PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2023
·Vol. 25
·期 19
·13716-13727
·
IF 3.3
Caihong Wang,Yong Liu,Fengshen Han,Yongzhe Han,Tianyu Liu,Haitao Ren,Xu Han
Using metal-free catalysts is widely recognized as a promising approach toward wastewater remediation because of the absence of metal leaching. However, the oxidation products involved in the oxidation process and the corresponding mechanisms are still not clear. In this work, N-doped carbocatalysts (CN) were fabricated using as-prepared g-C3N4 and glucose solution, and the reactivity of the as-prepared catalysts was optimized by controlling calcination temperature. Correspondingly, increasing the calcination temperature promotes the catalytic oxidation of BPA. The positive correlations between the contents of pyridinic-N and graphitic-N and the kobs values of BPA oxidation, as well as XPS analysis indicate the important roles of pyridinic-N and graphitic-N in BPA oxidation. According to the series of characterizations of the oxidation products and Raman analysis of the reaction process, the moderately activated persulfate (PS) on the CN catalyst is the predominant species in BPA oxidation and BPA can be oxidized to BPA polymers with high selectivity by H-abstraction under alkaline conditions. This work highlights the important role of the moderate activation of PS in the polymerization of phenolic contaminants under alkaline conditions, which enriches our understanding of the oxidation of aromatic contaminants by PS under alkaline conditions.
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MICROCHIMICA ACTA
·
2018
·Vol. 185
·期 9
·1-10
·
IF 5.705
Zhou Xiu-Jie,Zhang Li-Shun,Song Wen-Fang,Huang Yan-Ping,Liu Zhao-Sheng
An inorganic-organic hybrid monolith incorporated with stellated mesoporous silica nanoparticles (SMSNs) was prepared. Using binary solvents, deep eutectic solvents and room temperature ionic liquids, an SMSN-incorporated poly(butyl methacrylate- co -ethylene glycol dimethacrylate) monolith demonstrated uniform structure with good column permeability. A systematic investigation of preparation parameter was performed, including SMSN content, crosslinking monomer content, and the component of binary solvent. The optimized monoliths were characterized by field emission scanning electron microscopy, transmission electron microscopy, area scanning energy dispersive spectrometry, and nitrogen adsorption. Column performance was tested by separating four groups of analytes (alkylbenzenes, anilines, naphthalenes and phenols) by capillary electrochromatography (CEC). Baseline separation of all analytes was obtained with column efficiencies of up to 266,000 plates m −1 . The performance of the resulting monolith was further investigated in detail by separating mixtures of polycyclic aromatic hydrocarbons (PAHs), nonsteroidal antiinflammatory drugs (NSAIDs), and hydroxybenzoic acid isomers. Compared with the corresponding SMSN-free monolith, the CEC performance was improved by about six times. Successful extraction of PAHs and quinolones (QNs) were also performed using this capillary. Improved extraction efficiency (20.2%) for complex samples, lake water, was also found when the material was applied to solid phase microextraction of fluoranthene.
A poly(butyl methacrylate-co-ethylene glycol dimethacrylate) monolith incorporated with stellated mesoporous silica nanoparticles was prepared. It demonstrated column efficiency up to 266,000 plates m −1 in capillary electrochromatography and ability as solid phase microextraction for organic small molecules with good column permeability.
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Microbial Cell Factories
·
2022
·Vol. 21
·期 1
·1-14
·
IF 6.352
Liu Yan,Wang Xiaoliang,Nong Sujin,Bai Zehui,Han Nanyu,Wu Qian,Huang Zunxi,Ding Junmei
Background Carbamate pesticides have been widely used in agricultural and forestry pest control. The large-scale use of carbamates has caused severe toxicity in various systems because of their toxic environmental residues. Carbaryl is a representative carbamate pesticide and hydrolase/carboxylesterase is the initial and critical enzyme for its degradation. Whole-cell biocatalysts have become a powerful tool for environmental bioremediation. Here, a whole cell biocatalyst was constructed by displaying a novel carboxylesterase/hydrolase on the surface of Escherichia coli cells for carbaryl bioremediation.Results The carCby gene, encoding a protein with carbaryl hydrolysis activity was cloned and characterized. Subsequently, CarCby was displayed on the outer membrane of E. coli BL21(DE3) cells using the N-terminus of ice nucleation protein as an anchor. The surface localization of CarCby was confirmed by SDS–PAGE and fluorescence microscopy. The optimal temperature and pH of the engineered E. coli cells were 30 °C and 7.5, respectively, using pNPC4 as a substrate. The whole cell biocatalyst exhibited better stability and maintained approximately 8-fold higher specific enzymatic activity than purified CarCby when incubated at 30 °C for 120 h. In addition, ~ 100% and 50% of the original activity was retained when incubated with the whole cell biocatalyst at 4 ℃ and 30 °C for 35 days, respectively. However, the purified CarCby lost almost 100% of its activity when incubated at 30 °C for 134 h or 37 °C for 96 h, respectively. Finally, approximately 30 mg/L of carbaryl was hydrolyzed by 200 U of the engineered E. coli cells in 12 h.Conclusion sHere, a carbaryl hydrolase-containing surface-displayed system was first constructed, and the whole cell biocatalyst displayed better stability and maintained its catalytic activity. This surface-displayed strategy provides a new solution for the cost-efficient bioremediation of carbaryl and could also have the potential to be used to treat other carbamates in environmental bioremediation.
