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Immobilization of laccase on organic–inorganic nanocomposites and its application in the removal of phenolic

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 867-879 doi: 10.1007/s11705-022-2277-5

摘要： Polydopamine-functionalized nanosilica was synthesized using an inexpensive and easily obtainable raw material, mild reaction conditions, and simple operation. Subsequently, a flexible spacer arm was introduced by using dialdehyde starch as a cross-linking agent to bind with laccase. A high loading amount (77.8 mg∙g‒1) and activity retention (75.5%) could be achieved under the optimum immobilization conditions. Thermodynamic parameters showed that the immobilized laccase had a lower thermal deactivation rate constant and longer half-life. The enhancement of thermodynamic parameters indicated that the immobilized laccase had better thermal stability than free laccase. The residual activity of immobilized laccase remained at about 50.0% after 30 days, which was 4.0 times that of free laccase. Immobilized laccase demonstrated excellent removal of phenolic pollutants (2,4-dichlorophenol, bisphenol A, phenol, and 4-chlorophenol) and perfect reusability with 70% removal efficiency retention for 2,4-dichlorophenol after seven cycles. These results suggested that immobilized laccase possessed great reusability, improved thermal stability, and excellent storage stability. Organic–inorganic nanomaterials have a good application prospect for laccase immobilization, and the immobilized laccase of this work may provide a practical application for the removal of phenolic pollutants.

关键词： polydopamine     pollutant removal     thermodynamic     phenolic pollutants     immobilized laccase    

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Enhanced production of laccase by

Wei SUN, Meiying XU, Chunyu XIA, Anhua LI, Guoping SUN

《环境科学与工程前沿（英文）》 2013年 第7卷 第2期   页码 200-210 doi: 10.1007/s11783-012-0457-0

摘要： The effect of physical parameters of cultivation (load volume, temperature, pH, agitation, inoculum size, and incubation period) in the production of laccase by wood-rotting basidiomycete were studied using diluted molasses distillery wastewater (MDW) as a major composition. Using fractional factorial design, our study first identified load volume, agitation, and inoculum size as statistically significant factors. Optimal preferences and mutual interactions of the factors were then determined by the response surface method, which is based on the center composite design. A quadratic model was used to fit the experimental data. The optimized operational parameters for laccase production were determined to be the following: culture temperature of 25°C, pH 4, load volume of 40 mL diluted MDW in 150 mL flask, agitation rate of 183 r·min , inoculation of 11.5% v/v, and cultivation time of 6 d. The experimental validation under these conditions (the maximum laccase production of 2198.2 U·mL was within the confidence interval) subsequently verified the accuracy of the constructed model. Moreover, the removal of chemical oxygen demand and nitrogen of MDW reached 62.85% and 48.00% respectively, and the decolorization ratio under the optimal condition was 41.85%. The enhanced production of laccase by is a new recovery strategy for MDW.

关键词： laccase     Coriolus hirsutus     fractional factorial design     response surface method     molasses distillery wastewater    

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Immobilized

Pei MA, Dan ZHANG

《环境科学与工程前沿（英文）》 2012年 第6卷 第4期   页码 498-508 doi: 10.1007/s11783-012-0429-4

摘要： To investigate the potential use of ( ) residue for Cd adsorption, poly alcohol Na alginate (PVA) was applied to immobilize it. The parameters including contact time, pH, adsorbent dosages, and coexisting metal ions were studied. The suitable pH for immobilized was 4–7 wider than that for raw (pH 6–7). In the presence of Pb concentration varying from 0 to 30 mg·L , the Cd adsorption ratios declined by 6.71% and 47.45% for immobilized and raw , respectively. While, with the coexisting ion Cu concentration varied from 0 to 30 mg·L , the Cd adsorption ratios declined by 12.97% and 50.56% for immobilized and raw , respectively. The Cd adsorption isotherms in single–metal and dual-metal solutions were analyzed by using Langmuir, Freundlich, and Dubinin–Radushkevich models. The Cd adsorption capacities ( ) in single-metal solution were 6.448 mg·L and 2.832 mg·L for immobilized and raw , respectively. The of immobilized were 1.850 mg Cd·g in Cd + Pb solution and 3.961 mg Cd·g in Cd + Cu solution, respectively. The Cd adsorption processes subjected to both adsorbents follow pseudo-second-order model. Mechanism study showed the functional group of was –OH, –NH, –CO, and PVA played an important role in metal adsorbing. Mining wastewater treatment test showed that PVA–SA-immobilized was effective in mixed pollutant treatment even for wastewater containing metal ions in very low concentration.

