COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Zi-Wen Zhou,Chun-Xiu Liu,Chun-Xian Cai,Na Wang,Xiao-Qi Yu
In this work, PEG modified photocatalytic covalent organic framework (PEG@CTF-OMe) was co-immobilized with laccase into Cu doping calcium alginate gel beads (Ca/Cu-PEG@CTF-OMe-lac). PEG@CTF-OMe improved the light stability of laccase under blue light irradiation , and external introduction of copper into gel beads stabilized the conformation and improved pH adaptability of laccase. With the help of 2,2-binamine-di-3-ethylbenzothiazolin-6-sulfonic acid (ABTs), the immobilized laccase (Ca/Cu-PEG@CTF-OMe-lac) presented outstanding synergistic removal of pollutants by photocatalysis and enzymatic catalysis, as well as ABTs radicals generation promoting by copper ions in the laccase-mediator system. The removal recyclability performance assay found that the Ca/Cu-PEG@CTF-OMe-lac gel beads had more than 80 % removal efficiency for phenol , 4-chlorophenol, 2,4-dichlorophenol, nonyl phenol, bisphenol A and indole in water at 25 °C after 5 cycles, when the concentration reached as high as 70 mg/L, 60 mg/L, 120 mg/L, 100 mg/L, 100 mg/L and 100 mg/L, respectively. The high synergistic removal performance obtained by the gel beads co-immobilizing laccase and photocatalytic CTFs showed greater practical application value.
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Sustainable Chemistry and Pharmacy
·
2023
·
IF 6
Qiuyun Zhang,Yaping Wu,Xingyue Hong,Zhenying Li,Yanting Lei,Rongfei Yu,Taoli Deng,Yutao Zhang,Peihua Ma
Different ligand functionalized bimetallic organic framework ((Zr/Ce)UiO-66- X ( X = H, NO 2 , NH 2 and (OH) 2 ) solids-supported phosphotungstic acid (HPW) has been fabricated through a facile impregnation process, and used in the esterification of methanol with oleic acid (OA). The obtained composites were characterized by FTIR , XRD, NH 3 -TPD, SEM-EDS, N 2 adsorption-desorption isotherm, TG , Py-FTIR, and XPS. The characterization analysis shows that the HPW/(Zr/Ce)UiO-66-NO 2 composite possesses the proper catalytic features, such as the greatest number of both strong Brønsted and Lewis acid sites, wider pores, relatively high surface area, and the existence of synergistic catalytic effects between HPW and (Zr/Ce)UiO-66-NO 2 framework. In the screening, the maximum OA conversion rate using (Zr/Ce)UiO-66-NO 2 , HPW/(Zr/Ce)UiO-66-NO 2 , HPW/(Zr/Ce)UiO-66, HPW/(Zr/Ce)UiO-66-NH 2 , HPW/(Zr/Ce)UiO-66-(OH) 2 catalysts is 13.7%, 91.6%, 81.6%, 80.7%, and 72.6% at 110 °C for 3 h, respectively. Moreover, the HPW/(Zr/Ce)UiO-66-NO 2 catalyst presents the better reusability over four cycles. Besides these, the HPW/(Zr/Ce)UiO-66-NO 2 catalyzed esterification reaction is estimated to have an activation energy of 33.7 kJ/mol. This present study provides an effective route for realizing biofuel production on an industrial scale involving heteropolyacids/bimetallic MOFs synergistic catalysts.