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NEW JOURNAL OF CHEMISTRY
·
2023
·
IF 3.3
Xiaomeng Liu,Yitian Zhong,Haosheng Feng,Yanxi Zhao,Qin Li,Tao Huang
The AgI/BiOI composites were prepared with BiOI nanosheets as the substrate by in-situ ion exchange and characterized by a series of characterization methods. The photocatalytic performance tests showed that the effective separation of photogenerated electron-hole pairs as well as the photocatalytic activities of the AgI/BiOI composites could be achieved by adjusting the Ag/Bi molar ratios, which may result in changes in composition and structure of AgI/BiOI composites. Among them, the AgI/BiOI-1.2 sample with a Ag/Bi molar ratio of 1.2 demonstrated Bi5O7I composition and the highest separation efficiency of photogenerated electron-hole pairs as well as the best photocatalytic performance for norfloxacin (NOR) photodegradation. More than 98.8% of NOR could be removed on over AgI/BiOI-1.2 within 120 min under the optimum conditions. Radical quenching experiments confirmed that the photo-generated holes and ∙O2‒ radicals played significant roles during the process of photocatalytic NOR degradation. A possible Z-type heterojunction mechanism for photocatalytic degradation of NOR over AgI/BiOI-1.2 was proposed.
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Journal of Physical Chemistry C
·
2023
·
IF 3.7
Yuanbo Gao,Chi Zhang,Man Fang,Yunchao Li,Louzhen Fan,Xiaohong Li
Oxidase-mimicking nanozymes are some of the most important nanozymes, which are investigated in various buffer concentrations. However, buffer concentration-dependent catalytic performance is rarely investigated. Herein, with o-phenylenediamine (OPD) as a substrate, the catalytic performance of Cu-Adenine oxidase mimic (fabricated with Cu2+ as an active center and adenine as a ligand) gradually decreases upon Tris–HCl buffer concentration (CTris–HCl) increasing from 10 to 200 mM, exhibiting buffer concentration-dependent catalytic activity. Such buffer concentration-dependent catalytic activity is believed to be because Tris–HCl and OPD competitively bind with Cu-Adenine, leading to differences in catalytic activity. Similarly, with 2,4-dichlorophenol (2,4-DP) as a substrate and 4-aminoantipyrine (4-AP) as a chromogenic agent, the same results are obtained. However, with 2,2′-azino-bis(3-ethylbenzothiazoline-6-sulfonic acid) (ABTS) and 3,3′,5,5′-tetramethylbenzidine (TMB) as substrates, the catalytic oxidation cannot be observed at CTris–HCl ≥ 50 mM. Tris–HCl and substrate competitively binding with Cu-Adenine produces buffer concentration-dependent catalytic performance. Subsequently, substrates are successfully expanded to other aromatic amines (p-phenylenediamine (PPD), 1,5-naphthalenediamine (1,5-NDA), 1,8-naphthalenediamine (1,8-NDA)) and phenols (phenol, 3-cresol, 1-naphthol). Based on the results, with 50 and 150 mM Tris–HCl buffer solutions as sensing channels, a Cu-Adenine-based colorimetric sensor array is constructed for discriminating four representative aromatic amines (OPD, PPD, 1,5-NDA, 1,8-NDA) and four phenols (2,4-DP, phenol, 3-cresol, 1-naphthol) as low as 50 μM. The performance is further validated through accurately identifying binary, quaternary, and even senary and octonary mixtures. Finally, the designed sensor array is successfully applied for identifying eight representative aromatic amines and phenols in river water, seawater, and sewage water, presenting great potential and valuable applications for large-scale scanning levels of aromatic amines and phenols in water samples.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 42
·19569-19577
·
IF 3.3
Xiaoqi Zhao,Xue Zhang,Yingxiao Li,Ling Liu,Yanfang Gao
