Frontiers in Bioengineering and Biotechnology
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2024
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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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JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2024
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IF 3.1
Wenchan Deng,Rongrong Huang,Yuanjiang Pan,Cuirong Sun
The metabolism process of amino acids is closely related to the growth of normal and cancer cells. It is still not clear how L/D-configuration amino acids participate in the metabolism of colorectal cell. Herein, intra- and extra-cellular metabolic distribution of L/D-amino acids in colorectal cell (HCT116) and human normal intestinal epithelial cell (NCM460) were profiled utilizing HPLC-MS/MS coupled with a chiral probe. The results displayed the differential metabolic portrayal for the two cell lines. Compared with NCM460 cell, 13 kinds of significant differential amino acids were founded in a lower concentration within HCT116 cell, and L-Gln was even not detected for intra-cell; as for extra-cell culture medium, the HCT116 cell consumed more L-Gln, D-Phe and D-Leu, while L-Met was low ingested in HCT116 cell. L-Ala and Gly were excretion in both two cell lines, excepted L-Cit which was uptake in HCT116 and excretion in NCM460 cell. Furthermore, the dynamic changes of chiral amino acids displayed that phenylalanine, tyrosine and tryptophan biosynthesis and arginine biosynthesis is the major pathway for intra-cellular metabolites and extra-cellular metabolites, respectively. Moreover, with additional D-amino acids in culture medium, the results exhibited that high concentration of D-amino acids have no significant effect on the proliferation of NCM460 cell, but could influence the profiling of amino acids metabolites, and further affect the proliferation of HCT116 cell. This present work enhances the understanding of these differential amino acids metabolic network and depicts a dynamic process of metabolic dysregulation of HCT116 and NCM460 cell.
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APPLIED SURFACE SCIENCE
·
2024
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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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APPLIED MICROBIOLOGY AND BIOTECHNOLOGY
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2024
·Vol. 108
·期 1
·1-13
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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
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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
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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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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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 Sustainable Chemistry & Engineering
·
2025
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IF 7.3
Jinhuan Liang,Xiaoqi Wu,Jingwen Ma,Jin Huang,Jiaxin Wu,Rongrong Zhong,Zehua Zou,Yanjun Hou,Qingxiang Wang,Xuan Zheng
Constructing efficient and durable bifunctional electrocatalysts for overall water splitting (OWS) under industrial current densities remains a critical challenge. Herein, we report a crystalline–amorphous (C–A) Schottky junction catalyst, NiFe(OH)x/Fe7S8/IF, featuring a nanosphere-assembled hierarchical architecture synthesized via a two-step in situ growth strategy. The hybrid integration of conductive Fe7S8 nanorods and amorphous NiFe(OH)x nanosheets generates a robust C–A heterointerface. Mechanistic investigations reveal that the built-in electric field (BIEF) at the Schottky interface not only narrows the band gap of NiFe (oxy)hydroxide to improve charge transport, but also modulates the adsorption behavior of reaction intermediates by tuning the d/p-band center proximity (Δεd–p) of surface reaction sites. First-principles calculations demonstrate that Δεd–p serves as a reliable electronic descriptor for optimizing HER and OER pathways of NiFe (oxy)hydroxide-Fe7S8 heterointerface via balancing H adsorption and weakening OOH binding, respectively. Benefiting from these unique electronic regulations, the resulting catalyst exhibits exceptional bifunctional electrocatalytic performance, requiring overpotentials of only 359 mV for the hydrogen evolution reaction (HER) at 1 A cm–2 and 380 mV for the oxygen evolution reaction (OER) at 500 mA cm–2. When integrated into a two-electrode electrolyzer, the NiFe(OH)x/Fe7S8/IF couple achieves a low cell voltage of 1.42 V at 10 mA cm–2 and sustains 1 A cm–2 over 300 h with minimal current density decay. This work sheds light on a generalizable interfacial design strategy and introduces Δεd–p as a conceptual framework for the rational design of cost-effective, high-performance water-splitting electrocatalysts.