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BIOPROCESS AND BIOSYSTEMS ENGINEERING
·
2021
·Vol. 44
·期 10
·2193-2204
·
IF 3.21
He Song,Wu Xiaomei,Ma Baodi,Xu Yi
The novel Ni-NTA-functionalized magnetic chitosan microspheres (MCS-NTA-Ni) were prepared via amino functionalization of MCS with epichlorohydrin and ethylenediamine, followed by the introduction of the aldehyde groups and NTA in turn, and nickel (II) ions were chelated in the end. MCS-NTA-Ni contained numerous long-armed NTA-Ni surface groups, ensuring high enzyme loading and providing more space and flexibility to attach enzymes and maintain their activity. This microsphere can have highly selective adsorption of his-tagged recombinant protein. The his-tagged recombinant Microbacterium esterase of E. coli BL21 (DE3)/pET21a-EstSIT01 was first immobilized on MCS-NTA-Ni by affinity fixation, giving high immobilization yield (90.1%) and enzyme loading (120 mg/g). Compared with free esterase, the immobilized esterase was found to exhibit higher pH stability and thermal stability. In addition, the immobilized esterase had excellent reusability for the synthesis of key chiral intermediate of d -biotin and the substrate conversion could still keep 100% after 8 cycles continuously.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Hongpo Zhou,Yang Zhou,Juan Xu,Lanxiang Liu,Jinju Ma,Wenwen Zhang,Kun Li,Hong Zhang,Kai Li
We report a feasible and universal approach to fabricate nanocarbon material (NCM) coatings onto a wide range of silicon-based substances. Benefitting from the phenolic hydroxyl and star-shaped branched molecular structure, tannic acid (TA) could act as a functional agent for immobilization and fixation of NCMs in the aqueous phase. More specifically, steered molecular dynamics simulations verified that some unionized chains of TA could tightly attach to the NCM’s surface in the neutral aqueous environment by π–π stacking interactions, and other free arms with ionized phenolic hydroxyl could act as surface charges of the TA/NCM coacervates, resulting in enhanced colloidal stability of this dispersion. Subsequently, these free arms could also interact with the aminated silicon-based substances, enabling TA to act as a “bridge” between the NCM and the silicon-based substances to form the nanocarbon coating. The obtained polydimethylsiloxane with TA/NCM coating represents favorable electrical and thermal conductivity along with excellent electromechanical performance under the cyclic compression-release test. This strategy is a great improvement for the fabrication of NCM layers and devices, which is not necessary to make the hydrophilic modification of NCM and beneficial to enhance the interaction between the carbon layer and substrate, avoiding the coating separation from the substances.
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY
·
2016
·Vol. 182
·期 2
·482-494
·
IF 1.606
Bai Yin,Zhou Wen-Di,Mu Xian-Min,Zhang Qian,Yu Chen,Di Bin,Su Meng-Xiang
Human 17β-hydroxysteroid dehydrogenase type 1 (17β-HSD1), a potential target in breast cancer prevention and therapy, was extracted from human placenta and immobilized on nonporous silica (∼5 μm) with a covalent method for the first time. The optimum initial enzyme concentration and immobilization time during the immobilization process were 0.42 mg mL −1 and 12 h, repectively. The binding was confirmed by scanning electron microscope (SEM) and infrared spectroscopy (FT-IR). It could improve the pH, thermal and storage stability compared to free enzyme. Moreover, the immobilized enzyme could be reused at least four times. A screening method based on it coupled with liquid chromatography–time-of-flight mass spectrometer (LC-TOF/MS) was established, and the half-maximal inhibitory concentration (IC 50) of apigenin for the immobilized enzyme was 291 nM. Subsequently, 10 natural products were evaluated leading to inhibition of the activity of 17β-HSD1 at the concentration of 25 μM, and six of them inhibit the activity over 50%.
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FOOD CHEMISTRY
·
2024
·
IF 8.5
Xiaoxiao Liu,Kai Li,Luona Ye,Xinghong Cao,Pengbo Wang,Xiaoman Xie,Min Yang,Li Xu,Yunjun Yan,Jinyong Yan
We propose a co-immobilized chemo-enzyme cascade system to mitigate random intermediate diffusion from the mixture of individual immobilized catalysts and achieve a one-pot reaction of multi-enzyme and reductant. Catalyzed by lipase and lipoxygenase, unsaturated lipid hydroperoxides (HPOs) were synthesized. 13( S )-hydroperoxy-9Z, 11E-octadecadienoic acid (13-HPODE), one compound of HPOs, was subsequently reduced to 13( S )-hydroxy-9Z, 11E-octadecadienoic acid (13-HODE) by cysteine. Upon the optimized conditions, 75.28 mg of 13-HPODE and 4.01 mg of 13-HODE were produced from per milliliter of oil. The co-immobilized catalysts exhibited improved yield compared to the mixture of individually immobilized catalysts. Moreover, it demonstrated satisfactory durability and recyclability, maintaining a relative HPOs yield of 78.5% after 5 cycles. This work has achieved the co-immobilization of lipase, lipoxygenase and the reductant cysteine for the first time, successfully applying it to the conversion of soybean oil into 13-HODE. It offers a technological platform for transforming various oils into high-value products.
