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Science Advances · 2022 ·Vol. 8 ·期 18 · IF 14.957

Photocatalyst-mineralized biofilms as living bio-abiotic interfaces for single enzyme to whole-cell photocatalytic applications

Xinyu Wang,Jicong Zhang,Ke Li,Bolin An,Yanyi Wang,Chao Zhong

There is an increasing trend of combining living cells with inorganic semiconductors to construct semi-artificial photosynthesis systems. Creating a robust and benign bio-abiotic interface is key to the success of such solar-to-chemical conversions but often faces a variety of challenges, including biocompatibility and the susceptibility of cell membrane to high-energy damage arising from direct interfacial contact. Here, we report living mineralized biofilms as an ultrastable and biocompatible bio-abiotic interface to implement single enzyme to whole-cell photocatalytic applications. These photocatalyst-mineralized biofilms exhibited efficient photoelectrical responses and were further exploited for diverse photocatalytic reaction systems including a whole-cell photocatalytic CO2 reduction system enabled by the same biofilm-producing strain. Segregated from the extracellularly mineralized semiconductors, the bacteria remained alive even after 5 cycles of photocatalytic NADH regeneration reactions, and the biofilms could be easily regenerated. Our work thus demonstrates the construction of biocompatible interfaces using biofilm matrices and establishes proof of concept for future sustainable photocatalytic applications.

研究领域: 生物技术 · 材料科学 · 环境科学 · 光化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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International Journal of Nanomedicine · 2020 · IF 5.115

Self-Assembled Dual-Targeted Epirubicin-Hybrid Polydopamine Nanoparticles for Combined Chemo-Photothermal Therapy of Triple-Negative Breast Cancer

Xiang Li,Qian Zou,Jing Zhang,Peng Zhang,Xiong Zhou,Satya Siva Kishan Yalamarty,Xinli Liang,Yali Liu,Qin Zheng,Jianqing Gao

Purpose Folic acid and cyclic arginylglycylaspartic acid peptides were introduced to the surface of negatively charged lipid-coated hybrid polydopamine-cysteine cores for the delivery of epirubicin (EPI) (E/PCF-NPs). The combined chemo-photothermal therapy using E/PCF-NPs for triple-negative breast cancer was evaluated. Materials and Methods The temperature elevation and thermal toxicity of nanoparticles were studied. The morphology and properties of E/PCF-NPs were characterized by transmission electron microscopy, scanning electron microscopy, and atomic force microscopy. Physicochemical properties, including particle size, zeta potential, drug loading, entrapment efficiency (EE%), stability and in vitro release, were determined. The cell viability, reactive oxygen species (ROS) levels, ratios of oxidized nicotinamide adenine dinucleotide to its reduced form (NAD + /NADH), apoptosis assays, and cellular uptake of E/PCF-NPs were determined on 4T1 cells. Pharmacokinetic studies and tissue distributions were performed and detected by an ultra-high performance liquid chromatography/mass spectrometry system. The antitumor effects of E/PCF-NPs under near-infrared (NIR) laser irradiation were also evaluated. Results The sphere-like morphology of E/PCF-NPs showed a high EE%, uniform size of 106.7 nm, remarkable stability, and highly improved cytotoxicity under NIR laser, when compared to that of photothermal treatment alone. In vitro release of EPI from E/PCF-NPs was pH sensitive, and a greater response was achieved under NIR laser irradiation. Compared to chemotherapy or photothermal treatment alone, the combined treatment in vitro significantly inhibited the survival rate of 4T1 cells to 17.7%, induced ROS generation, and reduced NAD + /NADH significantly. Treatment with E/PCF-NPs under irradiation induced 4T1 cell apoptosis in approximately 93.6% cells. In vitro cellular uptake of E/PCF-NPs was time-dependent. The long-circulating and higher tumor accumulation of E/PCF-NPs resulted in complete ablation of breast tumor tissue through the enhanced photothermal effect by NIR laser irradiation-mediated cell apoptosis. Conclusion E/PCF-NPs show enhanced anti-cancer effects due to synergistic effects of chemotherapy with photothermal therapy and may be potential therapeutic agents for cancer treatment.

