APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
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2024
·Vol. 108
·期 1
·1-13
·
IF 3.9
Wu Zongzhan,Dou Wenyu,Yang Xiaolin,Niu Tengfei,Han Zhuzhen,Yang Li,Wang Rufeng,Wang Zhengtao
Abstract Oleanane-type ginsenosides are a class of compounds with remarkable pharmacological activities. However, the lack of effective preparation methods for specific rare ginsenosides has hindered the exploration of their pharmacological properties. In this study, a novel glycoside hydrolase Pl GH3 was cloned from Paenibacillus lactis 154 and heterologous expressed in Escherichia coli . Sequence analysis revealed that Pl GH3 consists of 749 amino acids with a molecular weight of 89.5 kDa, exhibiting the characteristic features of the glycoside hydrolase 3 family. The enzymatic characterization results of Pl GH3 showed that the optimal reaction pH and temperature was 8 and 50 °C by using p -nitrophenyl- β - d -glucopyranoside as a substrate, respectively. The K m and k cat values towards ginsenoside Ro were 79.59 ± 3.42 µM and 18.52 s −1 , respectively. Pl GH3 exhibits a highly specific activity on hydrolyzing the 28- O - β - d -glucopyranosyl ester bond of oleanane-type saponins. The mechanism of hydrolysis specificity was then presumably elucidated through molecular docking. Eventually, four kinds of rare oleanane-type ginsenosides (calenduloside E, pseudoginsenoside RP1, zingibroside R1, and tarasaponin VI) were successfully prepared by biotransforming total saponins extracted from Panax japonicus . This study contributes to understanding the mechanism of enzymatic hydrolysis of the GH3 family and provides a practical route for the preparation of rare oleanane-type ginsenosides through biotransformation. Key points • The glucose at C-28 in oleanane-type saponins can be directionally hydrolyzed. • Mechanisms to interpret PlGH3 substrate specificity by molecular docking. • Case of preparation of low-sugar alternative saponins by directed hydrolysis.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Ding-Ming Xue,Yi-Jun Zhang,Jing-Wen Chen,Hao Yang,Rui-Jie Xie,Shi-Chao Qi,Yuan-Qing Bu,Fei Liu,Hou-Hu Zhang,Jacques Lalevée
Covalent organic frameworks (COFs), as a newly emerging kind of porous and crystalline materials, serve as an ideal template for hydrogen peroxide (H 2 O 2 ) photosynthesis. However, the vision of achieving high efficiency and selectivity in H 2 O 2 photosynthesis is greatly hindered by the large exciton binding energy and limited charge separation efficiency influenced by the molecular structure of the building blocks. Herein, we developed three newly designed COFs with a donor–acceptor (D-A) structure and incorporated regulatory units (fluorine, F, and methoxyl, OCH 3 ) in the D-A pathway through molecular engineering to optimize electronic structure, the availability of activate sites, charge kinetics and O 2 activation capacity. Due to electron-donating effect, OCH 3 -functionalization (NIES-COF-3) can strengthen the intramolecular electron transfer and interaction with O 2 . This results in a reduction of the energy barrier of the rate-determining step (*O 2 → *OOH) and excellent O 2 -to-H 2 O 2 photocatalytic activity under visible light irradiation, delivering an H 2 O 2 production rate of 3238.4 μmol g −1 h −1 and a high apparent quantum yield of 3.17 %. In addition, F-functionalization (NIES-COF-2) primarily reduces the band-gap energy and improve the O 2 adsorption capacity compared to unfunctionalized NIES-COF-1. This work unveils insight into the catalytic activity-optimization mechanism of molecular engineering in the D-A structure and provides important references for photocatalysts.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Songlin Chen,Zhihao Shen,Shuming Wen,Guang Han,Qicheng Feng
Flotation separation of Cu–Fe sulfide minerals typically necessitate the addition of substantial quantities of lime to depress pyrite flotation. Because lime can harm the environment, there is an urgent need to develop novel environmentally friendly depressants that are non-toxic and biodegradable. In this study, we investigated an environmentally friendly pyrite depressant containing amino and carboxyl groups, namely D-arginine (DA). The effect of DA on the surface hydrophobicity of Cu–Fe sulfide minerals and thus collector adsorption was investigated by analyzing zeta potentials, adsorption capacities, and contact angles. Additionally, changes in the surface properties of the minerals induced by DA were examined using X-ray photoelectron spectroscopy (XPS), time-of-flight secondary ion mass spectroscopy (ToF-SIMS), and atomic force microscopy (AFM). Flotation tests revealed that 2 × 10 –4 mol/L DA reduced the flotation recovery of pyrite to 9.96 % at low alkalinity while leaving chalcopyrite recovery unchanged. The results of mineral surface analysis indicated that DA exhibited significantly stronger adsorption on the pyrite surface than on the chalcopyrite surface. Furthermore, DA effectively reduced the adsorption of the collector on the surface of pyrite, thereby weakening pyrite floatability at low alkalinity. Therefore, DA is a promising alternative depressant for the flotation separation of chalcopyrite from pyrite.