关键词： immobilization     Lentinus edodes residue     competitive adsorption     isotherm    

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Removal of 17β-estradiol in laccase catalyzed treatment processes

XIA Qing,KONG Deyang,LIU Guoqiang,HUANG Qingguo,ALALEWI Aamr,LU Junhe

《环境科学与工程前沿（英文）》 2014年 第8卷 第3期   页码 372-378 doi: 10.1007/s11783-013-0567-3

摘要： The removal of 17β-estradiol (E2) in laccase catalyzed oxidative coupling processes was systematically studied in this work. We focused on the influence of pH and natural organic matter (NOM) on the performance of the enzymatic treatment processes. It was found that the optimal pH for E2 removal was between 4 and 6. The removal of E2 was slightly inhibited in the presence of NOM. Enzymatic transformation of E2 was second-order in kinetics with first-order to both the concentrations of the enzyme and contaminant. Mass spectrum (MS) analysis suggested that coupling products were formed through radical-radical coupling mechanism. The results of this study demonstrated that laccase catalyzed oxidative coupling process could potentially serve as a treatment strategy to control steroid estrogens.

关键词： 17β-estradiol     laccase     oxidative coupling processes     kinetics     mechanisms    

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Transformation of triclosan by a novel cold-adapted laccase from

Yuanyuan Shi, Deyang Kong, Jiayang Liu, Junhe Lu, Xiaoming Yin, Quansuo Zhou

《环境科学与工程前沿（英文）》 2017年 第11卷 第3期 doi: 10.1007/s11783-017-0927-5

摘要： This work investigated the transformation of triclosan (TCS) by laccase produced by a pathogen isolated from rotten tomato. The pathogen was characterized as sp. FQ, belonging to subphylum . The laccase exhibited cold-adaptation with relatively high activity at 20°C. The laccase could effectively transform TCS. Approximately 62% TCS could be removed at dose of 1.0 unit·mL in 120 min. The reaction rate appeared to be to the concentration of the substrate, suggesting the laccase activity remained stable during the reaction. Transformation products of TCS were analyzed by mass spectrometry and it was revealed that TCS dimers were formed via radical coupling pathways. During this process, laccase catalyzed oxidation of TCS to form a radical intermediate is the rate limiting step. However, this step can be reversed by humic acid. Overall, the laccase showed great potential in the treatment of phenolic contaminants. Since laccase is widely presented in natural environment, this study also revealed an important pathway involved in the transformation of phenolic contaminants in the environment.

关键词： Laccase     Botrytis cinerea     Triclosan     Transformation     Kinetics    

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Biomineralization-inspired copper-cystine nanoleaves capable of laccase-like catalysis for the colorimetric

Miao Guan, Mengfan Wang, Wei Qi, Rongxin Su, Zhimin He

《化学科学与工程前沿（英文）》 2021年 第15卷 第2期   页码 310-318 doi: 10.1007/s11705-020-1940-y

摘要： Recently, many efforts have been dedicated to creating enzyme-mimicking catalysts to replace natural enzymes in practical fields. Inspired by the pathological biomineralization behaviour of L-cystine, in this study, we constructed a laccase-like catalyst through the co-assembly of L-cystine with Cu ions. Structural analysis revealed that the formed catalytic Cu-cystine nanoleaves (Cu-Cys NLs) possess a Cu(I)-Cu(II) electron transfer system similar to that in natural laccase. Reaction kinetic studies demonstrated that the catalyst follows the typical Michaelis-Menten model. Compared with natural laccase, the Cu-Cys NLs exhibit superior stability during long-term incubation under extreme pH, high-temperature or high-salt conditions. Remarkably, the Cu-Cys NLs could be easily recovered and still maintained 76% of their activity after 8 cycles. Finally, this laccase mimic was employed to develop a colorimetric method for epinephrine detection, which achieved a wider linear range (9–455 μmol·L ) and lower limit of detection (2.7 μmol·L ). The Cu-Cys NLs also displayed excellent specificity and sensitivity towards epinephrine in a test based on urine samples.

