APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Pan Li,Xinbao Li,Yang Wang,Pengfei Shen,Xinbo Zhu,Yingying Zhu,Zan Wu
A low-cost, high-performance catalyst for phenol steam reforming (PSR) at low temperature was prepared by introducing waste coal ash into Co/Al 2 O 3 . The optimized content of coal ash in the catalyst were ranged from 50 to 65 wt%, presenting over 97% phenol conversion and 92% H 2 yield at low temperature of 450 °C. The stability for the best catalyst with an ash content of 50 wt% exceeded 85 h. Two-step reduction of Co 3 O 4 to Co 0 via CoO was identified by in-situ XRD. DFT calculations showed that phenol adsorption and decomposition were preferred on the FeCo bimetal surface rather than the single Co surface. H 2 O adsorption and dissociation fascinated on the CaO incorporated Al 2 O 3 surface. Both Fe and Ca in the coal ash improved the catalyst performance in PSR at low temperature. This work gives an opportunity to solve the drawbacks of high reaction-temperature and low catalyst-stability in PSR, and furthermore benefits to get a deep insight into the reaction mechanism of PSR over the catalyst.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Yaoping Guo,Keng Xuan,Yifan Li,Chenxi Pu,Zequan Zeng,Zhanggen Huang,Yadan Guo,Hao Ruan,Jiale Li
Metal-free catalysis by using carbonaceous materials has propelled to the forefront in investigation of persulfate (PS) activation for green degradation of aqueous organic pollutants . Herein, sulfur-doped porous carbons (S-AC) were feasibly produced by chemical activation of Poly (phenylene sulphide) with KOH as activator. The influences of activation time on the porous structure, sulfur doping level, and chemical functionality of the as-prepared carbons were investigated by various characterization means. The S-AC samples were employed as metal-free catalysts to activate PS for phenol removal. Experiments results demonstrated that sulfur doping enhanced the catalytic activity of S-AC, and the S-AC-2 sample prepared by carbonization activation of 2 h was demonstrated to be a promising alternative to common metal oxides and other advanced carbon-based materials. Moreover, the S-AC-2/PS system could efficiently degrade various organics, which can be a green material for wastewater treatment and environmental remediation. In addition, the effects of various reaction parameters on phenol removal were discussed. It was found that S-AC-2 still presented an outstanding performance in a wide pH range. Furthermore, the PS activation mechanism over S-AC-2 was investigated by a series of classical radical quenching tests, EPR and Linear Sweep Voltammetry .
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Chenchen Meng,Zheng Wang,Wei Zhang,Lele Cui,Bo Yang,Haijiao Xie,Zhenghua Zhang
Practical applications for the degradation of organic contaminants by conventional batch-mode heterogeneous advanced oxidation processes remain elusive due to mass-transfer limitations of short-lived reactive oxygen species (ROS). Nanoconfinement catalysis has received increasing attention because of enhanced reaction efficiency and mass and electron transfer. Here, we implemented the concept of nanoconfinement catalysis using a two-dimensional membrane. Ultrathin cobalt-copper oxide nanosheets (Co-Cu ONS) rich in active sites and oxygen vacancies were prepared through a facile solution reduction method. The assembled Co-Cu ONS membrane with active sites confined within membrane nanochannels spontaneously activates peroxymonosulfate and facilitates the generation of ROS and the redox cycles of metal cations. Therefore, an ultimate degradation efficiency (∼100%), ultrafast (∼86 ms) decomposition of organic pollutants, and excellent catalytic stability (greater than120 h) were achieved. The degradation rate is 10 3−5 times faster than the best state-of-the-art. This approach offers an attractive alternative for water purification with membrane-based nanoconfinement catalysts.
