CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Baokang Xu,Xiao Zhang,Yue Zhang,Shiwen Wang,Peng Yu,Yongjun Sun,Xi Li,Yanhua Xu
The nonradical pathway selectively oxidizes pollutants with less interference from environmental factors, which can effectively improve the environmental suitability of peroxymonosulfate (PMS) activation. Herein, a Co-doped nanotubular carbon nitride catalyst (Co-CNNT) based on CoN x sites was constructed for stable and efficient PMS activation with a better specific surface area, number of CoN x sites, and electron transfer capability than Co-doped lamellar carbon nitride catalyst (Co-CN). Co-CNNT improved PMS utilization efficiency (∼50%) and enhanced the contribution of the electron transfer pathway to tetracycline (TET) degradation. The enhanced ability of Co-CNNT to adsorb PMS leads to Co-CNNT–PMS* generated by PMS at the CoN x site, which raises the Co-CNNT surface potential and allows PMS to be activated in a manner that captured electrons. Thus, the Co-CNNT/PMS system could effectively destroy electron-rich or low-potential pollutants within 24 min. The stronger environmental adaptability allows it to maintain catalytic activity in complex aqueous matrices, achieving effective oxidation of diluted tetracycline-based pharmaceutical wastewater. This paper reveals the effects of carbon nitride morphology control strategies on the properties of CoN x active sites and PMS activation mechanisms, providing new insights into the induction of nonradical PMS activation pathways.
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JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Qi He,Dandan Wang,Jing Shao,Yi Li,Ming Cheng,Lihui Dong,Yunhui Li,Jianwei Zhu,Hongji Li
A novel imprinting membrane (Ag/CuO/CNTs/Eggshell membrane -Molecularly Imprinted polymeric Membrances, ACCE-MIMs) based on surface enhanced Raman scattering (SERS) is successfully synthesized for the specific detection of spiramycin (SP). Firstly, CNTs and CuO are successively loaded on eggshell membrane (ESM) to increase the uniformity and sensitivity by virtue of the unique reticular structure of CNTs and excellent chemical enhancement of CuO. Through the abundant amino and carboxyl groups on ESM, Ag nanoparticles (Ag NPs) are anchored and growth on the surface of membrane by two in-situ reduction process and form a three-dimensional (3D) architecture. Eventually, the ACCE-MIMs are synthetized by silicon-based sol-gel method. With the help of imprinted polymers, the ACCE-MIMs present anti-interference performance during selective detection. The sensor presents a great liner relationship (R 2 = 0.9965) between SP concentration and the Raman peak intensity when the concentration of SP ranges between 1 × 10 −6 M ∼1 × 10 −12 M. The limit of detection concentration is 1 × 10 −12 M and the enhancement factor (EF) is 0.2956 × 10 7 . The ACCE-MIMs exhibits sensitive detection property and this procedure provides a promising future for detection process.
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ANALYST
·
2023
·Vol. 148
·期 6
·1322-1329
·
IF 4.2
Chunyan Zhang,Yifeng Fan,Liangliang Cai,Xiaofei Ma
The discovery of novel chiral selectors always fascinates us. This work describes the chiral separation performances of a new chiral selector (kasugamycin, KAS) in capillary electrophoresis (CE) for six pairs of stereoisomers, including ephedrine and pseudoephedrine, quinine and quinidine, cinchonine and cinchonidine, and amlodipine, promethazine and ofloxacin enantiomers. Kasugamycin, an aminoglycoside antibiotic in agriculture, shows significant biological activity against rice blast with low toxicity. As it turns out, this new chiral selector possesses good CE compatibility and stereoselectivity towards model analytes. In this work, we systematically investigated several separation parameters including kasugamycin concentration, buffer pH, separation voltage and the composition of the buffer solution. A detailed discussion about the chiral recognition mechanism was made based on Statistical Product and Service Solution (SPSS) analysis, NMR experiments (1D and 2D) and molecular modeling. This is the first time that kasugamycin is utilized as a chiral selector in CE, and the development of new chiral selectors from agricultural or veterinary antibiotics deserves more attention.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Bo Han,Qihui Pan,Yuhao Chen,Ding Liu,Chenggang Zhou,Kaisheng Xia,Qiang Gao