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TOXICOLOGY LETTERS
·
2024
·
IF 2.9
Yingxin Pang,Xiaoqi Tao,Zongmin Qin,Muran Jiang,Erqun Song,Yang Song
This work investigated the influence of surface chirality on cellular internalization, cytotoxicity, and tissue distribution of silver nanoparticles (AgNPs). D-cysteine and L-cysteine are chiral forms of the amino acid cysteine. These enantiomers exhibit distinct spatial arrangements, with D-cysteine having a different configuration from L-cysteine. This structural dissimilarity can lead to variations in how these forms interact with biological systems, potentially impacting their cytotoxic responses. Four distinct types of AgNPs were synthesized, each possessing a unique surface coating: pristine AgNPs (pAgNPs), L-cysteine coated AgNPs (AgNPs@L-Cys), D-cysteine coated AgNPs (AgNPs@D-Cys), and racemic AgNPs coated with both L-Cys and D-Cys (AgNPs@L/D-Cys). We found chiral-dependent cytotoxicity of AgNPs on J774A.1 cells. Specifically, AgNPs@L-Cys exhibited the highest toxicity, and AgNPs@D-Cys exhibited the lowest toxicity. Meanwhile, the cellular uptake of the AgNPs correlated nicely with their cytotoxicity, with AgNPs@L-Cys being internalized to the greatest extent while AgNPs@D-Cys displays the least internalization. Scavenger receptors and clathrin predominantly mediate the cellular internalization of these AgNPs. Strikingly, the dissimilar cellular internalization and cytotoxicity of AgNPs with different chirality were eliminated upon protein corona coverage. Notably, following intravenous injection in mice, these four types of AgNPs showed similar patterns among various organs due to the inevitable protein adsorption in the bloodstream. These findings underscored the pivotal role of surface chirality in governing the biological interactions and toxicity of AgNPs.
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Frontiers in Bioengineering and Biotechnology
·
2024
·
IF 4.3
Lei Han,Chaoqian Zhao,Yufang Zhu,Huang Li
Introduction: Bone tissue engineering is considered the ideal approach for bone repair. Mesoporous bioactive glass (MBG) possesses the characteristics of high drug-loading capacity and bioactivity. Low-intensity pulsed ultrasound contributes to promoting fracture healing and bone defect repair, and dimethyloxalyl glycine (DMOG) is a small molecular inhibitor that can suppress prolyl hydroxylase, reducing the degradation of hypoxia-inducible factor. Methods: In this study, we proposed to prepare DMOG-loaded MBG/poly(D,L-lactide) composite scaffolds (DMOG-MBG/PDLLA) for promoting bone repair. The effects of ultrasound stimulation and DMOG release on the cell responses of rat bone marrow mesenchymal stem cells (BMSCs) and human umbilical vein endothelial cells (HUVECs) and bone repair in vivo were investigated. Results and Discussion: The results showed that both ultrasound stimulation and DMOG release could promote the proliferation, adhesion and differentiation of BMSCs and HUVECs, respectively. After the implantation of scaffolds in rat cranial bone defect model for 8 weeks, the results indicated that the combined ultrasound stimulation and DMOG release contributed to the highest ability for promoting bone repair. Hence, the DMOG-MBG/PDLLA scaffolds with ultrasound stimulation are promising for application in bone repair.