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ADVANCES IN POLYMER TECHNOLOGY
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2022
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IF 2.502
Xuefeng Lei,Junxian Ma,Kaiwen Lin,Yuehui Wang,Zengfang Huang
A type of pentaerythritol cinnamaldehyde bisphenol dicyanate ester (PCBDCy) containing oxaspirocyclic structure is well designed and synthesized in three steps from cinnamaldehyde, pentaerythritol, phenol, and cyanogen bromide. The products in each step are characterized by elemental analysis, Fourier transform infrared (FT-IR) spectroscopy, and 1H NMR spectroscopy. The mechanical properties, dielectric properties, thermostability, and water absorption of PCBDCy are investigated in detail. The results show that compared with bisphenol A dicyanate (BADCy), the PCBDCy possesses more excellent comprehensive properties. The bending strength and flexural strength are increased by 10.71% and 47.62%, respectively. The fracture toughness and are 1.5 times and 2 times of BADCy, respectively, indicating that its mechanical properties have been considerably improved. The dynamic mechanical curves indicates that the degree of phase separation is significantly reduced, the tan (δ) value representing the flexible phase is obviously shifted to the high temperature region, and the initial decomposition temperature was 12°C higher than that of BADCy, indicating that the material has excellent thermal stability. In addition, the dielectric constant and loss tangent are almost as same as those of BADCy, maintaining good dielectric properties. The water absorption rate has increased to . Compared with BADCy, its comprehensive performance is more suitable for the field of microelectronic packaging.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 29
·期 55
·83211-83219
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IF 5.19
Yin Li,Wang Juan,Shi Kaipian,Zhang Yong,Xu Ying,Kong Desheng,Ni Lixiao,Li Shiyin
The protective mechanism of extracellular polymeric substance (EPS) secreted by a harmful cyanobacteria against tannins allelochemicals was explored in this study. The binding properties of soluble EPS (SEPS) and bound EPS (BEPS) of Microcystis aeruginosa to tannic acid (TA) were investigated via fluorescence spectroscopy. The results suggested that TA interacted with the proteins in SEPS and BEPS mainly with binding constants of 5.26 and 7.93 L/mol, respectively; TA interacted with the humic acids in SEPS and BEPS mainly with binding constants of 5.12 and 5.24 L/mol, respectively. Thermodynamic experiments confirmed that the binding was mainly controlled by the hydrophobic force. Combined with Fourier transform infrared spectroscopy, it was found that the amine, carbonyl, carboxyl, and hydroxyl groups in EPS were the main functional groups contributing to the interaction of TA with EPS. The existence of EPS reduced the toxicity of TA to algal cells, with the 96 h inhibition rate of 40 mg L −1 TA on algal cells decreasing by 48.95%. The results of this study may improve our understanding of the protective mechanism of cyanobacteria against tannins allelochemicals.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Minjun Liu,Ying Liu,Xinru Liu,Chengcheng Chu,Ducheng Yao,Shun Mao
Metal organic framework (MOF)-derived materials normally have three-dimensional (3D) structure, while little attention has been paid to two-dimensional (2D) MOF-derived materials with high catalytic activity. Nevertheless, the underlying agglomeration and metal leaching issues of 2D MOF-derived catalysts hinder their real applications. In this work, we report a bimetallic nanocomposite (Ni-Fe-C-600-acid/GO) derived from 2D Ni-Fe-MOF and graphene oxide (GO) network. Employing Ni(0) and Fe 3 O 4 as active site, the Ni-Fe-C-600-acid/GO shows high efficiency in peroxydisulfate (PDS) activation for the removal of p-chloroaniline (PCA), and the catalyst/PCA dosage ratio (0.8) is substantially lower than those of the previous studies (3.9–156.9). The prepared catalysts demonstrate high catalytic activity over a wide pH range of 3–9 and maintain high efficiency after five cycles with good tolerance to inorganic anions. The singlet oxygen is identified as the predominant active species and relatively weak contributions from sulfate free radicals and hydroxyl radicals are confirmed. This catalysis system presents new insights in 2D MOF-derived catalysts in advanced oxidation processes .
