ACS Sustainable Chemistry & Engineering
·
2024
·
IF 7.1
Mei Chen,Yarong Huang,Yanming Wang,Yuxia Pang,Hongming Lou,Zhixian Li,Dongjie Yang,Xueqing Qiu
Metal–organic frameworks (MOFs) have attracted considerable attention as promising platforms for enzyme immobilization due to their high porosity and ease of preparation. However, the economy and greenness of the MOF synthesis process and the stability of the MOF as well as the microporous structure of MOFs limiting the accessibility of the enzyme and substrate significantly affect their practical applications. Here, based on a competitive coordination and selective etching strategy, we propose a general, simple, fast, low-cost, reproducible, and high-yield synthesis technique for MOF-immobilized enzymes. In the aqueous phase at room temperature, we achieved rapid encapsulation of β-glucosidase (β-G) in MOF-74-2-MI by using 2-methylimidazole (2-MI) as a nucleation accelerator modulator. Followed by selective etching with tannic acid (TA), a hierarchical porous composite, β-G@TA-MOF-74-2-MI, was successfully formed. The results showed a significant increase in mesopore and macropore volumes, leading to a remarkable 6.41-fold enhancement in catalytic activity compared to the nonetched composite. Additionally, it exhibited superior temperature resistance and organic solvent tolerance compared with the free enzyme, along with outstanding cycling, storage, and crystallization stability. This work represents a significant advance in the controlled synthesis of hierarchical porous enzyme@MOF composites, which opens new possibilities for the efficient biocatalysis of macromolecular substrates.
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FOOD CHEMISTRY
·
2025
·
IF 9.8
Lu Gao,Qianwen Long,Baizhi Cen,Qi Gao,Mengyuan Tan,Ling Zhang,Juanli Yang,Yuan Ma,Xuechao Xu,Zhen-quan Yang
A chromogenic system utilizing a novel bacteriophage-integrated nanozyme was established for Proteus penneri detection. Initially, a novel bacteriophage PpZDSS02 was isolated and identified, demonstrating exceptional biological properties and harboring genes that exhibit specific recognition ability. Afterwards, a PpZDSS02-integrated Cu-MOF nanozyme (Cu-MOF@PpZDSS02) with peroxidase-mimicking activity was prepared, catalyzing 3, 3′, 5, 5′-tetramethylbenzidine (TMB) chromogenic reaction. Its peroxidase-mimicking activity can be modulated by P. penneri . Interestingly, low concentration of P. penneri can enhance its activity and high concentration of P. penneri inhibits its activity. Based on it, a visual quantification method with high sensitivity and specificity for P. penneri was achieved, offering a low limit of detection (3.3 CFU·mL −1 ). Moreover, Cu-MOF@PpZDSS02-based chromogenic system shows exceptional performance in the detection of authentic food samples, achieving ideal recoveries (89.00 % ∼ 111.81 %). These results indicate the potential application of Cu-MOF@PpZDSS02-based chromogenic system for colorimetric detection of P. penneri .
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高影响因子
MOLECULES
·
2025
·Vol. 30
·期 4
·912
·
IF 4.6
Huiyi Shang,Juntan Wang,Bishan Guo,Haihua Zhu,Huijuan Li
Phospholipase D (PLD) plays a pivotal role in the biosynthesis of phosphatidylserine (PS), but its practical application is constrained by limitations in stability and reusability. In this study, we successfully fabricated the Fe3O4@SiO2–graphene oxide (GO) nanocomposite by chemical binding of Fe3O4@SiO2and GO. Subsequently, PLD was immobilized onto the nanocomposite via physical adsorption, with the aim of enhancing catalytic stability, reducing mass transfer resistance, and improving reusability. Under optimal conditions, the immobilization efficiency reached 84.4%, with a PLD loading capacity of 111.4 mg/gsupport. The optimal pH for PS production by immobilized PLD shifted from 6.0 to 6.5, while the optimal temperature increased from 45 °C to 50 °C. Notably, the immobilized PLD demonstrated a shorter reaction time and a higher PS yield, achieving a 95.4% yield within 90 min, compared to the free PLD (78.1% yield within 150 min), representing a 1.04-fold improvement in production efficiency. Furthermore, the immobilized PLD exhibited outstanding storage stability and thermal stability, along with remarkable reusability. Even after being reused for 10 cycles, the PS yield still stays as high as 78.3%. These findings strongly suggest that the Fe3O4@SiO2–GO immobilized PLD has the potential for the efficient production of PS.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Qi Fang,Yanling Tan,Ran Yan,De Zhang,Mi Li,Xiaoyan Wu,Yilong Hua,Wenjing Xue,Rongzhong Wang