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TALANTA
·
2025
·
IF 6.1
Mingjiang Huang,Binbin Luo,Shengxi Wu,Miwan Shi,Yan Liu,Shenghui Shi
A D-Shaped, excessively tilted fiber grating (ExTFG) immunosensor modified with molybdenum disulfide (MoS 2 ) was developed for label-free and specific detection of growth-stimulated expressed gene 2 protein (ST2), a critical biomarker for heart failure. The D-Shaped ExTFG sensor was fabricated by side-polishing an ExTFG along its slow axis to enhance refractive index (RI) sensitivity. It was subsequently biofunctionalized with MoS 2 and anti-ST2 monoclonal antibodies (anti-ST2 MAbs) for ST2 immunoassays. The RI sensitivities of the sensor after side-polishing and MoS 2 coating were thoroughly investigated. Additionally, the immunodetection properties of the sensor were evaluated across varying concentrations of ST2 antigen solutions, as well as its specificity and clinical performance in serum samples from healthy individuals and patients. Experimental results revealed that the sensitivity of the MoS 2 -modified D-Shaped ExTFG immunosensor for ST2 reached 0.335 nm/[log(mg/mL)] over a wide linear testing range of 1 ng/mL to 1000 ng/mL, with a detection limit of 0.472 ng/mL. This represents an improvement of approximately 86 % compared to the ExTFG without D-Shaped modification and demonstrates excellent specificity for ST2 biomarkers even in complex clinical sera. The MoS 2 -modified D-Shaped ExTFG immunosensor exhibits notable advantages, including stability, practical usability, and high clinical specificity, making it a promising candidate for biomedical and other analytical applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Yunchao Ma,Yuxin Yao,Shengnan Qi,Chuanxue You,Yuanyuan Wu,Chunbo Liu,Bo Hu,Keyu Cui
Herein, we successfully synthesized two photoactive donor–acceptor (D-A) covalent organic frameworks by incorporating electric-deficient triazine and electric-rich benzotrithiophene moieties into the framework. The introduction of sulfur atom and triazine unit significantly change the intrinsic band gap of JLNU-COFs, this leads to an expanded range of light absorption, encompassing wavelengths from ultraviolet to visible. The narrow band gap of JLNU-311 allows for efficient utilization of visible light while maintaining the thermodynamic activity required for nitrogen reduction within appropriate energy bands. JLNU-311 modified with strong electron absorbing groups has higher activity to NH 3 production without co-catalyst or sacrificial agent, and yield can reach 325.6 µmol/g/h. Theoretical calculation further confirm that acceptor structure can effectively regulate the band gap width, promote the adsorption, dissociation and protonation of N 2 molecules on JLNU-COFs, and thus reduce the energy barrier of photocatalytic nitrogen reduction reaction (PNRR). Therefore, this study provides an effective strategy for design of active nitrogen fixing photocatalysts.
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Analytical Methods
·
2017
·Vol. 9
·期 43
·6131-6138
·
IF 1.9
Xiangyu Wang,Huihui Wu,Rongying Luo,Donghai Xia,Zhengjin Jiang,Hai Han
D-amino acids are currently paid attention to as new physiologically active substances. Foodstuffs and beverages containing D-amino acids are a matter of interest. Until now, the profiles of D-amino acids have not been reported in natural and fermented teas except theanine. In this study, an off-line 2D-HPLC method combining a Gemini C18 column and a CHIRALPAK® IC-3 column or a self-prepared poly(MQD-co-HEMA-co-EDMA) monolithic capillary column was employed for the separation and detection of D-amino acids in tea samples with the co-existence of a large amount of L-amino acids. The free amino acid fractions in longjing, black, oolong, and pu-erh tea samples were separated and collected after pre-column derivatization using 9-fluorenylmethoxycarbonyl (FMOC) chloride in the reversed-phase mode, and then were concentrated and separated to D- and L-forms on a chiral column. Among them, the D-form of isoleucine (Ile) (1.0–1.6%), alanine (Ala) (0.1–0.8%), phenylalanine (Phe) (0.1–0.4%), valine (Val) (0.2–0.3%), serine (Ser) (0.1–0.2%), aspartic acid (Asp) (0.2%), and proline (Pro) (0.1%) were detected in longjing and oolong teas. Differences between natural tea and fermented tea in the profiles of D-amino acids as well as the total amino acids were also observed. The results provided useful information for the bio-function research of D-amino acids in tea.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jiahe Chen,Yingying Zhang,Xin Guo,Yiyang Qiao,Ping Yu
Artemisinin (Art) is the primary therapies for plasmodium falciparum malaria. However, it is very cumbersome to extract artemisinin from the plant Artemisia annua L. Herein, a novel defect-type UiO-66 structure was proposed, which can adsorb artemisinin through effective sites provided by ‘template molecules’. At the same time, the delayed phase inversion technology was used to prepare the loofah membrane to make the defect-type UiO-66 uniformly dispersed in the pores. In addition, the inside of the biomass loofah membrane had good mechanical properties and loofah membrane wrapped with polyacrylonitrile (PAN) can make Art solution evenly dispersed in each channel, greatly improving the utilization rate of defect-type UiO-66. The defect-type UiO-66 and the UiO-66-D@loofah membrane were characterized using various methods, including SEM, EDS, FT-IR, XRD, contact angle, and mechanical performance analyses. Compared with the static adsorption behavior of powder and loofah membrane, it was found that the adsorption performance presented an optimal adsorption capacity (56.548 mg g −1 ) at the flow rate of 5 mL min −1 , which was better than that of powder (27.096 mg g −1 ) as well as the static loofah membrane (33.127 mg g −1 ). The structural design of the membrane has provided a new solution for the extraction of Art from Artemisia annua L.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Lili Yin,Wenjia Feng,Yang Hu,Xiangzhao Mao