CAS / MDL: 62-31-7
研究领域: 肿瘤学 · 纳米技术 · 药学 · 生物医学工程
✓ 已验证 产品关联 DOI PubMed 高影响因子
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FREE RADICAL BIOLOGY AND MEDICINE · 2024 · IF 7.1

Targeting ALDH2 to augment platinum-based chemosensitivity through ferroptosis in lung adenocarcinoma

Guangyao Shan,Yunyi Bian,Guangyu Yao,Jiaqi Liang,Haochun Shi,Zhengyang Hu,Zhaolin Zheng,Guoshu Bi,Hong Fan,Cheng Zhan

Ferroptosis is a regulated cell death driven by iron-dependent lipid peroxidation and associated with drug resistance in lung adenocarcinoma (LUAD). It's found that aldehyde dehydrogenase 2 (ALDH2), which is highly mutated in East Asian populations, is correlated with response to chemotherapy in LUAD patients. The rs671 variant knock-in, downregulation, and pharmacological inhibition of ALDH2 render LUAD cells more vulnerable to ferroptosis inducers and platinum-based chemotherapy. ALDH2 inhibits ferroptosis through the detoxification of 4-hydroxynonenal and malondialdehyde, the product of lipid peroxidation, as well as the production of NADH at the same time. Besides, ALDH2 deficiency leads to elevated intracellular pH (pHi), thus inhibiting the ERK/CREB1/GPX4 axis. Interestingly, ALDH2 is also regulated by CREB1, and the ALDH2 enzyme activity was decreased with elevated pHi. What's more, the elevated pHi caused by impaired ALDH2 activity promotes the biosynthesis of lipid droplets to counteract ferroptosis. At last, the effect of ALDH2 on ferroptosis and chemosensitivity is confirmed in patient-derived organoids and xenograft models. Collectively, this study demonstrates that ALDH2 deficiency confers sensitivity to platinum through ferroptosis in LUAD, and targeting ALDH2 is a promising new strategy to enhance the sensitivity of platinum-based chemotherapy for the treatment of LUAD patients.

研究领域: 肿瘤学 · 药理学 · 细胞生物学 · 分子生物学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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INTERNATIONAL BIODETERIORATION & BIODEGRADATION · 2019 · IF 3.824

Aerobic decolorization and detoxification of Acid Scarlet GR by a newly isolated salt-tolerant yeast strain Galactomyces geotrichum GG

Guang Guo,Fang Tian,Yanhong Zhao,Maomao Tang,Weijie Liu,Cong Liu,Shuwen Xue,Weina Kong,Yanmei Sun,Shiwei Wang

Azo dyes are huge social and environmental hazards. Selective fungi are potential degraders for azo dyes and are of great significance to cleaning up and bioremediation. In this study, a salt-tolerant yeast strain GG with the ability to aerobically degrade and detoxify various azo dyes was isolated and identified as Galactomyces geotrichum . The optimal growth and decolorization parameters of strain GG were 0.1 g/L of yeast extract, 2.0 g/L of glucose, 0.4 g/L of ammonium sulfate , ≤ 40 g/L of NaCl, and pH values of 7.0–8.0. Under the optimal condition more than 92% of 100 mg/L of Acid Scarlet GR could be decolorized within 10 h by degradation, which was further confirmed by Fourier transform infrared spectroscopy . In addition, enzymatic analysis showed that the reductase NADH-DCIP and two oxidoreductases lignin peroxidase and laccase played the key roles in the degradation of Acid Scarlet GR, and the decolorization metabolites of Acid Scarlet GR exhibited much less toxicity than the parent dye by phytotoxicity assessment. The results improved the knowledge of azo-dye-decolorizing G. geotrichum species and provided efficient fungal resource for treatment of industrial wastewater containing azo dyes and salts.

研究领域: 环境科学 · 微生物学 · 生物技术
✓ 已验证 DOI 高影响因子
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Advanced Science · 2024 · IF 14.3

Electro-Driven Multi-Enzymatic Cascade Conversion of CO2 to Ethylene Glycol in Nano-Reactor

Likun Luan,Yingfang Zhang,Xiuling Ji,Boxia Guo,Shaoyu Song,Yuhong Huang,Suojiang Zhang

Multi-enzymatic cascade reaction provides a new avenue for C─C coupling directly from CO 2 under mild conditions. In this study, a new pathway with four enzymes including formate dehydrogenase (PaFDH), formaldehyde dehydrogenase (BmFADH), glycolaldehyde synthase (PpGALS), and alcohol dehydrogenase (GoADH) is developed for directly converting CO 2 gas molecules to ethylene glycol (EG) in vitro. A rhodium-based NADH regeneration electrode is constructed to continuously provide the proton and electron of this multi-enzymatic cascade reaction. The prepared electrode can reach the Faradaic Efficiency (FE) of 82.9% at −0.6 V (vs. Ag/AgCl) and the NADH productivity of 0.737 mM h −1 . Shortening the reaction path is crucial for multi-enzymatic cascade reactions. Here, a hydrogen-bonded organic framework (HOF) nano-reactor is successfully developed to immobilize four enzymes in one pot with a striking enzyme loading capacity (990 mg enzyme g −1 material). Through integrating and optimization of NADH electro-regeneration and enzymatic catalysis in one pot, 0.15 mM EG is achieved with an average conversion rate of 7.15 × 10 −7 mmol CO 2 min −1 mg −1 enzymes in 6 h. These results shed light on electro-driven multi-enzymatic cascade conversion of C─C coupling from CO 2 in the nano-reactor.