Nanoscale zerovalent iron (Fe 0 )-based materials have been demonstrated to be a effective method for the U(VI) removal. However, limited research has been conducted on the long-term immobilization efficiency and mechanism of Fe 0 -based materials for U(VI), which are essential for achieving safe handling and disposal of U(VI) on a large scale. In this study, the prepared carboxymethyl cellulose (CMC) and sulfurization dual stabilized Fe 0 (CMC-Fe 0 /FeS) exhibited excellent long-term immobilization performances for U(VI) under both anoxic and oxic conditions , with the immobilization efficiencies were respectively reached over 98.0 % and 94.8 % after 180 days of aging. Most importantly, different from the immobilization mechanisms of the fresh CMC-Fe 0 /FeS for U(VI) (the adsorption effect of –COOH and –OH groups, coordination effect with sulfur species, as well as reduction effect of Fe 0 ), the re-mobilized U(VI) were finally re-immobilized by the formed FeOOH and Fe 3 O 4 on the aged CMC-Fe 0 /FeS. Under anoxic conditions , more Fe 3 O 4 was produced, which may be the main reason for the long-term immobilization U(VI). Under oxic conditions, the production of Fe 3 O 4 and FeOOH were relatively high, which both played significant roles in re-immobilizing U(VI) through surface complexation, reduction and incorporation effects.
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BIOCHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 3.7
Wenbo Li,Xin Yan,Wenli Xia,Linguo Zhao,Jianjun Pei
Prenylated flavonoids are the primary modification of flavonoids and exhibit a diverse range of physiological activities. In this study, a co-immobilization of two-enzyme cascade was developed to regenerate dimethylallyl diphosphate (DMAPP). Shigella flexneri promiscuous kinase (SfPK) and Methanolobus tindarius isopentenyl phosphate kinase (MtIPK) were immobilized onto carboxymethyl cellulose magnetic nanoparticles (CMN) with a maximum load of 0.35 mg/mg and 0.28 mg/mg, respectively. The optimal activity of CMN-SfPK and CMN-MtIPK were at pH 9.5 and 55°C, and pH 7.0 and 35 °C, respectively. CMN-SfPK and CMN-MtIPK exhibited superior catalytic efficiency compared to free enzymes. CMN-SfPK was coupled with CMN-MtIPK to develop an efficient DMAPP regeneration system from prenol. Subsequently, SfPK, MtIPK and Aspergillus fumigatus prenyltransferase (AfPT) were co-immobilized on CMN to form CMN-SfPK-MtIPK-AfPT (CSMA) according to the optimal ratio. The 3’-C-prenylnaringenin production rate in CSMA reached 0.37 mmol/L/h, which was 1.85 times that of single-immobilized enzymes. Finally, the total production and production rate of 3’-C-prenylnaringenin in CSMA reached 2.55 mM and 0.255 mmol/L/h with 10 cycles. Therefore, the method described herein for efficient production of DMAPP and 3’-C-prenylnaringenin by using co-immobilized enzymes can be widely used for the prenylation of flavonoids.
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FOOD CHEMISTRY
·
2025
·
IF 9.8
Ziyi Yang,Xiaoyan Dong,Zhenfu Wang,Yan Sun
Gluconic acid is widely used in food and pharmaceutical. However, its bio-synthesis by glucose oxidase (GOx) is blocked by depletion of dissolved O 2 , reduction of pH value, and accumulation of hydrogen peroxide (H 2 O 2 ). To remove the by-products and replenish O 2 , developing a nanozyme with high catalase (CAT)-like activity and stability under acidic conditions is a prescription. Herein, we developed a manganese-based nanozyme (ps-MnO x -BSA) through a stepwise strategy and encapsulated it in Fe-doped zeolitic imidazolate framework-8 (FZ). The as-prepared ps-MnO x -BSA@FZ (MFZ) exhibited not only high stability and CAT-like activity but also exceptionally no peroxidase-like activity at pH 5.5. Thereafter, GOx@MFZ was fabricated by the immobilization of GOx on MFZ and utilized for gluconic acid synthesis with a yield of 98.3 % within 30 min. GOx@MFZ retained 92.3 % of its initial activity after six batches. This work provided a novel strategy for the design of acid-resistant CAT-like nanozyme toward sustainable gluconic acid production.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Jinhong Gao,Lingli Zhang,Dongxin Zhao,Xin Lu,Qiang Sun,Heng Du,Hongyan Yang,Kui Lu