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 38
·20424-20430
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IF 14.511
Xian Wei,Yubing Peng,Wangxi Fang,Zhenyu Hu,Wenwei Li,Shenxiang Zhang,Jian Jin
Water-soluble volatile organic compounds (VOCs) widely exist in wastewater and are among the most difficult-to-treat contaminants. Purification and removal of VOCs rely on energy-intensive technologies such as distillation and reverse osmosis, or less efficient approaches such as adsorption and catalytic degradation. An advanced technology that can effectively remove VOCs from water with less energy consumption is highly desired. Here, solar-driven evaporation and molecular sieving processes are integrated to remove VOCs from water where a polyaniline (PANI) nanofiber array acts as a photothermal material to evaporate water, and a polyamide (PA) layer supported by the PANI array acts as the molecular sieving layer to intercept VOCs. The PANI–PA membrane exhibits high VOC rejection and high-water evaporation rates for water containing different kinds of VOCs. When treating water containing 200 mg L−1 phenol, the phenol rejection rate is above 97% and the water evaporation rate is ∼1.0 kg m−2 h−1 under 1 sun irradiation (1 kW m−2). Moreover, the PANI–PA photothermal membrane also demonstrates superior VOC removal performance when treating complex wastewater containing acid, base or emulsified oil. The high VOC removal rate, excellent chemical stability and anti-fouling property make the PANI–PA photothermal membrane a promising material for solar-driven water remediation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Jinke Wang,Yao Huang,Lingwei Ma,Xin Guo,Shanghao Wu,Chenhao Ren,Dawei Zhang
In this work, a smart coating with corrosion-sensing and self-healing dual functions was developed on carbon steel by incorporating the urea formaldehyde (UF) microcapsules loaded with 1,10-phenanthroline (Phen) molecules. Phen as both the corrosion-sensing indicator and corrosion inhibitor was encapsulated into the UF microcapsules via the oil-water (O/W) emulsion in-situ polymerization method. When the coating was damaged, the Phen molecules released from UF/Phen microcapsules would react with the Fe 2+ ions generated from the active anodic corrosion site of the carbon steel substrate, and displayed a prominent red color chelate compound for corrosion-sensing application. During the neutral salt spray test, the corrosion evolution underneath the damaged coating can be rapidly detected within 15 min. Besides, the corrosion activity near the coating scratch can be effectively inhibited due to the adsorption of released Phen on the exposed substrate surface. After 72 h of immersion in 3.5 wt% NaCl solution, the low frequency impedance modulus of the scratched coating containing 10 wt% UF/Phen microcapsules was almost 7 times that of the scratched blank coating. The smart coating can not only achieve timely corrosion sensing, but also suppress the corrosion activity, which is of great importance for practical corrosion protection applications.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 2
·3659-3667
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IF 5.19
Zhang Xu,Shu Xin,Zhou Xiaolin,Zhou Cheng,Yang Pu,Diao Muhe,Hu Haiyang,Gan Xinyu,Zhao Chen,Fan Chunzhen
Organics and heavy metals are common pollutants in many wastewaters and water bodies. Adsorption processes by magnetic materials can rapidly remove these pollutants from water and effectively recycle adsorbent. In this study, magnetic analyzer, X-ray diffraction, Flourier transform infrared spectroscopy, and granulometry were used to characterize the synthesized magnetic reed biochar materials (ZnFe 2 O 4 /biochar). Influences of adsorption time, pH, temperature, initial solution concentration, and adsorption equilibrium concentration on adsorption performances were investigated for Cu 2+ and phenol adsorption by ZnFe 2 O 4 /biochar. Adsorption kinetic and isotherm models were used to describe the adsorption processes. Adsorption of phenol and Cu 2+ by ZnFe 2 O 4 /biochar reached saturation within 45 min and increased slightly with the increase of temperature from 15 to 45 °C. Adsorption of Cu 2+ increased with the increase of pH, while the adsorption of phenol peaked at pH = 6. The adsorption processes fit the pseudo-second order kinetics model, and both conformed to the Langmuir model. The fitting results show that the maximum single-component adsorption capacity of phenol and Cu 2+ by ZnFe 2 O 4 /biochar is 63.29 and 12.20 mg/g, and the maximum bi-component adsorption capacity reaches 40.16 and 9.48 mg/g, respectively. All the findings demonstrate that ZnFe 2 O 4 /biochar has good adsorption performance for phenol and Cu 2+ .