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JOURNAL OF MOLECULAR STRUCTURE
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2025
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IF 4.7
Xinru Dong,Yang Li,Xuejun Zhang,Nan Liu,Peng Gao
A donor–acceptor (D–A) covalent organic framework (CoPcPA-COF) was constructed from a metal phthalocyanine donor and a polycarboxylic acid acceptor unit. Molecular structure modulation endowed the material with exceptional visible-light absorption (bandgap: 1.34 eV) and a strong photoelectronic response. In photocatalytic tetracycline degradation, CoPcPA-COF achieved 91.1% removal within 60 min and maintained stable performance in various real water matrices, demonstrating excellent environmental adaptability. Density functional theory (DFT) analysis revealed pronounced spatial charge separation (CT ratio: 88.97%), a high exciton binding energy (4.314 eV), and a ligand-to-metal charge transfer tendency. Density of states (DOS) calculations indicated a theoretical bandgap of 0.5 eV, corroborating its broad-spectrum light response and favorable electronic structure. This work provides a theoretical foundation for the development of visible-light-driven COF photocatalysts and offers a promising strategy for efficient remediation of antibiotic contamination in water.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Miaomiao He,Qiancun Wang,Zhijie Lin,Dan Sun,Guangfu Yin,Yi Deng,Weizhong Yang
Pathogenic infections pose a persistent threat to global public health, necessitating innovative antibacterial strategies with well-defined disinfection pathway. The antibacterial efficiency is confined in the contradiction between reactants adsorption and intermediates desorption. Here, the FeMoS 4 /MXene bio-heterojunction enzyme (FM BioHJzyme) is proposed and constructed. Under the inspiration of near-infrared light (NIR), the heterostructures between the FeMoS 4 and MXene facilitates efficient electron-hole separation with localized electron accumulation at FeMoS 4 sites. Crucially, the electronic push-pull effect induced by Mo polarizes oxygen-containing reactants (H 2 O 2 , H 2 O, O2) toward Fe active centers, enabling sequential electron capture for reactive oxygen species (ROS) generation. The results also reveal an enhancement in electron density at Fe sites compared to FeS/MXene controls, which is accompanied by a downshift in the Fe d-band center that reduces intermediates adsorption energy. The therapeutic efficacy is systematically evaluated using an S. aureus -infected full-thickness skin defect model. The bi-modulated FM BioHJzyme exhibits favorable antibacterial efficiency under NIR irradiation, while subsequent wound healing is facilitated through collagen deposition and angiogenesis in the following absence of NIR irradiation. This work offers a deep insight into the intricate mechanism-performance relationship of BioHJzyme platform in catalytic anti-bacterial application and proposes a sustainable approach of mechanism-guided materials design.
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Bioactive Materials
·
2025
·
IF 20.3
Qi Zhang,Zhe Zheng,Yiting Zhao,Qing Wu,Chu Wu,Xiuli Wang,Xia Wang,Qigang Wang,Peiru Wang
The transformation of O 2 is primarily facilitated by the catalytic action of redox enzymes, which play a pivotal role in sustaining cellular energy metabolism and redox balance. Bioinspired by O 2 distribution and ROS regulation related to cascade biocatalytic process, a D-peptide NapG D F D F D Y engineered hydrogel has been constructed with encapsulated dual-enzyme superoxide (SOD) and chloroperoxidase (CPO) cascade catalytic circuit and co-assembled photosensitizer of 5-aminolevulinic acid molecules (ALA). Multimodal oxygen modulation has been conducted by the concurrent oxygen generation via SOD-catalyzed ⋅O 2 − dismutation and oxygen consumption for 1 O 2 production by CPO and ALA, achieving self-sustaining enzymatic dynamic therapy (EDT)-photodynamic therapy (PDT) (EDT-PDT) synergy. The endogenous cascade-amplified EDT not only enhances the 1 O 2 efficacy in exogenous PDT therapy, but the intermediate O 2 can also alleviate local neuropathic pain caused by hypoxia for safe PDT treatment. This work pioneers enzyme-mediated dynamic control of tumor redox homeostasis, establishing a new therapeutic axis between biocatalytic amplification and photodynamic processes.
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ACS Catalysis
·
2025
·
IF 13.1
Ren Ma,Yujing Zhang,Feiyang Yu,Shilong Wei,Yang Xing,Chengfang Qiao,Zhengqiang Xia,Qi Yang,Gang Xie,Sanping Chen
High energy level difference between electron donor (D) and electron acceptor (A) and low energy loss during charge transfer are prerequisites for the construction of efficient D–A-type covalent-organic framework (COF) photocatalysts. However, the spatial structure characteristics of the building blocks inevitably lead to the torsion of the D–A COF skeleton during the construction process and thus prevent effective charge migration. Herein, with the high-energy-level triphenylamine (TPA) as a model electron donor, the formyl positional isomers of tris(3-formylbiphenyl) amine (NDC) and tri(4-formylbiphenyl) amine (NBC) react with an acceptor 1,3,5-tris(4-aminophenyl) triazine (TTA), producing both D–A COFs for photocatalytic CO2 reduction and benzylamine coupling reactions. Structural investigations evidence that the formyl positional isomerism imparts the dihedral angle of TPA single arm reducing from 51.09 to 2.12°, the interlayer spacing from 3.89 to 3.55 Å, and the exciton binding energy from 97.25 to 85.86 meV in TTA-COFs. Such the “near-flat” TTA-NDC structure with confined clover-like channels dramatically accelerates the intralayer and interlayer charge migration efficiency and improves CO2 adsorption and oxygen activation ability (O2•– concentration of 48.01 μmol·L–1 in 3 h). To the best of our knowledge, TTA-NDC exhibits the highest benzylamine coupling efficiency with a turnover frequency value of 518.4 h–1 among the pristine COF photocatalysts, and its electron consumption rate for photocatalytic CO2 reduction reaches 1632.2 μmol·g–1·h–1, 3.85-fold higher than TTA-NBC, far surpassing most COF-based photocatalysts. Parallelly, the protonated H-TTA-NDC shows high CO2 reduction to CH4 yield (310.1 μmol·g–1·h–1) and selectivity (85.1%) due to the improved proton conductivity (σ = 1.07 × 10–2 S·cm–1). Additionally, the durability, stability, and possible photocatalytic mechanisms of TTA-NDC were systematically investigated.
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