研究领域: 生物化学 · 生物技术 · 电化学 · 酶工程 · 纳米技术
✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2021 · IF 10.588

Hierarchical porous MoS2 particles: excellent multi-enzyme-like activities, mechanism and its sensitive phenol sensing based on inhibition of sulfite oxidase mimics

Yuanyuan Cai,Lingxi Niu,Xuan Liu,Yujiao Zhang,Zongmei Zheng,Lingxing Zeng,Aihua Liu

It is important to exploit highly efficient methods for detecting pollutants selectively and sensitively. Artificial enzymes are promising to replace natural enzymes with diverse functions for sustainable developments and various applications. However, it remains the challenge to develop novel mimic enzymes or multi-enzyme mimics for pollutant detection. Herein we report hierarchical porous MoS 2 particles prepared by a simple hydrothermal method, which demonstrated excellent sulfite oxidase (SuO x )-, nicotinamide adenine dinucleotide (NADH) oxidase- and superoxide dismutase-mimicking activities. In addition, the catalytic conditions for SuO x -like and NADH oxidase-like activities of MoS 2 were optimized. The catalytic mechanism of the NADH oxidase mimics is that O 2 involves in the oxidation of NADH, to generate O 2 .- intermediate and finally turn to H 2 O 2 , while SuO x mimics comes from that MoS 2 particles can effectively catalyze sulfite to reduce [Fe(CN) 6 ] 3- . Based on the excellent SuO x -like activity of MoS 2 particles, while phenol can inhibit the oxidation of sulfite, a phenol colorimetric sensor was explored with the dynamic range of 2–1000 μM and the limit of detection of 0.72 μM, applicable to detect phenol in effluents. Therefore, MoS 2 particles with the SuO x -like, NADH oxidase-like and SOD-like activities has broad application prospects in environmental monitoring and bio-analysis.

CAS / MDL: 9003-99-0
研究领域: 环境科学 · 材料科学 · 分析化学 · 生物化学
✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Enhanced nitrate removal by biochar supported nano zero-valent iron (nZVI) at biocathode in bioelectrochemical system (BES)

Siqi Zhang,Ziang Kong,Han Wang,Qun Yan,Dimitris V. Vayenas,Guangsheng Zhang

In this study, activated biochar (BC), nano zero-valent iron (nZVI) and biochar supported nano zero-valent iron (BC-nZVI) were used to remove cathodic nitrate in bioelectrochemical system (BES). With an initial NO 3 – -N concentration of 100 mg/L, it was found that the complete nitrate removal could be observed within 28 h for the group of BC-nZVI, whereas the accumulated ammonia reached 63.33 mg/L. Meanwhile, nitrate removal reaction rate constants reached 0.171, 0.110, 0.023 and only 0.010 h −1 for BC-nZVI, nZVI, BC and the Control groups, respectively. Besides, enzymatic activity of nicotinamide adenine dinucleotide (NADH) and nitrous oxide reductase (NOS) of the BC-nZVI group reached the peak faster than three other groups. As a carrier for nZVI, loading of nZVI onto BC could increase the surface area of BC-nZVI other than nZVI for microbial aggregation, while embedded nZVI would contribute to the granulation of sludge and nitrate reduction. Moreover, Cyclic Voltammetry (CV) and chronoamperometry (CA) indicated that BC-nZVI group obtain better electrochemical performances. Importantly, it was found that not only abundances of microbial genus, but relative abundances of those iron mediated enzymes responsible for electro-consuming, hydrogen production and preferential ammonia accumulated nitrate removal could all be enriched. Therefore, BC-nZVI could be implemented to enhance the nitrate removal at biocathode in BES.