Aspergillus oryzae β-D-galactosidase (β-Gal) efficiently hydrolyzes sesaminol triglucoside into sesaminol, which has higher biological activity . However, β-Gal is difficult to be separate from the reaction mixture and limited by stability. To resolve these problems, β-Gal was immobilized on amino-functionalized magnetic nanoparticles mesoporous silica pre-activated with glutaraldehyde (Fe 3 O 4 @mSiO 2 -β-Gal), which was used for the first time to prepare sesaminol. Under the optimal conditions, the immobilization yield and recovered activity of β-Gal were 57.9 ± 0.3 % and 46.5 ± 0.9 %, and the enzymatic loading was 843 ± 21 U enzyme /g support . The construction of Fe 3 O 4 @mSiO 2 -β-Gal was confirmed by various characterization methods, and the results indicated it was suitable for heterogeneous enzyme-catalyzed reactions. Fe 3 O 4 @mSiO 2 -β-Gal was readily separable under magnetic action and displayed improved activity in extreme pH and temperature conditions. After 45 days of storage at 4 °C, the activity of Fe 3 O 4 @mSiO 2 -β-Gal remained at 92.3 ± 2.8 %, which was 1.29 times than that of free enzyme, and its activity remained above 85 % after 10 cycles. Fe 3 O 4 @mSiO 2 -β-Gal displayed higher affinity and catalytic efficiency. The half-life was 1.41 longer than free enzymes at 55.0 °C. Fe 3 O 4 @mSiO 2 -β-Gal was employed as a catalyst to prepare sesaminol, achieving a 96.7 % conversion yield of sesaminol. The excellent stability and catalytic efficiency provide broad benefits and potential for biocatalytic industry applications.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Lijun Yang,Tiantian Zhou,Zhiyi Zhang,Wei Qi,Mengfan Wang
The enzymatic oxidation of amino acids using amino acid oxidases (AAOs) as biocatalysts for α-keto acid synthesis has garnered increasing attention due to its environmental friendliness and exceptional reaction efficiency. However, the by-product H 2 O 2 inevitably causes the decarboxylation of α-keto acids and subsequently deactivates the enzyme. Herein, we used a simple in-situ biomineralization method to immobilize Pt NPs with catalase-like activity and L-amino acid oxidase (LAAO) in to a hydrogen-bonded organic framework ( TW HOF) under a mild condition, and the synthesized LAAO-Pt@ TW HOF cascade catalytic system was applied to synthesis of α-keto acid. Compared with free LAAO, the LAAO-Pt@ TW HOF exhibited a 3.3-fold activity, well reusability and complete conversion (100 %) of L-tryptophan to indole-3-pyruvic acid was achieved. This work offers a potential application of HOF materials in constructing high-efficiency enzyme-metal coupled catalyst for cascade reactions.
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高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Shengnan Zhang,Xiaoyan Qian,Jie Ma,Xiao Liu,Juanxiang Zhang,Chong Liu,Xinqiang Liang,Xuefei Hu,Fayong Li
Tetracycline (TC) and copper (Cu) are among the most widely used additives in livestock and poultry production. When introduced into soils via organic fertilizers, they can co-occur and interact, creating complex contamination scenarios that may threaten environmental quality and human health. Biochar effectively inhibits the co-transport of TC and Cu in saline-alkali soils. However, the underlying quantum and molecular mechanisms remain unclear. In this study, column experiments, transport modeling, quantum chemical calculations, and molecular dynamics simulations demonstrated that biochar increases the microdomain pH (> 10), thereby facilitating the synergistic immobilization of TC and Cu within saturated porous media. Soil alkalinization promoted TC deprotonation, and di-deprotonation significantly enhanced the covalent complexation between TC and Cu. The binding energy for the di-deprotonated TC complexed with dual Cu reached –50.38 kcal·mol -1 . Cu binding at distinct TC sites formed molecular clusters with heterogeneous surface potentials, facilitating their aggregation and deposition, preferentially onto biochar and illite surfaces. This synergistic retention intensified with an increase in biochar dosage. Pig manure biochar (PMBC) exhibited a significantly higher retention capacity for TC-Cu complexes than that of cotton straw biochar, which was attributed to the substantially high hydroxyl and carboxyl functional groups and ash content of PMBC. The application of PMBC within a closed-loop cotton-pig farming system reduces environmental risks from combined antibiotic and heavy metal pollution while enhancing soil carbon sequestration. This provides a sustainable remediation strategy and its basis in environmental structural chemistry.
