SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
·
IF 9.8
Lan Liang,Guanyi Chen,Jianhui Zhao,Penghui Shao,Ning Li,Mengting He,Qinglong Fu,Beibei Yan,Li-an Hou
The peroxymonosulfate (PMS) process may be hindered severely due to natural organic matter (NOM) conversion in the treatment of emerging pollutants from river water, becoming a critical engineering and technical issue. In this study, a Fe(II)-induced river water (RW)/PMS catalytic system was constructed for investigating molecular transformation of NOM and related influence mechanism to sulfamethoxazole (SMX) degradation. Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) analysis indicated that NOM molecules containing no more than one heteroatom in river may be attacked by hydroxyl radicals ( OH) and then polymerized, converting into molecules with two or three heteroatoms during PMS oxidation. Based on the correlation analysis, CHONP-NOM, CHOSP-NOM and CHONSP-NOM showed a significant inhibition against SMX degradation, while CHONS-NOM exhibited a moderate inhibitory effect. Besides, more condensed aromatic structures, carbohydrates and tannins were generated via reactive species ( OH and sulfate radicals (SO 4 − )) oxidation, radical addition and polymerization reactions. Notably, condensed aromatic structures, carbohydrates and tannins presented weak, modest and strong inhibition to SMX degradation, respectively. Based on the current results, the inhibition of target pollutants degradation would be mitigated via regulation of NOM molecules in a Fe(II)-induced PMS activation system, providing valuable information to reduce NOM impact. In addition, this study paves the way to achieve efficient removal of emerging pollutants from river water.
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高影响因子
CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Gang Li,Ruiyang Tan,Xiangcheng Lu,Xinyu Zhang,Chengcheng Zhang,Bohong Gao,Yuting Zhou,Ke Chen,Ping Chen,Xinyi Wang
Chemical composition and morphological optimization are both effective strategies for constructing excellent electromagnetic wave absorption (EMWA) materials. While efficient EMWA materials derived from both metal-organic frameworks (MOFs) and MXenes have been extensively studied, composites derived from the Hofmann framework with MXene have not been reported. In this study, we employed a Hofmann framework ([Fe(pz)Ni(CN) 4 ], pz = pyrazine) and MXene (Ti 3 C 2 T x ) to create new MXene@Hofmann (MH1 and MH2) composites, using a simple co-precipitation method with two different contents of [Fe(pz)Ni(CN) 4 ]. The FeNi/C/TiO 2 composites with a multi-layered structure inherited from MXene were prepared by annealing the MXene@Hofmann composites at 500, 600, and 700 °C, resulting in the formation of MH1-500/600/700 and MH2-500/600/700 composites. Their compositions, morphologies, electromagnetic parameters, and EMWA performances were characterized. For the composites with a high [Fe(pz)Ni(CN) 4 ] content, MH2-600 has a minimum reflection loss ( RL min ) value of −30.63 dB at a thickness of only 1.8 mm and the broadest effective absorption bandwidth (EAB) of 3.90 GHz at 2.0 mm, while MH2-700 exhibits superior EMWA performance with an RL min value of −34.34 dB at 1.9 mm and an EAB value of 4.96 GHz at 2.1 mm. Their impressive EMWA performance might be attributed to the synergistic dielectric loss and magnetic loss and also the impedance matching from the reasonable ratio of the magnetic and dielectric components. This work demonstrates an effective strategy for constructing EMWA materials from the Hofmann framework and MXene.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Minghui Liu,Yutong Zhao,Ming Tian,Kejia Liu,Guoping Hu,Jian Zhang,Tianyan Xue,Tao Qi,Hui Zhang
Platinum group metals (PGMs) are scarce critical materials, and recovering PGMs from spent automotive catalysts (SAC) is economically and ecologically important. However, dissolving the Fe-Si-PGMs alloy derived from SAC is challenging, impeding PGMs recovery. This study aims to develop a more sustainable, efficient, and scalable leaching scheme. We demonstrate efficient leaching of Fe-Si-PGMs alloy using a thermochemical combined with mechanochemical leaching method with a HCl + FeCl 3 + H 2 O 2 solution. Kinetics parameters studies optimize the leaching process. The main obstacles to leaching are the chemical inertness of the alloy and the SiO 2 encapsulation formed. Ultimately, efficient dissolution of 99 % Pd, 95 % Pt and 88 % Rh was achieved, increasing PGMs leaching by 17 % compared to single thermochemical leaching. Additionally, this work remedies the scalability limitations of mechanochemical leaching and provides valuable insights for PGMs recovery.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Zheng Guo,Han-Yi Zheng,Zhong-Ying Huang,Yue-Zhen Liu,Yao-Hua Liu,Yun Chen,Jing Gao,Yong Hu,Chao Huang