关键词： biomineralization     laccase     L-cystine     colorimetric detection     enzyme mimic    

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Degradation of bisphenol A by microorganisms immobilized on polyvinyl alcohol microspheres

Xue BAI, Hanchang SHI, Zhengfang YE, Qiujin SUN, Qing WANG, Zhongyou WANG

《环境科学与工程前沿（英文）》 2013年 第7卷 第6期   页码 844-850 doi: 10.1007/s11783-013-0487-2

摘要： In this study, microorganisms (named B111) were immobilized on polyvinyl alcohol microspheres prepared by the inverse suspension crosslinked method. The biodegradation of bisphenol A (BPA) and 4-hydroxybenzaldehyde, a degradation product of BPA, by free and immobilized B111 was investigated. The BPA degradation studies were carried out at initial BPA concentrations ranging from 25 to 150 mg·L . The affinity constant K and maximum degradation rate were 98.3 mg·L and 19.7 mg·mg VSS·d for free B111, as well as 87.2 mg·L and 21.1 mg·mg VSS·d for immobilized B111, respectively. 16S rDNA gene sequence analyses confirmed that the dominant genera were and for BPA biodegradation in microorganisms B111.

关键词： bisphenol A     polyvinyl alcohol     immobilized microorganisms     4-hydroxybenzaldehyde    

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Mercury removal and recovery by immobilized

Meifang CHIEN, Ryo NAKAHATA, Tetsuya ONO, Keisuke MIYAUCHI, Ginro ENDO

《化学科学与工程前沿（英文）》 2012年 第6卷 第2期   页码 192-197 doi: 10.1007/s11705-012-1284-3

摘要： From several mercury removing microorganisms, we selected MB1, which is non-pathogenic, broad-spectrum mercury resistant, mercuric ion reducing, heat tolerant, and spore-forming, as a useful bacterium for bioremediation of mercury pollution. In this study, mercury removal performance of the immobilized MB1 was investigated to develop safe, efficient and stable catalytic bio-agent for mercury bioremediation. The results showed that the alginate gel immobilized MB1 cells efficiently removed 80% of mercury from the solution containing 10 mg/L mercuric chloride within 24 h. These cells still had high activity of mercury removal even after mercuric ion loading was repeated for nine times. The analysis of mercury contents of the alginate beads with and without immobilized MB1 suggested that a large portion of reduced metallic mercury was trapped in the gel beads. It was concluded that the alginate gel immobilized MB1 cells have potential to remove and recover mercury from mercury-containing water.

关键词： mercury removal     immobilized bacteria     alginate gel     bioremediation    

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Enhanced methane production during long-term UASB operation at high organic loads as enabled by the immobilized

《环境科学与工程前沿（英文）》 2022年 第16卷 第6期 doi: 10.1007/s11783-021-1505-4

摘要：

• Fungi enable the constant UASB operation even at OLR of 25.0 kg/(m3×d).

关键词： Anaerobic digestion     Fungi     Methane production     High OLR     Microbial community    

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of dilution rate on dynamic and steady-state biofilm characteristics during phenol biodegradation by immobilized

Veena Bangalore Rangappa, Vidya Shetty Kodialbail, Saidutta Malur Bharthaiyengar

《环境科学与工程前沿（英文）》 2016年 第10卷 第4期 doi: 10.1007/s11783-016-0863-9

摘要： Continuous pulsed plate bioreactor (PPBR) was used for phenol biodegradation. cells immobilized on granular activated carbon was used. Dynamic and steady state biofilm characteristics depend on dilution rate (DR). Lower DR favour phenol degradation and uniform, thick biofilm formation. Exo polymeric substance production in biofilm are favoured at lower dilution rates. Pulsed plate bioreactor (PPBR) is a biofilm reactor which has been proven to be very efficient in phenol biodegradation. The present paper reports the studies on the effect of dilution rate on the physical, chemical and morphological characteristics of biofilms formed by the cells of Pseudomonas desmolyticum on granular activated carbon (GAC) in PPBR during biodegradation of phenol. The percentage degradation of phenol decreased from 99% to 73% with an increase in dilution rate from 0.33 h?1 to 0.99 h?1 showing that residence time in the reactor governs the phenol removal efficiency rather than the external mass transfer limitations. Lower dilution rates favor higher production of biomass, extracellular polymeric substances (EPS) as well as the protein, carbohydrate and humic substances content of EPS. Increase in dilution rate leads to decrease in biofilm thickness, biofilm dry density, and attached dry biomass, transforming the biofilm from dense, smooth compact structure to a rough and patchy structure. Thus, the performance of PPBR in terms of dynamic and steady-state biofilm characteristics associated with phenol biodegradation is a strong function of dilution rate. Operation of PPBR at lower dilution rates is recommended for continuous biologic treatment of wastewaters for phenol removal.