Utilizing cobalt-containing oxides as catalysts is one of the most popular ways of activating peroxymonosulfate (PMS) to generate sulfate radical (SO 4 − ) for elimination of organic pollutants. However, it still remains a great challenge to realize high activity, good stability, and easy recyclability at the same time. Herein, we demonstrate that high-entropy perovskite oxide (HEPO) washcoated porous alumina ceramic (La(Co 0.2 Al 0.2 Fe 0.2 Mn 0.2 Cu 0.2 )O 3 @PAC) is a superb catalyst for PMS activation. In particular, benefiting from unique multimetallic composition and entropy-stabilized structure, the La(Co 0.2 Al 0.2 Fe 0.2 Mn 0.2 Cu 0.2 )O 3 @PAC manifested high catalytic activity with a turnover frequency (TOF) up to 15.38 min −1 in activating PMS for degradation of antibiotic pollutant metronidazole (MNZ). Meanwhile, the high stability of HEPO gave rise to a significant decrease of cobalt leaching (0.111 mg L −1 ) in comparison with LaCoO 3 @PAC catalyst (1.71 mg L −1 ). Moreover, monolithic porous architecture of La(Co 0.2 Al 0.2 Fe 0.2 Mn 0.2 Cu 0.2 )O 3 @PAC could not only endow this catalyst with easy recyclability but ensure high permeability for rapid mass transfer of guest species. Our work exemplifies the superiority of HEPO-based monolithic catalyst as a new promising activator of PMS for water remediation.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2022
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IF 4.831
Yuanjie Teng,Zhenni Wang,Shaohua Zuo,Xin Li,Yinxin Chen
Universal and fast antibiotic residues detection technology is imperative for the control of food safety in aquatic products. However, accurate surface-enhanced Raman scattering (SERS) quantitative detection of complicated samples is still a challenge. A recognition method powered by deep learning and took advantage of the unique fingerprint information merits of SERS was proposed. Herein, the spectra were collected by Ag nanofilm SERS substrate prepared by self-assembly of Ag nanoparticles on water/oil interface. A SERS-based database of commonly used antibiotics in aquatic products was set up, which is suitable for employed as input data for learning and training. The results show that the five types of antibiotics are successfully distinguished through principal component analysis (PCA) and each antibiotic in every type was successfully distinguished. Furthermore, one-dimensional convolutional neural networks (1-D CNN) was used to distinguish the antibiotics, and the results show that all the test samples were correctly predicted by 1-D CNN model. The results of this research suggest the great potential of the combination of SERS spectra with deep learning as a method for rapid and highly accurate identification of antibiotic residues in aquatic products.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Yujie Zhang,Qin Yang,Luchao Yue,Qian Liu,Yongsong Luo,Junyou Wu,Xiaowen Kang,Shengjun Sun,Yingchun Yang,Xuping Sun
In this work, Fe 3 O 4 nanoparticles anchored biomass juncus derived carbon (Fe 3 O 4 @JDC) was developed as a highly efficient heterogeneous peroxymonosulfate (PMS) activator to degrade organic pollutants. As-prepared catalyst was characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and vibrating sample magnetometer techniques. High loading and good dispersion of Fe 3 O 4 nanoparticles on JDC lead to excellent degradation performance for tetracycline (90.2 %, 60 min) and other pollutants (above 80 %), and the reaction rate constant (k) is 3.73 times (0.0384 min −1 ) than that of pure JDC (0.0103 min −1 ) in the presence of PMS. Additionally, chemical oxygen demand (COD) removal rate of Fe 3 O 4 @JDC/PMS system (64.7 %, 60 min) is best than other systems (JDC system, JDC/PMS system, etc.). The quenching tests and electron paramagnetic resonance (EPR) data further demonstrate that TC degradation is an integrative contribution of both non-radical ( 1 O 2 ) and free radical (O 2 − , SO 4 − , and OH) pathways. Furthermore, Fe 3 O 4 @JDC also exhibits superior reusability (81.1 % degradation efficiency after five cycles) and magnetic separation ability.