A ternary deep eutectic solvent (DES) consisting of choline chloride, lactic acid, and urea in a molar ratio of 1:2:2 was used to pretreat chamomile residue, followed by carbon dots (CDs) preparation using a one-pot solvothermal method . The CDs prepared under the suitable conditions had a high quantum yield of 47.34% and could be used as a bifunctional fluorescent probe for the detection of tartrazine and Fe(III). The concentration of tartrazine or Fe(III) had a good linear relationship with the fluorescence intensity of CDs that the determination coefficient ( R 2 ) was 0.9957 and 0.9943, and the limit of detection (LOD) was 40 nM and 119 nM, respectively. After verifying the different fluorescence quenching mechanisms of CDs by these two substances, a quantitative analysis was performed on real samples with recoveries of 90.70%∼104.29%. Overall, this study provided a promising technology for chemical conversion from low-cost chamomile residue to attractive bifunctional fluorescent probe.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Qun Ding,Xuejun Zou,Jun Ke,Yuying Dong,Yubo Cui,Hongchao Ma
Herein, a ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 heterojunction is successfully constructed through a facile hydrothermal strategy for enhancing solar energy harvesting and efficiency of catalytic nitrogen reduction induced by enlarged light absorption range, increasing interfacial charge transfer ability and desirable stability. Under the simulated sunlight irradiation, the N 2 fixation experiment shows that the yield of NH 3 reaches 1084.31 μmol/(g·h) over the TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalyst, and the yield is significantly enhanced, which is 33.68 and 13.94 times that is higher than the pure TiO 2 and g-C 3 N 4 , respectively. In a mean time, the excellent performance of the photocatalytic N 2 fixation over the ternary TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is verified based on density function theory calculation and the decisive step over the composite is investigated by calculating Gibbs free energies of nitrogen reduction paths. The performance enhancement mechanism of TiO 2 /MIL-88A(Fe)/g-C 3 N 4 is speculated, which indicates that the hybridized three-component system presents a desirable Z-scheme band alignment, resulting in the improvement of separation and transfer efficiency of photoinduced charge carriers. The article shows a new and high-efficiency TiO 2 /MIL-88A(Fe)/g-C 3 N 4 photocatalysis for excellent nitrogen reduction ability.
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高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Yingqian Zhang,Zhifei Ma,Xianchuan Xie,Daishe Wu,Xing Peng,Jianlong Li
Zero-valent iron (ZVI) is a promising technology for groundwater treatment , and its efficiency primarily depends on the electron transfer . However, there are still some problems such as low electron efficiency of ZVI particles and high yield of iron sludge that limits the performance, which warrant further investigation. In our study, a silicotungsten acidified ZVI composite (m-WZVI) was synthesized by ball milling to activate PS to degrade phenol. m-WZVI has a better performance on phenol degradation (with a removal rate of 91.82%) than ball mill ZVI(m-ZVI) with persulfate (PS) (with a removal rate of 59.37%). Compared with m-ZVI, the first-order kinetic constant (k obs ) of m-WZVI/PS is 2–3 times higher than that of the others. Iron ion was gradually leached in m-WZVI/PS system, being only 2.11 mg/L after 30 min, having to avoid excessive consumption of active substances. The underlying mechanisms of m-WZVI for PS activation mainly include: 1) were elucidated through different characterizations analyses that accounted for silictungstic acid (STA) can be combined with ZVI, and a new electron donor (SiW 12 4− ) was obtained, which improved the transfer rate performance of electrons for activating PS; 2) singlet oxygen ( 1 O 2 ) is the main active substance for phenol degradation, but other radicals also played an important role. Therefore, m-WZVI has good prospects for improving the electron utilization of ZVI.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Jing Zhang,Yi Shen,Chenge Liang,Huiyu Yi,Jining Liu,Yungui Li,Qingqing Li,Qile Fang