CAS / MDL: 16940-66-2
研究领域: 环境工程 · 电化学 · 微生物学 · 水处理
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY · 2024 · IF 5.7

Computer-Aided Flexible Loops Engineering of Glutamate Dehydrogenase for Asymmetric Synthesis of Chiral Pesticides l-phosphinothricin

Kai Yang,Yueshan Huang,Charles Amanze,Liyi Yao,Richmond Anaman,Bin Huang,Weimin Zeng

The access to the enantiopure noncanonical amino acid l-phosphinothricin (l-PPT) by applying biocatalysts is highly appealing in organic chemistry. In this study, a NADH-dependent glutamate dehydrogenase from Lachnospiraceae bacterium (LbGluDH) was chosen for the asymmetric synthesis of l-PPT. Three flexible loops undergoing big conformational shifts during the catalysis were identified and rationally engineered following the initial mutagenesis. The enzyme’s specific activity toward the key precursor of l-PPT, 2-oxo-4-[(hydroxy) (methyl) phosphinyl] butyric acid (PPO), was improved from negligible to 9 U/mg, and the Km value was reduced to 17 mM. The computational analysis showed that the modified loops broadened the enzyme’s narrow tunnels, allowing the substrate to access the binding pocket and get closer to the crucial residue D165, thereby enhancing the catalytic process. Utilizing the variant as the catalyst, the preparation of l-PPT achieved a 100% conversion rate within 60 min, coupled with a stereoselectivity exceeding 99.9%, demonstrating its practical capacity for industrial application. Similar enhancement in catalytic activity was obtained applying the same strategy to a typical NADH-dependent GluDH from Pyrobaculum islandicum (PisGluDH), indicating the effectiveness of our strategy for the protein engineering of GluDHs targeted to the biosynthesis of unnatural compounds.

研究领域: 生物化学 · 生物技术 · 有机化学 · 酶学 · 蛋白质工程
✓ 已验证 DOI PubMed 高影响因子
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SCIENCE OF THE TOTAL ENVIRONMENT · 2019 · IF 5.589

Enhanced denitrification performance of Alcaligenes sp. TB by Pd stimulating to produce membrane adaptation mechanism coupled with nanoscale zero-valent iron

Zeyu Wang,Cong Chen,Huan Liu,Dzmitry Hrynshpan,Tatsiana Savitskaya,Jianmeng Chen,Jun Chen

The microbial reduction of nitrate in the presence of nanoscale zero-valent iron (nZVI) was evaluated to assess the feasibility of employing nZVI for biological denitrification treatment. The effect of modified nZVI on the growth, metabolism, and denitrification performance of Alcaligenes sp. TB under aerobic conditions was studied. Results showed that Alcaligenes sp. TB with nZVI/Pd had 31.5% increase in nitrate removal and 18.1% decrease in nitrite accumulation within 28 h. nZVI/Pd exhibited less inhibition on the cell growth (OD 600  = 0.725), NADH/NAD + ratio (86% of control), and electron transfer system activity (68.5% of control). In addition, nZVI/Pd decreased the membrane fluidity by increasing the trans/cis isomerization ratio (317.7% of control) to enhance the resistance of nZVI. This study underlines the effects of nZVI/Pd on membrane susceptibility via membrane fatty acid transformation during denitrification and suggests the influence of engineered nanomaterials on denitrification.

研究领域: 环境微生物学 · 生物技术 · 水处理
✓ 已验证 产品关联 DOI PubMed 高影响因子
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ENZYME AND MICROBIAL TECHNOLOGY · 2022 · IF 3.705

Enhanced production of D-psicose from D-fructose by a redox-driven multi-enzyme cascade system

Lei Wang,Kecai Chen,Peng Zheng,Xiang Huo,Fei Liao,Liping Zhu,Meirong Hu,Yong Tao

D -Psicose, a new-generation sugar substitute, has been enzymatically synthesized through D -fructose isomerization. However, isomerization often causes low yields due to unfavorable thermodynamic equilibria, which limited its further industrial application. In this study, we present a redox-driven multi-enzyme cascade, two-step biotransformation system to produce D -psicose from D -fructose. Compared to D -fructose isomerization, this method has a maximized theoretical conversion rate of 100%. D -Psicose-3-epimerase from Clostridiales (CBDPE), ribitol 2-dehydrogenase from Providencia alcalifaciens (PRDH), and formate dehydrogenase from Starkeya (SFDH) were co-expressed in Escherichia coli in the first step to produce D -allitol from D -fructose. Afterward, NADH oxidase from Streptococcus pyogenes (SPNOX), and ribitol 2-dehydrogenase from Rubrivivax sp. (RSRDH) were co-expressed in E. coli to oxidize D -allitol into D -psicose in the second step. The two-step biotransformation system was optimized to maximize the D -fructose-to- D -psicose conversion rate (up to 90%), corresponding to a concentration of 450 mM. This study suggests that this redox-driven multi-enzyme cascade strategy through a sugar-to-alcohol-to-sugar pathway has the advantage of great application for enhanced production of D -psicose and other rare sugars.