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MOLECULES
·
2022
·Vol. 27
·期 23
·8324
·
IF 4.927
Xiuying Liu,Yuanyuan Cheng,Binbin Guan,Fei Xia,Ling Fan,Xue Gao,Xiaofei Sun,Xuepeng Li,Lijie Zhu
A multicolor immunochromatographic assay platform based on quantum dot nanobeads (QBs) for the rapid and simultaneous detection of nitrofuran metabolites in different aquatic products is documented. These metabolites include 3-amino-2-oxazolidinone (AOZ), 1-aminohydantoin (AHD), semicarbazide (SEM), and 3-amino-5-morpholino-methyl-1,3-oxazolidinone (AMOZ). QBs with emission colors of red, yellow, green, and orange were employed and functionalized with the corresponding antibodies to each analyte to develop a multicolor channel. The visual detection limits (cutoff values) of our method for AOZ, AHD, SEM, and AMOZ reached up to 50 ng/mL, which were 2, 20, 20, and 20 times lower than those of traditional colloidal gold test strips, respectively. The test strip is capable of detection within 10 min in real samples while still achieving good stability and specificity. These results demonstrate that the developed multicolor immunochromatographic assay platform is a promising technique for multiplex, highly sensitive, and on-site detection of nitrofuran metabolites.Keywords:nitrofuran metabolites;multiplex immunochromatographic assay;quantum dot nanobeads;fluorescent test strip
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xixi Chen,Wanyi Fu,Yulong Yang,Yanjun Li,Kai Yang,Xuanbo Xu,Xihui Zhang
Atomic H* has been reported to be thermodynamically feasible for activating hydrogen peroxide (H 2 O 2 ) to produce radicals, while the nonradical pathway and the contributions of metal sites and atomic H* in H 2 O 2 activation need further exploration. In this study, a TiO 2 @MnO 2 catalyst was synthesized via a facile hydrothermal method and surprisingly found to produce atomic H* over Mn sites in water without external energy input (e.g., light and electricity). Atomic H* plays an essential role in the activation of H 2 O 2 via a nonradical pathway, which induces the removal of tiamulin up to 80.4–91.7% in 20 min at a wide pH range of 4.0–11.0. Density function theory calculations prove that atomic H* owns a much lower total energy barrier (ΔG total = 0.68 eV) for the decomposition of H 2 O 2 to generate superoxide and singlet oxygen than Mn sites (ΔG total = 2.90 eV). This study is a re-visit to the mechanism of activating H 2 O 2 via atomic H* for efficient degradation of emerging organic contaminants .
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WATER RESEARCH
·
2022
·
IF 13.4
Li Chen,Tahir Maqbool,Ghazanfar Nazir,Congyu Hou,Yanna Xu,Yulong Yang,Xihui Zhang
A composite manganese-based catalytic ceramic membrane (Mn-CCM) was developed by a solid-state sintering method, and its effectiveness toward activation of peroxymonosulfate (PMS) for the degradation of 11 pharmaceutical and personal care products (PPCPs) mixture was tested. The optimized Mn-CCMs/PMS system showed remarkable degradation efficiencies for PPCPs mixture with total removal >90% in ultrapure water, river water and natural organic matter (NOM) solution. The Mn-CCMs/PMS system showed the contribution of different phenomena in PPCPs removal in the order of catalytic oxidation (54.7%, Mn-CCMs/PMS) > noncatalytic oxidation (42.3%, PMS oxidation) > adsorption (3.0%, by Mn-CCMs). The singlet oxygen ( 1 O 2 ) was the dominant reactive oxygen specie for the degradation of PPCPs in all water matrices proved by the quenching experiments and electro-paramagnetic resonance (EPR) spectroscopy. The extraordinary stability of Mn-CCMs for the activation of PMS has been noted in terms of repeatability experiments for PPCPs degradation with fewer leaching of Mn (1.9 to 3.6 µg/L). Mineralization was achieved in the range of 28–65% for different water matrices. The toxicity of the PPCPs mixture was reduced by 85.9%. The Mn-CCMs/PMS system showed a reduction (25–100%) in precursors of different carbon- and nitrogen-based disinfection by-products. This study found the Mn-CCMs/PMS system as a feasible purification unit for removing trace concentrations of PPCPs (ng/L) in real drinking water matrices.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-13
·
IF 17.694
Li Bang Lin,Luo Jun Jiang,Zou Hao Lin,Zhang Qing-Meng,Zhao Liu-Bin,Qian Hang,Luo Hong Qun,Leong David Tai,Li Nian Bing
The transfer of the concept of chirality from molecules to synthesized nanomaterials has attracted attention amongst multidisciplinary teams. Here we demonstrate heterogeneous nucleation and anisotropic accumulation of Au nanoparticles on multilayer MoS 2 planes to form chiroptically functional nanomaterials. Thiol amino acids with chiral conformations modulate asymmetric growth of gold nanoarchitectures on seeds of highly faceted Au/MoS 2 heterostructures. Consequently, dendritic plasmonic nanocrystals with partial chiral morphologies are synthesized. The chirality of dendritic nanocrystals inherited from cysteine molecules refers to the structural characteristics and includes specific recognition of enantiomeric molecules. With integration of the intrinsic photothermal properties and inherited enantioselective characteristics, dendritic Au/MoS 2 heterostructures exhibit chirality-dependent release of antimicrobial drugs from hydrogel substrates when activated by exogenous infrared irradiation. A three-in-one strategy involving synthesis of chiral dendritic heterostructures, enantioselective recognition, and controlled drug release system is presented, which improves nanomaterial synthetic technology and enhances our understanding of crucial chirality information.