Developing non-precious metal catalysts for the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is critical for Zn–air batteries. Herein, using NaCl and ammonium oxalate as templates to prepare a hierarchical porous Fe–N–C catalyst using an inorganic salt melting strategy is proposed. The prepared Fe–N–C-x catalysts have a hierarchical porous structure that increases the specific surface area, improves the exposure of a number of active sites and enhances the chance of contacting active sites. The structure change of a leaf-shaped zeolitic imidazolate framework (ZIF-L) during high-temperature pyrolysis was used to self-catalyze the growth of carbon nanotube structures, forming a structure of carbon nanotubes including Fe nanoparticles to provide additional active sites and reduce the aggregation of metal particles. From the perspective of economy and electrochemical performance, it is found that when the addition amount of NaCl and ammonium oxalate respectively is 2 g, the electrochemical performance of the ORR, OER and Zn–air batteries is better, and the preparation cost of the catalyst is more affordable. This strategy of forming hierarchical porous Fe–N–C catalysts by self-catalytic growth of Fe, N co-doped CNTs using inorganic salts provides a new design idea for the preparation of new hierarchical porous electrocatalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Haihong Wang,Huiyan Ma,Yan Li,Lin Cheng,Jucai Yang,Juming Liu
Efficient, low-cost, and easily scalable wide-spectral-responsive TiO2 photocatalysts are still extremely desired in driving photocatalytic degradation toward practical applications. In this work, a modified TiO2 with a narrow band gap and low valence band (VB) (CC-OV-TiO2) was successfully synthesized based on a facile sol–gel and low-temperature carbonization process, which can be used for the photocatalytic degradation and mineralization of a wide range of phenols. The results show that the interstitial doping of carbonates and the modification of surface oxygen vacancy (OV) defects together contribute to the formation of the VB tail states, which substantially narrow the band gap of TiO2 and widen the photoresponse range. Meanwhile, the carboxylated carbon species induce a substantial downward shift of the VB edge through coordination of the electron-withdrawing carboxyl groups, which further enhances the oxidation ability of the photogenerated holes. Accordingly, CC-OV-TiO2 with a narrow band gap and low VB exhibits superior and stable photocatalytic performance.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2021
·
IF 5.541
Yongdi He,Jinou Song,Yuan Zhuang,Jiuzhong Yang,Zhongwei Meng,Qiang Xu
An experimental study of 1-nitropropane (1-NP) pyrolysis was performed in a flow reactor at low pressure (4.0 kPa) in the temperature range of 623–973 K. The pyrolysis species was detected with the tunable synchrotron vacuum ultraviolet (VUV) photoionization and molecular-beam mass spectrometry (MBMS). Species from m/z = 15–87 were identified from near-threshold photoionization efficiency (PIE) spectra, such as radicals of CH 3 , C 2 H 5 , C 3 H 5 and C 3 H 7 ; isomers of C 2 H 4 O (ethenol and acetaldehyde), C 3 H 6 O (acetone and propanal), C 4 H 10 (butane and isobutane), HNC (hydrogen isocyanide), HCN (hydrogen cyanide)), C 3 H 5 N (ethyl isocyanide and species with unidentified structure) and C 3 H 5 NO (methoxyacetonitrile and species with unidentified structure). Their mole fraction profiles were evaluated at different temperature. Based on the mole fractions of species measured at the minimum temperature of 1-NP pyrolysis, some new channels of 1-NP primary pyrolysis were speculated, such as the channels involving O-transfer from N to C-atoms in different positions, deoxygenation, dehydrogenation and OH-abstraction. Based on the mechanisms proposed in the literature, the species produced from secondary or subsequent reactions were also discussed. These results are valuable to a further quantum mechanical calculation for a better understanding of 1-NP chemistry.