In response to phosphorus pollution, developing functional materials for phosphate adsorption is an ideal method to reach an ultralow phosphate concentration in effluent. Herein, a hexagon flower-shaped architecture constructed of Fe-composited lanthanum (La)-based hydroxide nanosheets was fabricated from LaFe cyano-bridged metal frameworks (CMs) via a self-templating strategy using NH 3 ‧H 2 O as the conversion reagent. The ion exchange process using weak alkaline reagent enables the formation of secondary nanosheets on the architecture, thus leading to a high surface area and a large number of mesopores that provide abundant active sites and mass transfer channels for phosphate adsorption. A superior adsorption capacity of 127.5 mg P/g can be obtained on the La/Fe-based architecture, which also shows satisfactory applicability over a wide pH range. A ligand exchange between -OH and phosphate ions is verified as the main adsorption mechanism, which properly accounts for its excellent selectivity for phosphate adsorption when coexisting with other anions/cations and natural organic matters . Overall, the present study provides a new method for constructing porous La-based hydroxide materials for phosphorus control in water.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 18
·5435-5448
·
IF 5
Xinyue Hu,Jialing Chen,Shaokang He,Tingyu Liang,Shenke Zheng,Lijun Lu,Chenxi Hao,Kaixin Chen,Tingting Li,Lan Yi,Li Guo,Xiaoqin Wu
Three OP-Fe-FER-x zeolites (with an FER structure) synthesized by a one-pot method with different Si/Al ratios (x = Si/Al =10–30) and similar iron contents (5.4–5.6 wt%) were compared with commercial IM-Fe/SSZ-20 zeolite (with a CHA structure) prepared by an incipient wetness impregnation method to investigate their catalytic activity and hydrothermal stability for the selective catalytic reduction reaction of NOx with NH3 (NH3-SCR). For both fresh (without hydrothermal aging treatments) and aged (with hydrothermal aging treatments) zeolites, the NOx conversions of OP-Fe-FER-x zeolites are much higher than that of IM-Fe/SSZ-20 zeolite, suggesting that the OP-Fe-FER-x zeolites are better catalysts for NH3-SCR than the commercial IM-Fe/SSZ-20 zeolite. Compared with the fresh zeolites, the NOx conversions of all four aged zeolites decrease in the low-temperature range (100–300 °C), while they increase at high temperatures (450–550 °C) to different extents. Based on XRD, N2 physisorption, NH3-TPD, UV-vis, XPS and H2-TPR experiments, the hydrothermal aging process of the OP-Fe-FER-x zeolites is depicted, which consists of partial collapse of the zeolite framework, removal of framework aluminum and iron atoms, and transformation and aggregation of iron species. Detailed characterization reveals that the OP-Fe-FER-x zeolites are more stable than the IM-Fe/SSZ-20 zeolite during the hydrothermal aging treatments. The obvious decline of NH3-SCR catalytic activity for the aged zeolites in the low-temperature range is mainly attributed to the transformation and aggregation behaviors of active isolated Fe3+ species. As for the increase of NH3-SCR activity for the aged zeolites at the high temperatures (450–550 °C), it is mainly attributed to the suppression of the NH3 oxidation side reaction due to the deteriorated NH3 storage capacity because of the loss of massive acid sites during the hydrothermal aging treatments.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2023
·Vol. 98
·期 10
·2577-2586
·
IF 3.4
Shili Yan,Jiamei Zhu,Hongmin Wang,Bingqian Liu,Qinling Bi
BACKGROUND Heavy oil has the characteristics of high viscosity and low American Petroleum Institute gravity, which makes it difficult to transport and produce. The key to efficiently utilizing heavy oil is reducing viscosity and improving quality. Hydroconversion has the advantages of viscosity reduction and decreased coke production, but it is difficult to separate nonmagnetic catalysts from the reaction system, which affects the industrial application. RESULTS A spherical Fe 3 O 4 (74.71 emu g −1 ) and a chain Fe Fe 2 O 3 (110 emu g −1 ) were prepared as magnetic cores, and coated with SiO 2 and Al 2 O 3 layers, respectively. The metal-supported catalyst modified with Co and Ni show irregular and honeycomb-shaped surfaces, and the magnetic saturation strength decreases to 24.91 and 14.63 emu g −1 , but still possessing superparamagnetic properties, enabling the catalysts to be separated from the reaction mixture. Fe-Fe 2 O 3 @SiO 2 @Al 2 O 3 @CoNi catalyst has the best viscosity reduction effect for Canadian oil sands asphalt residue at about 410 °C and 10 MPa hydrogen pressure. The viscosity of the liquid product decreased significantly from 56 600 to 135 mPa s at 50 °C, with a viscosity reduction of 99.8%. CONCLUSION Magnetic catalyst prepared from chain-like Fe-Fe 2 O 3 has an excellent honeycomb structure, which can provide increased active surfaces and exhibit improved viscosity reduction performance. This work provides a strategy for the recovery of heavy oil hydrogenation catalysts and is expected to play a key role in the practical application of heavy oil hydrogenation catalytic viscosity reduction. © 2023 Society of Chemical Industry.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Fangchao Cui,Lanling Li,Dangfeng Wang,Likun Ren,Jiesen Li,YiLin Lu,Yuqiong Meng,Rui Ma,Shulin Wang,Xuepeng Li,Tingting Li,Jianrong Li
