of other organic pollutants by the g-C 3 N 4 /TM/PMS system validated the universal adaptability in practical applications. This research provided an effective way to improve the g-C 3 N 4 photocatalytic activity in wastewater treatment.
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CHEMOSPHERE
·
2022
·
IF 8.943
Xuesong Ye,Zhencheng Ge,Qiliang Xiao,Bohan Liu,Meng Chen,Fangmin Wu,Jun Nan
In remote areas, low-pressure ultrafiltration membrane (LPM) systems can be applied in decentralized water supplies for the treatment of groundwater containing Fe 2+ , Mn 2+ , and NH 4 + . However, improving the performance of the LPM systems, such as the stable flux and removal capacity, presents a challenge. In this study, a novel opposite-flow low-pressure ultrafiltration membrane (O-LPM) system was applied, and its performance was evaluated. Experimental results showed that after 46 days of operation, the steady flux of the O-LPM systems were 1.87-fold and 1.74-fold higher than that of the conventional D-LPM systems under Mn 2+ concentration of 0.3 mg L −1 and 1.5 mg L −1 , respectively. With a mixed pollutant system containing Fe 2+ (0.5 mg L −1 ), Mn 2+ (0.3 mg L −1 ), and NH 4 + (1.0 mg L −1 ), the O-LPM-ripening period for Mn 2+ removal was shortened from 16 days to 8 days, and the NH 4 + removal efficiency was increased from 61.46% to 80.97%. The bio-cake layer in the O-LPM systems was thinner and had a higher uniformity than in the D-LPM systems, resulting in a larger stable flux range. The relative abundance of functional bacteria (MnOB, IOB, and NOB) was generally higher in O-LPM systems than in the D-LPM systems. Overall, these results are of high relevance for groundwater treatment in remote areas, providing guidance for the widespread application of the O-LPM system in decentralized water supplies.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Yu Liu,Yanan Cao,Cong Zhang,Cheng Ye,Qinglai Bian,Xue Cheng,Hui Xia,Junping Zheng,Hongtao Liu
The inhibition of hydrogen peroxide (H 2 O 2 ) on the cysteine-mediated aggregation of gold nanoparticles (AuNPs) has great potential to rapidly visualize H 2 O 2 and disease-associated biomarkers. However, associated applications have been rigid due to the low cysteine-oxidation efficiency or the insufficient interference-resistance of previous catalysts. Here, we proposed a novel AuNPs colorimetric method termed Fe 2+ -catalyzed H 2 O 2 -preventing aggregation of AuNPs by oxidizing Cysteine (FeHOAuC) for the visible and rapid detection of H 2 O 2 with high specificity. Formed Fe 2+ -cysteine composites in the beginning, Fe 2+ accelerates the oxidation of cysteine by H 2 O 2 with an intramolecular electron-transferring model, and the generated cysteine oxides (including cysteic acid or cystine , dependent on the ratio of cysteine to H 2 O 2 molecules) lose the pro-aggregation effect on AuNPs. Notably, FeHOAuC can quantify 2–30 μM of H 2 O 2 within 5 min, and the monitoring process works well with tolerance to the impact of dissolved oxygen. The FeHOAuC paired with lactate oxidase was successfully used for measuring lactic acids in real sweat samples with a practicable detection window (2–60 μM) and a low variable coefficient (<10%). In summary, FeHOAuC is a feasible platform for rapid and convenient detection of H 2 O 2 and oxidase-specific substrates.