CAS / MDL: 488-44-8 50-70-4 57-48-7
研究领域: 生物化学 · 生物技术 · 酶学 · 代谢工程
✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Nano-sized mesoporous hydrogen-bonded organic frameworks for in situ enzyme immobilization

Wenping Li,Jiafu Shi,Yu Chen,Xinyue Liu,Xiangxuan Meng,Zheyuan Guo,Shihao Li,Boyu Zhang,Zhongyi Jiang

Hydrogen-bonded organic frameworks (HOFs) are promising carriers for enzyme immobilization. HOFs suitable for enzyme reactions containing nicotinamide cofactors and/or larger molecule substrates are to be explored. Herein, we report the first example of nano-sized mesoporous HOFs ( nm HOFs) for in situ enzyme immobilization. Taking tetrakis(4-amidiniumphenyl) methane (TAM) and 1,3,6,8-tetrakis(p-benzoic acid) pyrene (H 4 TBAPy) as building blocks, enzymes induce the assembly of TAM and H 4 TBAPy into enzyme- nm HOF (named [email protected] ) in aqueous solution. The larger π-conjugated H 4 TBAPy building block and the electrostatic/hydrogen-bonding interactions between TAM in nm HOF and –COOH/–NH 2 residues in enzymes trigger the formation of TaTb with pore aperture of 2.4 nm and particle size from 19.9 ± 6.4 to 56.4 ± 20.1 nm. As a demonstration, lactate dehydrogenase (LDH) that can convert pyruvate into lactate in the presence of NADH is immobilized in TaTb nm HOF. Compared with [email protected] and [email protected] , [email protected] affords faster diffusion of NADH and pyruvate, thus exhibiting ultrahigh activity close to the free LDH. Meanwhile, the exoskeleton of TaTb nm HOF is capable of stabilizing enzymes through spatial confinement, rendering superior stability against external negative stimuli. The TaTb nm HOF is also used for immobilizing α-amylase and horseradish peroxidase. Our study may facilitate the development of HOFs into platform carriers for enzyme immobilization.

研究领域: 材料科学 · 生物化学 · 化学工程
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BIOMEDICINE & PHARMACOTHERAPY · 2024 · IF 6.9

Aqueous extract of Phellinus igniarius ameliorates hyperuricemia and renal injury in adenine/potassium oxonate-treated mice

Lei Wang,Yufeng Tao,Xuesong Wang,Yuhan Gan,Yuting Zeng,Shasha Li,Qing Zhu

Phellinus igniarius is an important medicinal and edible fungus with diverse biological activities. This study aimed to investigate the effects of aqueous extract from P. igniarius (API) on the treatment of hyperuricemia (HUA) and related kidney damage. The chemical constituents of API were determined. The therapeutic effects of API on HUA and renal injury were assessed in adenine/potassium oxonate (PO)-treated mice. The constituent analysis of API revealed a predominance of polysaccharides (33.4 %), followed by total flavonoids (9.1 %), and total triterpenoids (3.5 %). Compared to control, the adenine/PO treatment greatly elevated serum uric acid (UA) levels but this elevation was attenuated by API. In the liver, the expression and activity of xanthine oxidase (XOD) were increased by HUA which were diminished by API. Furthermore, API was found to enhance the expression of UA transporter ABCG2 in the kidney and intestine of HUA mice, suggesting elevating UA excretion. Additionally, API ameliorated HUA-induced renal injury, as indicated by reduced serum BUN/creatinine levels, decreased glomerular and tubular damage, and lowered fibrotic levels. Network pharmacology analysis predicted that P. igniarius may regulate mitochondrial function to improve HUA-related renal injury. This prediction was then substantialized by the API-induced upregulation of NAD+/NADH ratio, ATP level, SOD2 activity, and expression of SOD2/PCG-1α/PPARγ in the kidney of HUA mice. Our results demonstrate that API may effectively ameliorate HUA by reducing UA production in the liver and enhancing UA excretion in the kidney and intestine, and it might be a potential therapy to HUA-related renal injury.

研究领域: 药理学 · 医学 · 生物化学 · 分子生物学
✓ 已验证 DOI PubMed 高影响因子
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