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PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
·
2021
·
IF 3.963
Jing-jing Xu,Yong-mei Chang,Mei Lu,Yuan Tie,Yan-ling Dong,Guang-you Chen,Zhi-qing Ma,Xi-li Liu,Yong-qiang Li
Carboxylesterases (CarEs) usually play critical roles in the detoxification of toxic chemicals and therefore may be involved in insecticide resistance in agricultural pests. Previous work has shown that CarE 001C from Helicoverpa armigera was able to metabolize the isomers of cypermethrin and fenvalerate . In this study, seven mutants of CarE 001C with single amino acid substitution were produced and expressed in the Escherichia coli. Enzyme kinetic analysis indicated that all seven mutations dramatically reduced enzymatic activities toward the generic substrate α -naphthyl acetate, but in vitro metabolism assay showed that two of the mutations, H423I and R322L, significantly improved hydrolase activities toward fenvalerate, with their recorded specific activities being 3.5 and 5.1 nM·s −1 ·mg −1 proteins, respectively. Further, thermostability assay showed that the stability of one mutant enzyme was enhanced. This study will help us better understand the potential of CarEs in insecticide detoxification and resistance in H. armigera .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Ying Liu,Runxia Wang,Haiyan Wang,Xijuan Yu,Xien Liu,Peng He,Xilin She,Tianrong Zhan
It is established that ultrathin layered double hydroxide nanosheets (LDHNS) and zeolitic imidazole frameworks (ZIF) are desirable electrochemical sensing modifiers owing to their large surface area and abundant catalytic sites. Integration of them is thus an effective solution to maximize their electrocatalytic activity . Herein, a novel reaction–diffusion framework (RDF) technique is applied for the in situ growth of ZIF-67 on ultrathin CoAl-LDHNS (CoAl-LDHNS@ZIF-67). In a confined space of the agar gel matrix of RDF, the coordination reaction between organic ligands and CoAl-LDHNS without an additional Co 2+ source achieves the controllable growth of ZIF-67 crystals through a long vertical diffusion . The prepared composite comprises both CoAl-LDHNS and ZIF-67 components with a certain ratio and provides a large surface area and amply catalytic sites, thus realizing a rapid transfer of electron and mass. The CoAl-LDHNS@ZIF-67 modified electrode is employed for the simultaneous detection of naphthol isomers by differential pulse voltammetry . Naphthol isomers display anodic reactions with a wide peak potential difference, allowing their simultaneous detection feasible. Voltammetric responses of α-naphthol and β-naphthol follow good linearity against the concentration in a wide range from 0.3 to 150 μM with limits of detection of 54 and 82 nM, respectively. The proposed sensor also demonstrates excellent selectivity , stability, reproducibility, and practicability for the simultaneous detection of naphthol isomers.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2021
·Vol. 413
·期 11
·3017-3026
·
IF 4.157
Ren Zixuan,Zhou Xingchen,Gao Xingxing,Tan Yan,Chen Huaying,Tan Songwen,Liu Wenfang,Tong Yaonan,Chen Chuanpin
The long-term consumption of food with pesticide residues has harmful effects on human health and the demand for pesticide detection technology tends to be miniaturized and instant. To this end, we demonstrated the first application of indirectly detecting two carbamate pesticides, metolcarb and carbaryl, by gold nanoparticle–modified indium tin oxide electrode in dual-channel microchip electrophoresis and amperometric detection (ME-AD) system. m -Cresol and α -naphthol were obtained after pesticide hydrolysis in alkaline solution, and then separated and detected by ME-AD. Parameters including the detection potential and running buffer concentration and pH were optimized to improve the detection sensitivity and separation efficiency. Under the optimal conditions, the two analytes were completely separated within 80 s. m -Cresol and α -naphthol presented a wide linear range from 1 to 100 μM, with limits of detection of 0.16 μM and 0.34 μM, respectively (S/ N = 3). Moreover, the reliability of this system was demonstrated by analyzing metolcarb and carbaryl in spiked vegetable samples. Graphical abstract
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 28
·15678-15683
·
IF 12.732
Shuli Yin,Songliang Liu,Shiqian Jiao,Hugang Zhang,You Xu,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Benefiting from the interaction of inorganic and organic building blocks, the design of metal–organic nanohybrids is of great significance for the oxygen reduction reaction (ORR). Herein, a universal strategy is presented to controllably synthesize tannic acid (TA) functionalized AuPd lavender-like nanochains (AuPd@TA LCs) by a chemical reduction method at low temperature. Due to the unique structural characteristics and polyphenolic modification, the AuPd@TA LCs show superior ORR performance in an alkaline electrolyte. Moreover, the surface decorated TA polymers can act as a molecular screen window to prevent methanol molecules from accessing the active site of the catalyst, thus resulting in high methanol tolerance and catalytic stability. The presented molecular screen window strategy is highly valuable for designing ORR electrocatalysts with high methanol tolerance.
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