APPLIED SURFACE SCIENCE
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2023
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IF 6.7
Boxuan Yao,Ke Zhang,Xiaoyang Liu,Hua Wei,Zihan Li,Jiarui Zhou,Guangfei Yuan,Xin Wang,Shenghong Yang,Jian Liu
Pursuing special negatively charged adsorbents is critical to selectively removing cationic pollutants from effluent. Herein, we proposed a versatile preparation strategy of negatively charged saccharide-based polymers using easily available saccharides as building blocks and hexachlorocyclotriphosphazene as a linker in a facile “one-step” method. Because of the existence of numerous hydroxyl groups and phosphine nitrile units in the skeleton, these polymers show selective adsorption capacity towards cationic dyes and pharmaceuticals, but not for ionic dyes and uncharged bisphenol A. Notably, β-cyclodextrin-based polymers (β-CDPs) displayed remarkable adsorption towards methylene blue (Q m , 1563 mg g −1 ) and promethazine (Q m , 944 mg g −1 ). Systematic experiments revealed that the synergy of “host-guest” inclusion, electrostatic attraction, and π-π interaction promoted the selective and efficient adsorption of cationic pollutants. Given the efficiently selective adsorption of cationic dyes and pharmaceuticals, these negatively charged saccharide-based polymers should be candidates for the adsorption of other cationic pollutants, including heavy metal ions. This work expanded the scope of the special utilization of biomass-based adsorbents for water remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
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IF 9.136
Yang Li,Yihao Jing,Yiguo Zhao,Wentao Li,Jing Li,Yuqing Song,Yue Yang,Tingting Feng,Gen Peng,Zhenpeng Huang,Ting Yang,Qi Zhou
In this study, novel Co-embedded hollow N -doped carbon polyhedrons, derived from ZIF-8@ZIF-67 core–shell structure, were synthesized and used for activating peroxymonosulfate (PMS) towards efficient bisphenol A (BPA) degradation. The contents of different N species, especially Co-N x and graphitic N sites, were tuned by different calcination temperatures (800, 900, and 1000 °C). Characterization results demonstrated that hollow polyhedron with high graphitization degree and abundant porosity anchored numerous Co nanoparticles, which could enhance the catalytic performance. Compared to other as-prepared catalysts, Co/HNCP-900 (pyrolyzed at 900 °C) showed a more outstanding performance of PMS activation towards BPA degradation, and 95.1 % of BPA (20 mg/L) could be removed within 3 min. Abundant Co-N x sites were a critical factor to induce the reaction process. Based on trapping, radical scavenger, and electrochemical analysis experiments, a nonradical process (singlet oxygen and direct electron transfer) was proposed to play the dominant role in BPA degradation. Benefiting from the nonradical process, BPA degradation efficiency almost remained stable either in a wide pH range (2.5–8.0) or in the presence of coexisting ions and natural organic matter. The findings of this study will elucidate a new opportunity for improving environmental remediation.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Da Ouyang,Ronghao Wu,Zhaojun Xu,Xiaomin Zhu,Yimin Cai,Ruihuan Chen,Changyin Zhu,Damià Barceló,Haibo Zhang
Advanced oxidation processes (AOPs) based on persulfate (PDS) activation by iron materials have attracted significant attention due to their high organic pollution removal efficiency and relatively low remediation costs. However, one of the iron-based materials’ shortcomings is the weak activation ability of Fe 3+ on PDS and the low sustainability of Fe 2+ in the oxidation environment. In this study, biochar-supported molybdenum dioxide (MoO 2 @BC) was employed as a co-catalyst to enhance the Fe 3+ based PDS activation for Bisphenol A (BPA) degradation. Results showed that >96 % of BPA was removed during 60 min, and the BPA degradation efficiencies only slightly decreased after four reuses of MoO 2 @BC. Electron paramagnetic resonance (EPR) analysis and quenching experiments indicated that reactive oxidation species (ROSs) contributing to the degradation of BPA were SO 4 − , OH and 1 O 2 . Besides, it was found that biochar supporting favours the adsorption of Fe 3+ on the MoO 2 surface and promotes the electron transfer from Mo(IV) to Fe 3+ based on the combination of X-ray photoelectron spectroscopy (XPS) analysis, electrochemical tests and density functional theory calculation (DFT). This work provides a new insight for enhancing the performance of organic contaminants degradation through AOPs based on persulfate activation by iron material.