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Water
·
2023
·Vol. 15
·期 10
·1931
·
IF 3.4
Runjuan Zhou,Kuo Zhang,Ming Zhang
A back-propagation neural network (BPNN) was used to model and optimize the process of hydroxylamine (HA)-enhanced Fe2+activating peroxymonosulfate (PMS). Using HA-enhanced Fe2+to activate PMS is a cost-effective method to degrade orange II (AO7). We investigated the individual and interactive effects of the concentrations of Fe2+, HA, and PMS on the degradation of AO7. TheR2of the BPNN model was 0.99852, and the data were distributed aroundy=x. Sensitivity analysis showed that the relative importance of each factor was as follows: HA > Fe2+> PMS. The optimized results obtained by the genetic algorithm were as follows: the concentration of Fe2+was 35.33 μmol·L−1, HA was 0.46 mmol·L−1, and PMS was 0.93 mmol·L−1. Experiments verified that the AO7 degradation effect within 5 min was 95.7%, whereas the predicted value by the BPNN was 96.2%. The difference between predicted and experimental values is 0.5%. This study provides a new tool (machine learning) to accurately predict the concentrations of HA, Fe2+, and PMS to degrade AO7 under various conditions.Keywords:advanced oxidation process;machine learning;BPNN;sensitivity analysis;genetic algorithm
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Deng Pan,Gaoyuan Ren,Jingwei Zhang,Li Wang,Shudong Wang
The effects of dicarboxylic acids (oxalic acid, malonic acid and succinic acid) on the H 2 O 2 stability during tungsten (W) chemical mechanical planarization (CMP) process were studied for the first time. The dicarboxylic acids can coordinate with Fe 3+ in the slurry and impact the reaction process by blocking the interaction between H 2 O 2 molecule and Fe 3+ , decreasing the Fe-complex redox potential and promoting the reduction of Fe 3+ to Fe 2+ . Among the three dicarboxylic acids, oxalic acid shows the superior coordination ability with Fe 3+ , resulting in a significant improvement of H 2 O 2 stability in the slurry. Appropriate amount of oxalic acid can improve the wafer surface quality (Ra=1.435 nm) while keeping the high material removal rate (MRR = 917 Å/min) at the same time. An increasing amount of dicarboxylic acids can result in a high degree of coordination between Fe 3+ and dicarboxylic acid in the slurry. The results also indicate that the main reaction path from Fe 3+ to Fe 2+ in this system is the reaction between Fe 3+ and H 2 O 2 . Meanwhile, the MRR keeps almost unchanged after one-week storage with the 2:1 mol ratio of oxalic acid to Fe 3+ .
研究领域:
材料科学
·
化学工程
·
半导体制造
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Jiaqi He,Jianlin Sun,Yanan Meng,Huajie Tang,Ping Wu
Nanofluids containing nanocomposite materials have broad application prospect in lubrication . In the present study, MoS 2 -Al 2 O 3 nanocomposite was synthesized by solvothermal method . Then water-based nanofluid containing MoS 2 -Al 2 O 3 nanoparticles was prepared and it exhibited optimal stability and wettability . The tribological properties of MoS 2 -Al 2 O 3 nanofluid under steel/steel contact were investigated. Through chemical analysis of worn surface, tribochemical reactions occurred and tribofilm generated at friction interface were studied to reveal the lubrication mechanism. The results showed that MoS 2 -Al 2 O 3 nanofluid exhibited outstanding effect on reducing the friction force and wear rate of friction pairs. The superior lubrication performance was partly attributed to the entry and movement of nanoparticles at friction interface. More importantly, due to interfacial tribochemistry , a tribofilm with double layer structure composed of adsorption film and reaction layer was formed on the metal surface , preventing the direct contact of steel surfaces. The adsorption film with a thickness of about 16 nm was predominated by amorphous substrates and crystal phases (ultrafine Al 2 O 3 and MoS 2 debris) embedded in the top. And the reaction layer beneath adsorption film contained high mechanical properties iron oxides (mainly Fe 3 O 4 and Fe 2 O 3 ) and self-lubricating Fe 2 (SO 4 ) 3 , which further alleviated friction and enhanced the wear-resistance of materials.
研究领域:
材料科学
·
摩擦学
·
化学工程
·
机械工程
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Petroleum Science
·
2016
·Vol. 14
·期 1
·195-202
·
IF 0.901
Chen Shi-Jia,Chen Bin,Zhu Hong-Qing,Wang Cheng-Sheng,Wu Xiao-Yan,Lv Peng
The influence of emulsified oil, suspended solids, Fe 3+ , Fe 2+ , cationic water clarifier and sulfate-reducing (SR) bacteria on the aggregation behavior of residual hydrophobic modified polyacrylamide in treated oily wastewater from polymer flooding was studied by fluorescence spectroscopy and dynamic light scattering. The result of I
1
/I
3 showed that the polarity of hydrophobic microdomains increased, whereas the size of the hydrophobic microdomains may be decreased, where the value of I
1
/I
3 represents the ratio of the intensity of peak I
1 (374.0 nm) to that of peak I
3 (385.0 nm) of the vibration fine structure of pyrene monomer emission in residual polymer solution. The results of the ratio of I
1 at 48 h to I
1 at 0 h ( I
1,48h
/I
1,0h ) indicated that oil and cationic water clarifier could inhibit the aggregation to some extent, while Fe 2+ and suspended solids were helpful for aggregation, and Fe 3+ and SR bacteria had no significant influence on the aggregation of polymer.