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高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2021
·
IF 4.759
Xiuhong Wu,Boquan Qu,Yongkang Liu,Xingxuan Ren,Shaoyan Wang,Yanling Quan
In this study, an enzyme immobilization method for the effective biotransformation of ginsenoside Rb1 to impart activity and stability was developed. Using a hydrolase enzyme model, β-glucosidase from Aspergillus niger , immobilization within chemically affinity-linked amino-based silica provided an immobilization efficiency 5.86-fold higher than that of free enzyme. Compared with the free enzyme, the immobilized enzyme functioned optimally at a wider pH range and had higher thermostability. The optimum pH for the free and immobilized enzymes was 5.5. The optimal reaction temperature of the immobilized enzyme was 45 °C, which was 5 °C higher than that of the free enzyme. The Michaelis constant ( K m ) values before and after immobilization were 0.482 mmol•L −1 and 0.387 mmol•L −1 , respectively. The catalytic rate ( K cat ) for the immobilized and free enzymes was 22.269 mmol•L −1 and 8.800 mmol•L −1 , respectively, and the catalytic efficiency ( K cat / K m ) activity of the immobilized enzyme was 3.30-fold higher than that of the free enzyme. The immobilized enzyme could preserve 97 % of the activity after 45 cycles of repeated use. The high catalytic activity and significant operational stability are beneficial for industrial applications.
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Sensors and Actuators Reports
·
2025
·
IF 7.6
Yashuang Hei,Lisi Ba,Ling Yu,Bingxiao Zheng,Sisi Wen,Nan Ma,Zhiju Zhao
In this work, a novel bienzymatic lactate biosensor was developed by co-immobilization of lactate oxidase (LOD) and horseradish peroxidase (HRP) onto the screen-printed electrode (SPE) modified by the three-dimensional (3D) carbon nanoballs cross-linked carbon aerogels (3D-CNCAs), which is derived from the biomass of sugarcane. The 3D-CNCAs, with large surface area and porous structure, play a crucial role in facilitating direct electron transfer between the electroactive center of HRP and the biosensor electrode. The experimental parameters including the amount of 3D-CNCAs suspension, the ratio of the two enzymes, the buffer pH and the operation potential were optimized. The bienzymatic lactate biosensor exhibits linear current response for lactate in the concentration ranges of 1-1690 μM, with a detection limit of 0.23 μM (S/N = 3), which is superior to the one based on monotypic enzyme of LOD. The bienzymatic lactate biosensor also exhibits a high level of selectivity, reproducibility, repeatability and long-term stability (87% of the original value after storage for 30 days), and was further applied in lactate detection in diluted real samples of lactic acid cream and commercial beverage. The outstanding analytical performance of the bienzymatic lactate biosensor demonstrates the preponderance of the bienzymatic over the one based on monotypic enzyme, and holds broad application prospects in the future.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123953
·
IF 7.5
Suqing Zhu,Qunxian Yuan,Donglan Ning,Jinyue Wei,Wenhan Sun,Xinpeng Wang
The safe interception and permanent stabilization of radioactive iodine released during nuclear fuel processing are critical for ecological security and public health. However, traditional adsorbents for capturing and storing iodine vapor are still plagued with unsatisfactory uptake capacity, poor structural robustness. Herein, a unique core-satellite ZIF-67-on-MIL-167 (MOF-on-MOF) composite is fabricated through a controllable heterogeneous nucleation and growth route, which was designed for the efficient capture of radioactive iodine. Experimental data shown that delivers a maximum iodine vapor uptake of 5.600 g/g under dry atmosphere, representing a 2.03-fold and 1.42-fold increase compared to pure ZIF-67 and MIL-167, respectively. It is important to note that the iodine adsorption capacity of ZIF-67-on-MIL-167 is rarely influenced by the humid environment in a relative humidity of 18%. Furthermore, ZIF-67-on-MIL-167 exhibited excellent chemical and thermal stability, maintaining a stable framework structure at temperatures as high as 283 °C, and the iodine-loaded ZIF-67-on-MIL-167 exhibited an exceptionally high radioiodine outstanding iodine retention efficiency of 94.25% after being exposed to ambient conditions for 7 days. The composite material exhibited a high degree of synergy between its N-rich imidazole structure, abundant Ti−oxo clusters, and uncoordinated carboxylic (C O) functional groups. This synergy resulted in the provision of numerous active sites and the facilitation of charge transfer, thereby enabling the efficient capture of radioactive iodine. The adsorbent developed in this work is both reliable and effective, showing promise for practical application in radioactive iodine capture.
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