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DESALINATION
·
2022
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IF 11.211
Xiaoxiang Cheng,Cunxian Lai,Xuewu Zhu,Senlin Shao,Jingtao Xu,Fengxia Zhang,Jialin Song,Daoji Wu,Heng Liang,Xinsheng Luo
Nanofiltration (NF) membranes featuring high water permeance , excellent antifouling properties, and selective organic matter/minerals separation for drinking water are highly desirable in the environmental water treatment process. In this work, an ultra-permeable NF membrane was tailored via a low temperature-assisted interfacial polymerization (LTIP) method. The surface morphologies , structural compositions, and separation performances of the NF membranes were further regulated by changing the addition of the aqueous monomer . The optimized NF membrane (NFM-0.2) showed ultrahigh water permeance of 31.8 L m −2 h −1 bar −1 and 95.1 % Na 2 SO 4 rejection while maintaining superior antifouling behaviors. During the filtration of natural surface water, NFM-0.2 presented 75.5 % higher removals of DOC , UV 254 , and bisphenol A. The application of NFM-0.2 for filtrating ground water indicated that NFM-0.2 could remove 50.0 % and 62.9 % of organic matter and total hardness, respectively. The permeate water not only had no potential to form scaling after boiling but also preserved mineral ions, which was helpful for providing high-quality drinking water. Combined with the feasibility and practicability of the LTIP method, the facile strategy provides a facile way for tailoring ultralow pressure NF membranes featuring both highly selective separation of organic matter/minerals and superior antifouling abilities for practical water treatment.
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MICROCHIMICA ACTA
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2022
·Vol. 189
·期 12
·1-10
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IF 6.408
Sun Min,Wang Xiuqin,Ding Yali,Feng Juanjuan
In order to improve the selectivity and stability of melamine–formaldehyde (MF) aerogel, it was composited with TiO 2 aerogel. A TiO 2 -MF hybrid aerogel was in situ prepared on the surface of carbon fibers for in-tube solid-phase microextraction (SPME). The extraction performance of TiO 2 -MF aerogel was regulated by changing the ratio of TiO 2 sol and MF sol during the material preparation. Coupled with high-performance liquid chromatography-diode array detection (HPLC–DAD), the extraction tube filled by TiO 2 -MF aerogel-coated carbon fibers was evaluated with several types of environmental pollutants including polycyclic aromatic hydrocarbons (PAHs), estrogens, and ultraviolet filters. Because of favourable extraction performance of PAHs they were selected as model analytes, and some important influence factors were optimized for satisfactory sensitivity. The detection limits were in the range 0.05–0.10 μg L −1 , owing to high enrichment factors (653–1007). The online in-tube SPME-HPLC–DAD method was verified for the determination of trace PAHs in environmental water samples, and acceptable recovery (70–118%) was achieved. The analytical methods also displayed some advantages in comparison with other reports. Moreover, the extraction tube exhibited satisfactory chemical stability. Graphical abstract
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Limin Duan,Huihao Jiang,Wenhao Wu,Daohui Lin,Kun Yang
Introducing crystal defects into iron based metal-organic frameworks (Fe-MOFs) is regarded as a promising strategy to enhance Fenton-like performance. However, developing a facile and effective strategy to construct defective Fe-MOFs as highly efficient Fenton-like catalyst is still a challenge. Herein, MIL-100(Fe) (Def-MIL-100(Fe)) with missing ligands defects was synthesized by a simple heterogeneous reaction using zero-valent iron. The bisphenol A degradation efficiency in the Def-MIL-100(Fe)/H 2 O 2 system reached up to 91.26% within 10 min at pH 4 with a low catalyst dosage of 0.05 g/L, while the perfect MIL-100(Fe) has almost no Fenton-like performance. It was observed that missing ligands defects in the Def-MIL-100(Fe) play a key role in the Fenton-like reaction. The missing ligands defects could increase the Lewis acidity for fast H 2 O 2 adsorption and accelerate the electron transfer between Fe II and Fe III cycling, leading to faster and more·OH generation. Moreover, the missing ligands defects could promote the mass transfer for improving·OH utilization efficiency. This work provides a novel strategy to construct defective Fe-MOFs as highly efficient Fenton-like catalyst to degrade organic pollutants in water.