关键词： Biofilm     Exopolymeric substances     Phenol     Dilution rate     Pulsed plate bioreactor    

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Regioselective acylation of pyridoxine catalyzed by immobilized lipase in ionic liquid

BAI Shu, REN Mengyuan, WANG Lele, SUN Yan

《化学科学与工程前沿（英文）》 2008年 第2卷 第3期   页码 301-307 doi: 10.1007/s11705-008-0060-x

摘要： The regioselective acylation of pyridoxine catalyzed by immobilized lipase () in 1-butyl-3-methylimidazolium hexafluorophosphate ([BMIM]PF) has been investigated, and compared with that in acetonitrile (ACN). The acetylation of pyridoxine using acetic anhydride in [BMIM]PF gave comparable conversion of pyridoxine to 5-monoacetyl pyridoxine with considerably higher regioselectivity (93%–95%) than that in ACN (70%–73%). Among the tested parameters, water activity () and temperature have profound effects on the reaction performances in either [BMIM]PF or ACN. For the reaction in [BMIM]PF, higher temperature (50°C–55°C) and lower (<0.01) are preferable conditions to obtain better conversion and regioselectivity. Mass transfer limitation and intrinsic kinetic from the ionic nature of ionic liquids (ILs) may account for a different rate-temperature profile and a lower velocity at lower temperature in [BMIM]PF-mediated reaction. Moreover, consecutive batch reactions for enzyme reuse also show that lipase exhibited a much higher thermal stability and better reusability in [BMIM]PF than in ACN, which represents another advantage of ILs as an alternative to traditional solvents beyond green technology.

关键词： ACN     stability     1-butyl-3-methylimidazolium hexafluorophosphate     different rate-temperature     alternative    

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Extraction and biodegradation of ginkgolic acids from

Qi LI, Wei SUN, Yan JIANG, Fuliang CAO, Guibin WANG, Linguo ZHAO

《农业科学与工程前沿（英文）》 2017年 第4卷 第4期   页码 465-472 doi: 10.15302/J-FASE-2017181

摘要： Ginkgolic acids are unwanted constituents in standard leaves extracts. Thus, for the quality control of ginkgo extracts, it is important to establish an effective degradation method, with high catalytic efficiency and safety, to remove ginkgolic acids. Laccases are oxidases with potential for application in elimination of hazardous phenolic compounds. In this study, single-factor and orthogonal experiments were used to optimize extraction of ginkgolic acid from sarcotestae. The results showed that ethanol was the best solvent, with the highest extraction rate for ginkgolic acid at 85% ethanol. On this basis, we measured ethanol volume fraction, extraction time, temperature and solid-liquid ratio using an orthogonal experiment. By using absorbance of 310 nm as standard, the optimal extraction conditions were 85% ethanol with, solid-liquid ratio of 1:14 at 40°C for 12 h. These conditions gave a ginkgolic acid yield of 73.1 mg·g . Subsequently, recombinant laccase was used to degrade the ginkgolic acid in several laccase/mediator systems, of which LacC was the best. At 50°C, pH 4.5, enzyme concentration of 0.01 U·mL , 0.5 mmol·L mediator ABTS and reaction time of 3 h, the degradation rate of ginkgolic acid reached 100%. These results lay the foundation for research on and application of biological enzymes for detoxification of extracts.

关键词： biodegradation     extraction     ginkgolic acid     laccase     orthogonal method    

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A magnetic adsorbent based on salicylic acid-immobilized magnetite nano-particles for pre-concentration

Hossein Abdolmohammad-Zadeh, Arezu Salimi

《化学科学与工程前沿（英文）》 2021年 第15卷 第2期   页码 450-459 doi: 10.1007/s11705-020-1930-0

摘要： In this research, an eco-friendly magnetic adsorbent based on Fe O /salicylic acid nanocomposite was fabricated using a facile one-pot co-precipitation method. The crystalline and morphological characterization of the prepared nanocomposite was performed by field emission scanning electron microscopy, X-ray diffraction, and Fourier transform infrared spectroscopy. The nanocomposite was employed as a magnetic solid-phase extraction agent for separation of Cd(II) ions from synthetic solutions. Some experimental factors affecting the extraction efficiency were investigated and optimized. Following elution with acetic acid (pH 3.5), the pre-concentrated analyte was quantified by flame atomic absorption spectrometry. In optimal conditions, a linear calibration graph was achieved in the concentration range of 0.2‒30 ng·mL with a determination coefficient ( ) of 0.9953. The detection limit, the enhancement factor, inter- and intra-day relative standard deviations (for six consecutive extractions at the concentration level of 10 ng·mL ) were 0.04 ng·mL , 100, 2.38% and 1.52%, respectively. To evaluate the accuracy of the method, a certified reference material (NIST SRM 1643e) was analyzed, and there was a good agreement between the certified and the measured values. It was successfully utilized to determine cadmium in industrial wastewater samples and the attained relative recovery values were between 96.8% and 103.2%.