Phosphatidylserine (PS), a rare phospholipid in Antarctic krill oil (AKO) critical for brain development, can be produced from the abundant phosphatidylcholine (PC) using phospholipase D (PLD) in Pickering emulsion interfacial catalysis (PIC) systems. However, the exposure of PLD to organic solvent around the emulsion interface diminished PLD activity, limiting the conversion efficiency of PS. In this study, we proposed a strategy to fabricate a PIC system with high efficiency and stability by immobilizing PLD in a specific phase on the emulsion interface, based on investigating the effect of the interfacial microenvironment on PLD activity. Janus-poly(acrylic acid)/polystyrene (JPP) and Janus-polyethylenimine/octadecane (JPO) particles were fabricated as carriers to realize the specific-phase immobilization of PLD. The highest activity was observed when PLD was immobilized on the hydrophilic side of JPP (PLD@JPP(W)), 1.9-fold that of free PLD. The catalytic efficiency of PLD@JPP(W) was 1.7-fold that of free PLD, confirmed by the kcat/Km value enhancement. Immobilization on the hydrophilic side also enhanced the thermal stability of PLD. The half-lives of PLD were extended from 4 to 36 h at 40 °C and from 6 to 28 days at 4 °C. Importantly, PLD@JPP(W) showed excellent catalytic efficiency as a PIC system, achieving a PS productivity of 93% within a short time of 2 h at an enzyme dosage of 0.05 mg. PLD@JPP(W) exhibited a 3.6 times higher yield than free PLD in the production of PS from PC rich in Antarctic krill oil. The strategy in this work could also be applied to other lipases, providing a promising method for the efficient conversion of functional lipids.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Mengtian Cui,He Wang,Xia Fan,Jianhao Zhang,Changrui Xing,Wenjing Yan
The widespread use of organophosphorus pesticides (OPPs) in foods, poses a serious threat to human and environmental health, it is crucial to develop methods that can efficiently degrade residual OPPs . Herein, a chiral TiO 2 photocatalyst was developed by modification TiO 2 with D-cys/Au NPs (DAT) for the simultaneous degradation of four OPPs (chlorpyrifos, chlorpyrifos-methyl, malathion, and parathion) by natural light. The influence of D-Au NPs concentration on the degradation process was optimized, along with the initial pesticide concentration. Under optimal conditions, the photocatalytic degradation efficiencies of DAT for four OPPs were 96.7 %, 56.9 %, 42.6 %, and 49.2 %, respectively, after 12 h of natural light exposure. 12 degradation products of OPPs were identified, among which three products were identified for the first time. The degradation pathway revealed that the degradation of OPPs by DAT involves the oxidation of the P═S bond and the cleavage of the P-O bond and C-O bond. This study establishes a theoretical foundation for applying chiral TiO 2 nanomaterials for the photocatalytic degradation of OPPs in foods.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Huabin Lian,Riming Hu,Lin Zheng,Daowei Gao,Shuai Wang,Rongyao Wang,Bin Wang,Guozhu Chen
The electrocatalytic reduction of biomass-derived furfural represents a sustainable pathway for the production of furfuryl alcohol and 2-methylfuran, serving respectively as value-added chemicals and biofuels. However, the production of these high-value-added products under mild conditions is hampered by low Faradaic efficiency. In this study, we develop a strategy to establish strong metal-support interactions, enabling Cu/NC (nitrogen-doped carbon) catalysts to efficiently produce value-added products under mild conditions. Specifically, we prepare a cost-effective NC support with highly dispersed ultrafine nano-Cu particles of approximately 1 nm in diameter. Under mild pH conditions, our comparative experiments show that the Faradaic efficiency for value-added products (furfuryl alcohol and 2-methylfuran) is nearly four times higher than that of commercial foam copper. We elucidate the influence of nitrogen-doped supports on the behavior of the supported metal Cu. Comprehensive in-situ infrared reflection absorption spectroscopy characterization and DFT theoretical calculations reveal a positive shift in the d-band center of the Cu 3d orbitals. This shift enhances the adsorption of furfural C1=O1 bonds on the Cu/NC catalyst and improves its capacity to bind active hydrogen, thereby increasing the Faradaic efficiency of the value-added products. Our findings advance theoretical understanding and providing practical insights for electrocatalytic hydrogenation of furfural under mild pH conditions.
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