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Journal of Water Process Engineering
·
2023
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IF 7
Yanhui Cheng,Fukang Zheng,Huiyu Dong,Fei Pan,Lei Sun,Nevskii Aleksandr,Xiangjuan Yuan
A novel advanced oxidation technology of ozone and ferrate (ozone/Fe (VI)) was investigated and used to degrade micropollutants ( e.g. , sulfamethoxazole (SMX), diclofenac sodium (DCF)) in this study. The results demonstrated that the ozone/Fe(VI) process can rapidly and efficiently degrade SMX and DCF. The SMX and DCF degradation was substantially accelerated by increasing the Fe(VI) dosage (5 to 25 μM) or ozone concentration (10 to 52 μM), up to 77.0 % and 82.7 % of SMX and DCF were obtained, respectively. The removal efficiencies of SMX and DCF was higher in acidic conditions, and decreased from 98.4 % to 44.7 % and from 94.3 % to 62.9 %, respectively, at pH 5–9 in the presence of buffer. Besides, CO 3 2− , Cl − , and HA had a little negative effect on SMX and DCF removal, and the ozone/Fe(VI) process still obtained high degradation efficiency (>64.5 %) for SMX and DCF in real water. On the basis of the finding of scavenging and probe experiments, ozone, Fe(VI), OH , and Fe(IV)/Fe(V) species were identified as the predominant oxidants for SMX and DCF degradation. Sixteen and eighteen transformation products (TPs) of SMX and DCF in ozone/Fe(VI) process were detected by UPLC-QTOF-MS. Then, the reaction pathways of SMX and DCF were proposed by Fukui function analysis and TPs identification. Using the ECOSAR software, the ecotoxicity of SMX, DCF, and their TPs were evaluated. These findings might provide useful information and a theoretical foundation for the application of ozone/Fe(VI) process in water treatment .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Li Lin,Fangjie Zhang,Xing Hou,Linlin Wang,Weijie Wu,Longfei Wang,Yi Li,Haijiao Xie
The advanced oxidation processes based on the electro-Fenton reactions show great potentials as a wastewater treatment approach for removing emerging contaminants. In the electro-Fenton system, some factors still exist affecting the treatment efficiency, e.g., the formation of iron sludge, a narrow pH working range, and slow conversion rates between Fe 2+ and Fe 3+ . In this research, a novel heterogeneous flow-through electro-Fenton system was constructed, and carbon felt was used as the template material for the preparation of an etched carbon felt cathode loaded with zero-valent iron and iron oxide (Fe@Fe 2 O 3 /ECF) for the degradation of bisphenol A , which addressed the aforementioned issues. The Fe@Fe 2 O 3 /ECF electrode showed excellent performance across a pH range between 3 and 11, with exceptional stability and resistance to other substances in water. For the three pollutants, bisphenol A, tetracycline and ciprofloxacin, the highest degradation efficiency can reach 99.3 %. Compared to traditional electro-Fenton systems, the novel process exhibited superior performances due to synergistic effects from feasible flow design, enhanced electrochemical reactivity and greater exposure of active sites. Through electron spin resonance and free-radical quenching experiments, it was determined that the primary species participating in the heterogeneous electro-Fenton process were the hydroxyl radical and superoxide anion. Specifically, the hydroxyl radical was identified as playing a pivotal role in the degradation of bisphenol A. After a continuous operation of 240 min, the electrode showed low metal ion leaching rate and good stability, with the concentrations of leached Fe and Co ions to be only 17 and 7 μg/L, respectively. Meanwhile, the removal efficiency was only decreased by 5.7 % during the process. Through density functional theory calculation and intermediate product analysis, three potential degradation pathways were proposed, with the cleavage of carbon bonds serving as the main degradation approach. The toxicity analysis demonstrated that the intermediates were generally less toxic than BPA during treatments. This research provides a fresh means for promoting a valence state cycling of ferric species in electro-Fenton system, which has potential applications in wastewater treatment containing emerging contaminants.
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JOURNAL OF APPLIED POLYMER SCIENCE
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2023
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IF 3
Yiqing Xia,Shuai Yan,Rui Shi,Linze Liu,Junlong Zhu,Yuntao Zeng,Chen Gao,Wilfred Emori,Yuping Sheng
With the rapid development of ultra-large-scale integrated circuits and aerospace, the demand for materials with excellent overall performances is on the rise. In this study, we have successfully synthesized novel main-chain benzoxazine precursors ((BPA-AD/dd1) main ) containing both cycloaliphatic and aliphatic structures by employing adamantanediamine and Priamine 1074 for the first time, and their chemical structures and polymerization behaviors were characterized using Fourier transform infrared spectroscopy (FT-IR), NMR spectroscopy ( 1 H-NMR) and differential scanning calorimetry (DSC). The results showed that the exothermic onset of the (BPA-AD/dd1) main shifted to lower temperatures with an increasing molar ratio of Priamine 1074. Furthermore, the thermal properties, dielectric properties, surface hydrophobicity, and tensile properties of P(BPA-AD/dd1) main films were explored via dynamic mechanical analysis (DMA), thermogravimetric analysis (TGA), contact angle measuring instrument, an impedance analyzer and universal testing machine. The molar ratio of Priamine 1074 and 1,3-Bis(4-anilino)-adamantane (AD) significantly influenced the thermal properties, dielectric properties, and surface hydrophobicity of P(BPA-AD/dd1) main . P(BPA-AD 0.75) main exhibited a high T g of 296.8°C, excellent dielectric properties ( Dk = 2.58 and Df = 0.0055 @ 10 MHz), and large water contact angle as high as 105.8°, qualifying it as a potential candidate for interlayer materials in ultra-large-scale integrated circuits and resin matrix in high-performance composites.