关键词： cadmium     magnetic solid-phase extraction     Fe3O4 nanoparticles     Fe3O4/salicylic acid nanocomposite     flame atomic absorption spectrometry    

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Pentachlorophenol (PCP) degradation microorganism community structure under microaeration condition

Chen Yuancai, Hao Yuan, Fu Shiyu, Zhan Huaiyu

《化学科学与工程前沿（英文）》 2007年 第1卷 第4期   页码 411-415 doi: 10.1007/s11705-007-0075-8

摘要： The comparison of pentachlorophenol (PCP) degradation was conducted under micro-aeration and anaerobic condition with three series of batch experiment, results of which indicated that during micro-aeration condition co-immobilized of anaerobic granular sludge and isolated aerobic bacterial species could enhance the efficiency of PCP reduction through the synergism of aerobes and anaerobes reductive dechlorination and exchange of metabolites within the co-immobilized granular sludge. While during anaerobic condition, there was no great difference in the three series. The specific activities experiment further confirmed that strict anaerobes were not affected over the presence of micro aeration environment. Microorganism community construction of co-immobilized anaerobic granular sludge and the mixed isolated aerobic community was also deduced. By the efficient cooperation of aerobes and anaerobes, the high efficiency removal rate of PCP was implemented.

关键词： comparison     co-immobilized anaerobic     anaerobic granular     exchange     PCP    

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Response of bioaerosol cells to photocatalytic inactivation with ZnO and TiO impregnated onto Perlite and Poraver carriers

《环境科学与工程前沿（英文）》 2021年 第15卷 第3期 doi: 10.1007/s11783-020-1335-9

摘要：

•ZnO/Perlite inactivated 72% of bioaerosols in continuous gas phase.

关键词： Immobilized catalysts     Continuous flow     Photocatalysis     Bioaerosols     Cytotoxicity     Inactivation mechanism    

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标题 作者 时间 类型 操作

Immobilization of laccase on organic–inorganic nanocomposites and its application in the removal of phenolic

期刊论文

Enhanced production of laccase by

Wei SUN, Meiying XU, Chunyu XIA, Anhua LI, Guoping SUN

期刊论文

Immobilized

Pei MA, Dan ZHANG

期刊论文

Removal of 17β-estradiol in laccase catalyzed treatment processes

XIA Qing,KONG Deyang,LIU Guoqiang,HUANG Qingguo,ALALEWI Aamr,LU Junhe

期刊论文

Transformation of triclosan by a novel cold-adapted laccase from

Yuanyuan Shi, Deyang Kong, Jiayang Liu, Junhe Lu, Xiaoming Yin, Quansuo Zhou

期刊论文

Biomineralization-inspired copper-cystine nanoleaves capable of laccase-like catalysis for the colorimetric

Miao Guan, Mengfan Wang, Wei Qi, Rongxin Su, Zhimin He

期刊论文

Degradation of bisphenol A by microorganisms immobilized on polyvinyl alcohol microspheres

Xue BAI, Hanchang SHI, Zhengfang YE, Qiujin SUN, Qing WANG, Zhongyou WANG

期刊论文

Mercury removal and recovery by immobilized

Meifang CHIEN, Ryo NAKAHATA, Tetsuya ONO, Keisuke MIYAUCHI, Ginro ENDO

期刊论文

Enhanced methane production during long-term UASB operation at high organic loads as enabled by the immobilized

期刊论文

of dilution rate on dynamic and steady-state biofilm characteristics during phenol biodegradation by immobilized

Veena Bangalore Rangappa, Vidya Shetty Kodialbail, Saidutta Malur Bharthaiyengar

期刊论文

Regioselective acylation of pyridoxine catalyzed by immobilized lipase in ionic liquid

BAI Shu, REN Mengyuan, WANG Lele, SUN Yan

期刊论文

Extraction and biodegradation of ginkgolic acids from

Qi LI, Wei SUN, Yan JIANG, Fuliang CAO, Guibin WANG, Linguo ZHAO

期刊论文

A magnetic adsorbent based on salicylic acid-immobilized magnetite nano-particles for pre-concentration

Hossein Abdolmohammad-Zadeh, Arezu Salimi

期刊论文

Pentachlorophenol (PCP) degradation microorganism community structure under microaeration condition

Chen Yuancai, Hao Yuan, Fu Shiyu, Zhan Huaiyu

期刊论文

Response of bioaerosol cells to photocatalytic inactivation with ZnO and TiO impregnated onto Perlite and Poraver carriers

期刊论文