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Scientific Reports
·
2024
·Vol. 14
·期 1
·1-12
·
IF 3.8
Ainiwaer Meihaguli,Jia Hongtao,Zhang Tuo,Huang Jiaqing,Zhang Nan,Yin Xianqiang,Peng Limei,Li Hongbin,Zeng Xibai
Sepiolite-modified nano-zero-valent iron (S-nZVI) is used as an amendment and incubated to remediate As-Cd-contaminated soil under three different soil‒water management conditions [moderately wet (MW), continuously flooded (CF) and alternately wet and dry (AWD)]. The results showed that soil pH is in the order of CF > AWD > MW. The soil pH increased approximately 0.5 to 1 unit by 3% and 5% doses after 36 d of incubation. Soil pH was negatively correlated with available As-Cd content under the three water regimes ( p < 0.01). All doses of S-nZVI significantly reduced soil available As-Cd under the three soil moistures by 45-80% for As and 5-45% for Cd. Moreover, S-nZVI addition also promoted the transformation of As-Cd in the acid-extracted fraction, oxidation fraction, and reduced fraction to a more stable residue fraction. High-throughput sequencing results showed that high doses of S-nZVI had a significant adverse effect on soil bacterial diversity and richness. After 36 d of incubation, the Chao1 index and the Shannon index were significantly decreased in MW, CF, and AWD, respectively. Decreasing the S-nZVI dose and increasing the incubation time simultaneously reduced As-Cd availability and S-nZVI ecotoxicity in the soil, thereby effectively maintaining the survivability of the original dominant bacteria, increasing the soil pH, and promoting the interaction between dominant bacteria and soil factors in As-Cd cocontaminated soil.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Pengyu Zhang,Jin Fan,Xiaoyun Xu,Zibo Xu,Yulu Yu,Ling Zhao,Hao Qiu,Xinde Cao
Zero-valent iron-embedded biochar (ZVI/BC) is considered as an effective material for arsenic (As) immobilization in soil, but the stability of As after remediation against aging remains unknown. Herein, the effects of dry-wet and freeze-thaw aging on the immobilization of As in two As-contaminated soils amended by ZVI/BC were evaluated. ZVI/BC showed high immobilization capacity for As-contaminated soils with an over 82% decrease of bioavailable As, mainly due to the As-Fe co-precipitation accompanied with ZVI oxidation. The aging of dry-wet and freeze-thaw had an opposite effect on the bioavailability of As. After 35 rounds of dry-wet aging, bioavailable As concentration increased from 1.25‐9.50 to 1.83‐21.75 mg/kg, because of the oxidation dissolution of ZVI and the formation of mobile reduced As(III). By contrast, the crystallization of amorphous iron with the structural incorporation of sorbed As and the oxidation of As(III) into stable As(V) occurred during the 35 rounds of freeze-thaw aging, leading to the decrease of bioavailable As concentration from 9.50‐1.25 to 5.42‐0.45 mg/kg. Our results revealed that the stability of soil As after remediation by ZVI/BC varied with the different aging process, which needs more consideration for the long-term soil As immobilization in the different whether areas.
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ENERGY & FUELS
·
2022
·
IF 4.654
Xue-Lei Duan,Yuan-Ming Cao,Chong Gao,Sheng-Li Niu,Yi-Wen Shen,Qi Guo,Jiao-Jiao Xie,Kai-Qiang He,Chun-Gang Yuan
One novel/multifunctional selenium-doped SrFeO3-δ/HNTs composite was fabricated and used for immobilization of gaseous mercury. The composite showed excellent performances for Hg0 removal via adsorption coupled with photocatalytic oxidation in visible-light conditions. The adsorption capacity of 4271.15 μg·g–1, rate of 5.0 μg·g–1·min–1, and removal efficiency of ∼100% were obtained under N2+O2, which was further confirmed by reaction kinetics. SrFeO3-δ was selenized into iron diselenide and a Se–Fe bond with high affinity toward Hg0. In addition, the yielding of •O2– and the separation of photoexcited electrons and holes (h+) promoted the photocatalytic oxidation of mercury. The composite with intrinsic magnetism could be easily recycled for reuse by magnetic separation. Moreover, the composite possessed favorable tolerance to the complicated flue gas. An online lab-built thermal decomposition system demonstrated that the immobilized Hg was primarily HgSe, which exhibited very high stability and low toxicity. Density functional theory (DFT) calculations proved that the composite was half metal with magnetism, indicating that Hg on Se-SrFeO3-δ/HNTs formed the stable structure releasing 1.055 eV. The doping of selenium promoted the charge transfer between O (2p) and Hg (6s), which also favored Hg0 removal. Se-SrFeO3-δ/HNTs with recyclability possess great potentials for Hg0 efficient removal and immobilization/detoxification from flue gas.