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Lianxu Wang,Zhen Lei,Sining Yun,Xiaohuan Yang,Rong Chen
Biotransformation is one of the dominant processes to remove organic micropollutants (OMPs) in wastewater treatment . However, studies on the role of molecular structure in determining the biotransformation rates of OMPs are limited. We evaluated the biotransformation of 14 OMPs belonging to different chemical classes under aerobic and anaerobic conditions , and then explored the quantitative structure-biotransformation relationships (QSBRs) of the OMPs based on biotransformation rates using valid molecular structure descriptors (electrical and physicochemical parameters). Pseudo-first-order kinetic modeling was used to fit the biotransformation rate, and only 2 of the 14 OMPs showed that the biotransformation rate constant ( k bio ) values were higher under anaerobic conditions than aerobic conditions , indicating that aerobic conditions were more favorable for biotransformation of most OMPs. QSBRs infer that the electrophilicity index (ω) is a reliable predictor for OMPs biotransformation under aerobic conditions. ω corresponds to the interaction between OMPs and microbial enzyme active sites, this process is the rate-limiting step of biotransformation. However, under anaerobic conditions the QSBR based on ω was not significant, indicating that specific functional groups may be more critical than electrophilicity. In conclusion, QSBRs can serve as alternative tools for the prediction of the biotransformation of OMPs and provide further insights into the factors that influence biotransformation.
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MATERIALS RESEARCH BULLETIN
·
2023
·
IF 5.4
Menghan Pang,Dongbo Wang,Donghuan Meng,Rongjian Qiu,Chenghua Fan,Yuyan Feng,Juncheng Han
In the present work, the flower spherical Bi 2 WO 6 /Bi 5 O 7 I S-scheme heterojunction was constructed by solution precipitation under room-temperature for photocatalytic degradation of organic pollutants and the working mechanism was investigated. As a special feature, 0.05 BWBOI performed the best photocatalytic capacity under visible light irradiation and was significantly able to degrade 98% of rhodamine B and 92% of bisphenol A in 90 min, whereas ciprofloxacin was degraded to 67% in 120 min. The composite structure was determined by XRD, FT-IR, XPS, and BET characterization, while the electron migration direction and heterojunction scheme were determined by electrochemical and ESR characterization. Eventually, addition of Bi 2 WO 6 not only broadened the light absorption range of the composites, but also achieved the successful construction with Bi 2 WO 6 /Bi 5 O 7 I of S-scheme heterojunctions to accelerate the transport rate of photogenerated carriers. Finally, the current work presents a novel bismuth-based photocatalyst and offers new ideas for the facile preparation of semiconductor heterojunctions.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lu Xu,Xiaojia Wei,Yuetong Qi,Wei Qiao,Juan Shi,Yabo Shang,Keqian Li,Xin Jin,Xue Bai,Xuan Shi,Pengkang Jin
The activation of persulfate (PS) in dissolved organic matter (DOM) solution using visible light has demonstrated potential for advanced wastewater treatment. This study presents a novel visible light-assisted homogeneous Fenton-like process (DOM-Fe 3+ -PS-Vis) for the efficient DOM degradation, based on the ligand-to-metal charge transfer (LMCT)-induced enhanced Fe 3+ reduction and PS activation. The simultaneous addition of Fe 3+ and PS to DOM-enriched solutions under visible light significantly improved PS activation, leading to the degradation of DOM and coexisting organic contaminants. The PS decomposition rate constant in the DOM-Fe 3+ -PS-Vis process was calculated to be 3.5–20.69 times higher than that of the DOM-PS-Vis, Fe 3+ -PS-Vis, and DOM-Fe 3+ -PS-Dark systems. Notably, over half of the decomposed PS in the DOM-Fe 3+ -PS-Vis process was activated by Fe 2+ generated via the LMCT between DOM and Fe 3+ . SO 4 − and OH were identified as the dominant reactive species present in the DOM-Fe 3+ -PS-Vis process with the steady-state concentration of 1.63–4.11 × 10 −13 M and 0.07 × 10 −13 M, respectively, which were 2.4–81.5 and 0.5–7 times higher than those in the DOM-PS-Vis, Fe 3+ -PS-Vis, and DOM-Fe 3+ -PS-Dark systems. Additionally, hydrophobic components with more aromatic carbon in DOM were found to promote the catalytic performance of the DOM-Fe 3+ -PS-Vis process. This study highlights the efficiency and promise of LMCT-induced enhanced Fe 3+ reduction and PS activation in DOM-enriched solutions under visible light for advanced wastewater treatment.
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