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TALANTA
·
2022
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IF 6.556
Hao-Fei Sun,Yuan-Yuan Cui,Chang-Qing Zhen,Cheng-Xiong Yang
Microporous organic networks (MONs) are promising in high performance liquid chromatography (HPLC) with large specific surface area, good hydrophobicity and stability. However, their superhydrophobic structures restrict MONs-based HPLC only in reversed-phase mode. To decrease the hydrophobicity of pristine MONs and to expand their broad application in HPLC, here we described the monomer-mediated fabrication of core-shell MON-2COOH@SiO 2 microspheres for reversed-phase liquid chromatography (RPLC)/hydrophilic interaction liquid chromatography (HILIC) mixed-mode chromatography for the first time. The –COOH groups were introduced into MONs’ skeleton to improve their hydrophilicity and to provide hydrophilic interaction sites. The MON-2COOH was grafted onto silica via a monomer mediated method to produce monodispersed core-shell microspheres. By adjusting the concentration of reactants, the thickness of MON-2COOH shell was easily manipulated. The packed MON-2COOH@SiO 2 column showed high resolution and selectivity for separating both hydrophobic (alkylbenzenes, polycyclic aromatic hydrocarbons , anilines and phenols) and hydrophilic (nucleoside and nucleic bases) probes, highlighting the promise of MONs in mixed-mode HPLC. The MON-2COOH@SiO 2 column also achieved good separation to sulfonamides, nonsteroidal anti-inflammatory drugs, flavonoids and phenylurea herbicides , and offered better resolution than commercial C18 and pristine SiO 2 column. Multiple retention mechanisms were also found on MON-2COOH@SiO 2 packed column, underlining the great potential of MONs in mixed-mode HPLC.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xianhang Yan,Yanxin Wang,Bingyang Li,Zhenzhen Huang,Zhiyuan Gao,Xinhui Mao,Wei Wang,Zhijun Zhu,Matt J. Kipper,Linjun Huang,Jianguo Tang
Cu 2+ contamination in drinking water poses a threat to humans and the environment, and high concentrations of Cu 2+ in human blood can induce disease. In recent years, fluorescence sensing of Cu 2+ prepared from rare earth elements has been widely used for the accurate detection and quantification of Cu 2+ . In this paper, we report that europium (Eu), 4,4′,4-trimethyltriphenylamine (TTA), and 1,10-phenanthroline (Phen) undergo a complexation reaction to form the Eu(TTA) 3 Phen complex, which is loaded on SiO 2 nanoparticle to form SiO 2 @Eu 3+ . We use electrospinning of SiO 2 @Eu 3+ and polyacrylonitrile (PAN) co-blended solutions to prepare PAN fluorescent nanofiber membranes (FPNM). FPNM are hydrolyzed hydrolysis to obtain Cu 2+ sensors (HFPNM). The super hydrophilic surface of HFPNM undergoes fluorescence quenching upon contact with Cu 2+ . HFPNM is capable of accurately detecting 100–1000 nmol/L of Cu 2+ . Moreover, EDTA can be used as a reversible on/off switch for detection, and HFPNM can still be used as a Cu 2+ sensor after 5 cycles of use. The HFPNM have the advantages of high detection sensitivity and environmental friendliness for recycling compared to other Cu 2+ sensors. Fluorescent nanofibers can be combined with bio-nanotechnology allowing for promising future applications in Cu 2+ detection and wearable smart fabrics.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2022
·Vol. 119
·期 30
·e2202682119
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IF 12.779
Mingjie Huang,Yu-Sheng Li,Chuan-Qi Zhang,Chao Cui,Qing-Qing Huang,Mengkai Li,Zhimin Qiang,Tao Zhou,Xiaohui Wu,Han-Qing Yu
Heterogeneous peroxymonosulfate (PMS)–based advanced oxidation processes (AOPs) have shown a great potential for pollutant degradation, but their feasibility for large-scale water treatment application has not been demonstrated. Herein, we develop a facile coprecipitation method for the scalable production (∼10 kg) of the Cu-Fe-Mn spinel oxide (CuFeMnO). Such a catalyst has rich oxygen vacancies and symmetry-breaking sites, which endorse it with a superior PMS-catalytic capacity. We find that the working reactive species and their contributions are highly dependent on the properties of target organic pollutants. For the organics with electron-donating group (e.g., -OH), high-valent metal species are mainly responsible for the pollutant degradation, whereas for the organics with electron-withdrawing group (e.g., -COOH and -NO2), hydroxyl radical (•OH) as the secondary oxidant also plays an important role. We demonstrate that the CuFeMnO–PMS system is able to achieve efficient and stable removal of the pollutants in the secondary effluent from a municipal wastewater plant at both bench and pilot scales. Moreover, we explore the application prospect of this PMS-based AOP process for large-scale wastewater treatment. This work describes an opportunity to scalably prepare robust spinel oxide catalysts for water purification and is beneficial to the practical applications of the heterogeneous PMS-AOPs.
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