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Nanomaterials
·
2024
·Vol. 14
·期 5
·390
·
IF 4.4
Ruliang Yu,Yujiao Zhao,Jiyang Liu
Convenient and highly sensitive detection of oxalate ions in body fluids is of crucial significance for disease prevention, diagnosis, and monitoring of treatment effectiveness. Establishing a simple solid-state electrochemiluminescence (ECL) sensing system for highly sensitive detection of oxalate ions is highly desirable. In this work, a solid ECL sensor was fabricated by immobilizing the commonly used emitter ruthenium(II)tris(bipyridine) (Ru(bpy)32+) on a double-layered bipolar silica nanochannel array film (bp-SNA)-modified electrode, enabling sensitive detection of oxalate ions in serum or urine samples. Cost-effective and readily available indium tin oxide (ITO) was used as the supporting electrode. Convenient fabrication of multiple negatively charged SNA (n-SNA)-modified ITO electrodes was achieved through the one-step Stöber solution growth method. Subsequently, a positive outer layer film (p-SNA) was rapidly prepared using an electrochemical-assisted self-assembly method. The double-layered bipolar silica nanochannel array film achieved stable immobilization of Ru(bpy)32+on the electrode surface, facilitated by the electrostatic adsorption of Ru(bpy)32+by n-SNA and the electrostatic repulsion by p-SNA. Utilizing oxalate ions as a co-reactant for Ru(bpy)32+, combined with the electrostatic enrichment of oxalate ions by p-SNA, the constructed sensor enabled highly sensitive detection of oxalate ions ranging from 1 nM to 25 μM and from 25 μM to 1 mM, with a detection limit (LOD) of 0.8 nM. The fabricated ECL sensor exhibited high selectivity and good stability, making it suitable for ECL detection of oxalate ions in serum and urine samples.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Qiuyu Chen,Yongyi Zhang,Haiwang Liu,Peng Liu,Xinxin Ye,Xing Xia,Xiangwei Wu
Straw-derived dissolved organic matter (DOM) is widespread in farmland soils, but the relationship between straw-derived DOM and As in their co-sorption on minerals and the underlying mechanisms remain unclear. Here, batch experiments and spectroscopic analyses were employed to investigate the co-sorption of straw-derived DOM and As(III/V) on γ-Al 2 O 3 . Results showed a trade-off between the As(III/V) and DOM immobilization on γ-Al 2 O 3 under different pH levels, which was caused by competitive sorption. The rape straw-derived DOM (DOM_Ra) exhibited a stronger inhibition on As(III/V) sorption than rice straw-derived DOM (DOM_Ri). This could be due to more aromatic fractions in the DOM_Ra and DOM_Ri, which were preferentially sorbed by γ-Al 2 O 3 . In turn, the preferential sorption of aromatic DOM components was weakened by As(V) sorption, which, however, was not found in As(III) and DOM co-sorption. Furthermore, spectral results indicated that carboxylic groups on the sorbed DOM could provide additional binding sites for As(III/V) to form ternary complexes, but its role was overwhelmed by the DOM competitive sorption, which ultimately exhibited the inhibitory effect of DOM on As(III/V) sorption. These findings enhance the fundamental understanding of the co-sorption of As(III/V) and DOM on soil minerals and contribute to predicting As mobility and OM stability in As-contaminated farmlands with straw return.
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WASTE MANAGEMENT
·
2026
·
IF 7.3
Tianhang Tang,Chenlu Yang,Huikang Song,Hao Liu,Hao Shi,Yaji Huang
A highly efficient and environmentally friendly plasma co-melting vitrification process was developed. • The mechanisms of heavy metal fixation and migration during the plasma melting process were investigated. • Changes in the valence states and forms of various elements during the melting process were studied. Hazardous fly ash (HFA) contains large amounts of toxic heavy metals and poses significant potential risks to the environment. In this study, HFA was co-melted with hazardous bottom ash (HBA) and waste glass (WG) in a plasma system to investigate its vitrification behavior, heavy metal migration, and solidification mechanisms. The results indicate high vitrification efficiency (99.5 %) and ash solidification rate (97.1 %). The original multi-phase crystalline structure transformed into a structure dominated by an amorphous silicate network following plasma melting and rapid cooling. The surface became smoother and denser, and heavy metals were distributed uniformly, indicating enhanced physical encapsulation capacity and a more homogeneous structure. Although a considerable amount of heavy metals remained in the melt product (GP), the leaching concentrations of all detected heavy metals were significantly reduced. BCR results further indicate improved long-term stability of heavy metals. Additionally, the solidification mechanism was elucidated, involving a synergistic process of glass network encapsulation, fixation in iron-rich crystalline phases, and volatilization-redistribution-residual stabilization. As, Pb, and Cu are primarily immobilized in the glass phase, while Cr and Ni are preferentially stabilized in iron-rich spinel/ferrite-like phases; Zn and Mn exhibit dual-host behavior between the glass and crystalline phases. The results demonstrate that plasma co-melting vitrification is an effective method for the detoxification, stabilization, and resource utilization of hazardous incineration residues.
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危险品化学品经营许可证（带存储）