Bacterial biofilm infections cause about 600 million foodborne illnesses and about 420,000 confirmed deaths annually. However, traditional antibiotics and emerging nanomaterials have the problem of causing bacterial resistance, no catalytic activity and low biocompatibility. Herein, one new antibacterial carbon dots-based nanozyme Fe/N-CDs was developed with antibiofilm ability, excellent peroxidase activity and high biocompatibility. The Fe/N-CDs nanozyme manifested outstanding broad-spectrum antibacterial activity (even multidrug-resistant bacteria) by catalyzing the decomposition of H 2 O 2 to •OH through a peroxide-like reaction (V max /K m =1.07×10 -6 /s), which was 5.35-fold that of horseradish peroxidase (V max /K m =0.20×10 -6 /s). The antibacterial activity increased more than 500-fold after catalysis. The inhibitory capability of Fe/N-CDs nanozyme for Hafinia alvei biofilm was up to 80.2% of by inhibiting extracellular polymeric substances, total protein, AKP enzyme and ATPase. Notably, no obvious cytotoxicity and development of bacteria resistance were observed after co-culturing with the Fe/N-CDs nanozyme. Furthermore, the fresh test results demonstrated that the Fe/N-CDs nanozyme could effectively extend the shelf life of salmon for 3–6 days. These findings indicated that nanozyme could be used to extend the shelf life of food. What’s more, this antibiofilm Fe/N-CDs nanozyme provides the potential idea for developing carbon-based nanomaterials with catalytic activity and prevention of bacterial infections in food preservation.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Huifang Feng,Yitong Sun,Qiaozhen Xu,Hong Liu
Developing efficient photocatalyst to promote the conversion of CO 2 into value-added chemicals remains challenging. Here, novel NH 2 -MIL-101(Fe)@Bi 2 MoO 6 S-scheme heterojunctions were fabricated via a solvothermal method, in which Bi 2 MoO 6 (BMO) nanoparticles uniformly growing on the NH 2 -MIL-101(Fe) (NM101) octahedrons with intimate contact interface. The resultant heterojunctions revealed significantly enhanced activity for CO 2 photoreduction. The optimal performance was achieved when the content of BMO was 10 wt%, and the formation rate of CO reached 67.0 μmol·g −1 ·h −1 under visible light illumination (with apparent quantum efficiency of 0.09 % at 450 nm), which was 3.2-fold of individual NM101. The boosting activity benefited from the formation of S-scheme heterojunction at the NM101 @BMO interfaces, which facilitated the separation of photoinduced electron-hole pairs with strong redox ability at the interface. This S-scheme charge transfer mechanism was further validated by the in-situ XPS and fluorescence probe molecular experiment. Besides, the intermediates and preliminary mechanism of photoreaction were unraveled based on in-situ DRIFTS analysis. This work provides some novel insights for designing efficient S-scheme photocatalysts for CO 2 photoreduction.
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Catalysts
·
2023
·Vol. 13
·期 8
·1150
·
IF 3.9
Xinying Chen,He Zhang,Shizhe Xu,Xiaoge Du,Kaida Zhang,Chun-Po Hu,Sihui Zhan,Xueyue Mi,Wen Da Oh,Xiao Hu,Ziyong Pan,Yueping Bao
In the current work, a novel Co-Fe bimetallic immobilized cellulose hydrogel bead (CoFeO@CHB) was prepared via in situ chemical precipitation followed by heat treatment and applied for tetracycline (TC) degradation in the presence of peroxymonosulfate (PMS). The characterization results indicated that the Co-Fe particles were evenly distributed within the porous cellulose hydrogel beads, without affecting their morphologies or crystal structures. During the TC degradation, the CoFeO@CHB/PMS system showed a high resistance and stability to different water bodies, and the common anions and natural organic matters showed a limited effect on TC degradation. The chemical quenching experiments (using chemicals to react with specific reactive species) as well as electron paramagnetic resonance (EPR) results showed that CoFeO@CHB can effectively active PMS to generate multiple reactive oxygen species (ROS, such as SO4•−,•OH and1O2), in which the1O2-dominated non-radical pathway played a vital role in TC degradation. Both Co and Fe were proposed as the active sites for PMS activation, and the CoFeO@CHB/PMS system showed a high potential in practical application due to its high selectivity and robustness with much less toxic intermediate products. Furthermore, a long-term continuous home-made dead-end filtration device was constructed to evaluate the stability and application potential of the CoFeO@CHB/PMS system, in which a >70% removal was maintained in a continuous 800 min filtration. These results showed the promising potential for cellulose hydrogel beads utilized as a metal-based nanomaterial substrate for organic degradation via PMS activation.Keywords:hydrogels;peroxymonosulfate;non-radical;tetracycline
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危险品化学品经营许可证（带存储）