研究领域:
环境科学
·
生物化学
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MOLECULES
·
2016
·Vol. 21
·期 5
·604
·
IF 2.465
Xican Li,Jingjing Liu,Jian Lin,Tingting Wang,Jieyuan Huang,Yongqiang Lin,Dongfeng Chen
As a natural flavonoid inAmpelopsis grossedentata, dihydromyricetin (DHM,2R,3R-3,5,7,3′,4′,5′-hexahydroxy-2,3-dihydroflavonol) was observed to increase the viability of •OH-treated mesenchymal stem cells using a MTT [3-(4,5-dimethylthiazol-2-yl)-2,5-diphenyl] assay and flow cytometry analysis. This protective effect indicates DHM may be a beneficial agent for cell transplantation therapy. Mechanistic chemistry studies indicated that compared with myricetin, DHM was less effective at ABTS+• (2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid radical) scavenging and reducing Cu2+, and had higher •O2−and DPPH• (1,1-diphenyl-2-picrylhydrazyl radical) scavenging activities. Additionally, DHM could also chelate Fe2+to give an absorption maximum at 589 nm. Hence, such protective effect of DHM may arise from its antioxidant activities which are thought to occur via direct radical-scavenging and Fe2+-chelation. Direct radical-scavenging involves an electron transfer (ET) pathway. The hydrogenation of the 2,3-double bond is hypothesized to reduce the ET process by blocking the formation of a larger π-π conjugative system. The glycosidation of the 3–OH in myricitrin is assumed to sterically hinder atom transfer in the •O2−and DPPH• radical-scavenging processes. In DHM, the Fe2+-chelating effect can actually be attributed to the 5,3′,4′,5′–OH and 4–C=O groups, and the 3–OH group itself can neither scavenge radicals nor chelate metal.Keywords:dihydromyricetin;mesenchymal stem cells;antioxidant mechanisms;hydroxyl radical-induced;Fe2+-chelation;3–OH group;2,3-double bond;electron transfer (ET) pathway
研究领域:
药理学
·
细胞生物学
·
化学
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Jiaqiao Yuan,Hongyu Lu,Xiang Gong,Mingjun Chen,Hao Lai,Shuming Wen,Shaojun Bai,Dandan Wu
The development of high-efficiency beneficiation processes for ilmenite has garnered widespread attention. This study proposed the utilize of a heterogeneous Fenton catalytic technology involving H 2 O 2 and Fe 2+ to enhance ilmenite flotation. The flotation results indicated that pre-oxidation of ilmenite with H 2 O 2 -Fe 2+ before adding collector could recover over 80 % of ilmenite from titanaugite. Electron Paramagnetic Resonance and slurry iron component concentration analyses revealed that the •OH generated within the ilmenite-H 2 O 2 -Fe 2+ catalytic system could oxidize Fe 2+ to Fe 3+ . The stronger binding capability of Fe 3+ with NaOL led to a remarkable discrepancy in floatability between ilmenite and titanaugite. Zeta potential analysis further confirmed that the oxidation degree of the ilmenite surface and the adsorption of iron species were higher than those of titanaugite. Additionally, Time-of-Flight Secondary Ion Mass Spectrometry and X-ray photoelectron spectroscopy analyses provided evidence for the selective activation of ilmenite by the H 2 O 2 -Fe 2+ . Furthermore, Density Functional Theory calculations revealed that the stable adsorption of Fe 2+ and Fe(OH) 2 + offered additional active sites on the ilmenite surface for NaOL adsorption. Moreover, the adsorption of •OH significantly affected the electronic spin density of the Fe 3d orbitals of Fe atom in ilmenite, and played a crucial positive in the surface activity of ilmenite.
研究领域:
矿物加工工程
·
化学工程
·
材料科学
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Wenjun Gong,Yating Pang,Chenyu Wang,Wenming Wang,Hong-Fei Wang
The dinitrosyl iron complex (DNIC) is a ubiquitous functional brick often used as a vehicle for the NO radical and chelatable iron pool, with a key role in chemical and biomedical applications. In this work, four DNICs modified with different thiolate bridging ligands (–SL) were synthesized. These complexes were characterized by 1H-NMR, electrospray ionization mass spectrometry, and X-ray crystal diffraction. Photoinduced NO release from the complexes in solution was further explored by time-resolved infrared and time-resolved electron paramagnetic resonance (EPR) spectra. The cluster complexes showed relatively lower cytotoxicity against the normal human liver cell line HL-7702 and higher cytotoxicity against human cervical cancer cells, with a selectivity index of 2.4–4.8. The cluster complexes with different L groups had different rates of NO release and protein binding constants. Moreover, NO released upon photoirradiation entered living cells, which were successfully imaged using an NO-selective fluorescent probe. The ferritin complex adducts further enhanced the cytotoxicity and cellular fluorescent intensity of NO, and the crystal structure revealed the coordination of the Fe(SL)2 unit with Cys102 of ferritin. This study provides insight into the photodynamic mechanism of nitrosyl iron−sulfur clusters to understand their physiological activity.
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