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WATER RESEARCH
·
2023
·
IF 12.8
Xixi Chen,Wanyi Fu,Zhichao Yang,Yulong Yang,Yanjun Li,Hui Huang,Xihui Zhang,Bingcai Pan
Hydrogen peroxide (H 2 O 2 ) is the most commonly used oxidant in advanced oxidation processes for emerging organic contaminant degradation. However, the activation of H 2 O 2 to generate reactive oxygen species is always accompanied by O 2 generation resulting in H 2 O 2 waste. Here, we prepare a Ti doped Mn 3 O 4 /Fe 3 O 4 ternary catalyst (Ti-Mn 3 O 4 /Fe 3 O 4 ) to create abundant oxygen vacancies (OVs), which yields electron delocalization impacts on enhancing the electrical conductivity, accelerating the activation of O 2 to produce H 2 O 2 . In Ti-Mn 3 O 4 /Fe 3 O 4 /H 2 O 2 system, OVs-mediated O 2 /O 2 •− /H 2 O 2 redox cycles trigger the activation of locally generated O 2 , boost the regeneration of O 2 •− and on site produce H 2 O 2 for replenishment. This leads to a 100% removal of tiamulin in 30 min at an unprecedented H 2 O 2 utilization efficiency of 96.0%, which is 24 folds higher than that with Fe 3 O 4 /H 2 O 2 . Importantly, further integration of Ti-Mn 3 O 4 /Fe 3 O 4 catalysts into membrane filtration achieved high rejections of tiamulin (> 83.9%) from real surface water during a continuous 12-h operation, demonstrating broad pH adaptability, excellent catalytic stability and leaching resistance. This work demonstrates a feasible strategy for developing OVs-rich catalysts for improving H 2 O 2 utilization efficiency via activation of locally generated oxygen during the Haber-Weiss reaction.
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Journal of Materials Chemistry C
·
2022
·Vol. 11
·期 3
·1165-1172
·
IF 8.067
Yating Wang,Chaosheng Peng,Airu Liu,Jinyue Song,Xingang Li,Tao Jiang
The precise intramolecular-tailored strategy is deemed to have abundant potential to promote the activity of metal-free photocatalysts yet remains a daunting task. In this work, we report a simple one-step calcination method for skillfully incorporating alkyl into the tri-s-triazine ring of graphite carbon nitride (g-C3N4). The photocatalytic tetracycline photodegradation rate of the optimal ethyl modified g-C3N4 (CN-E-75) is significantly higher than that of the original g-C3N4. Experimental and theoretical calculation results show that the significantly enhanced photocatalytic activity is mainly due to the optimization of the electronic band structure of g-C3N4 by introducing ethyl defects attached to N atoms in the tri-s-triazine rings. The ethyl defect mainly splits the Np orbitals to generate mid gap states under the conduction band edge, thereby consequently narrowing the band gap to extend visible light harvesting, but also meanwhile accelerates charge delivery to boost the photogenerated charge separation, inhibiting electron–hole recombination, and thus considerably increases the photocatalytic properties. Moreover, as-fabricated CN-E-75 verifies the satisfied stability after five cycling runs for photocatalytic water splitting for H2 evolution and tetracycline photodegradation. This work sheds light on deep understanding of intramolecular tailored defect engineering and offers guidance to design other efficient photocatalytic systems.
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