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Journal of Energy Chemistry · 2024 · IF 14

Influence of O–O formation pathways and charge transfer mediator on lipid bilayer membrane-like photoanodes for water oxidation

Yingzheng Li,Shaoqi Zhan,Zijian Deng,Meng Chen,Yilong Zhao,Chang Liu,Ziqi Zhao,Hongxia Ning,Wenlong Li,Fei Li,Licheng Sun,Fusheng Li

Inspired by the function of crucial components in photosystem II (PSII), electrochemical and dye-sensitized photoelectrochemical (DSPEC) water oxidation devices were constructed by the self-assembly of well-designed amphipathic Ru(bda)-based catalysts (bda = 2,2ʹ-bipyrdine-6,6ʹ-dicarbonoxyl acid) and aliphatic chain decorated electrode surfaces, forming lipid bilayer membrane (LBM)-like structures. The Ru(bda) catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O–O formation mechanisms. However, compared to the slow charge transfer process, the O–O formation pathways did not determine the PEC water oxidation efficiency of the dye-sensitized photoanodes, and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs. Instead, charge transfer plays a decisive role in the PEC water oxidation rate. When an indolo[3,2-b] carbazole derivative was introduced between the Ru(bda) catalysts and aliphatic chain-modified photosensitizer in LBM films, serving as a charge transfer mediator for the tyrosine-histidine pair in PSII, the PEC water oxidation performance of the corresponding photoanodes was dramatically enhanced.

研究领域: 生物化学 · 材料科学
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Biomicrofluidics · 2016 ·Vol. 10 ·期 6 · IF 2.708

Label-free discrimination of membrane-translocating peptides on porous silicon microfluidic biosensors

Li Zhen,Luo Qiaohui,Wu Jianmin

A label-free optical sensor was constructed by integrating electrochemically etched porous silicon (pSi) and supported phospholipid bilayers in a microfluidic chip. The translocation of peptides through the phospholipid bilayers could induce a red shift in effective optical thickness of the pSi layer, which could be monitored by reflective interferometric Fourier transform spectroscopy. By measuring the kinetic data of membrane translocating on the phospholipid bilayers/pSi chip, the relationship between the behavior of membrane-translocating peptides (MTPs) and translocating mechanism was established. With these optical data, MTPs with different action modes on the cell membrane can be correctly discriminated. The bio-functionalized microfluidic sensor will provide a reliable and cost-effective platform to study the transmembrane behavior of peptides, which is of great importance in the MTP screening and peptide function study.

CAS / MDL: 596-09-8
研究领域: 生物传感器 · 分析化学 · 分子生物学
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NEW JOURNAL OF CHEMISTRY · 2022 ·Vol. 46 ·期 16 ·7748-7757 · IF 3.925

Structural effects of zinc on phosphatidylserine-containing lipid membranes: kinetic analysis of membrane reorganization

Danling Cheng,Hewen Li,Shipeng Hu,Tao Zhao

The interaction between metal ions and phospholipids plays an essential role in cellular signal transduction, oxidative lipid damage and other biological processes. Herein, we report fluorescence microscopy analysis of the interaction between Zn2+ on planar supported lipid bilayers (SLBs), as model membranes. The results show that Zn2+ interacts with palmitoyl oleoyl phosphatidylserine (POPS), a negatively charged phospholipid, in palmitoyl oleoyl phosphatidylcholine (POPC) SLBs, which leads to significant structural reorganization of the bilayer. Upon Zn2+ binding, the formation of bilayer stacks was observed, which led to the subsequent disruption of the membrane. The kinetics of bilayer stack formation could be described with a characteristic sigmoidal profile and a three-stage mechanism consisting of a lag phase for initial nucleation (formation of stable nuclei), a subsequent exponential phase for growth (growth of nuclei to bilayer stacks) and a final stationary phase was proposed. The lag time reduced in an exponential fashion with increasing Zn2+ concentration and the lag phase could be essentially eliminated in SLBs with high POPS content. Moreover, a linear dependency of the apparent first-order rate constant for bilayer stack growth on Zn2+ concentration was established. Besides, the equilibrium dissociation constants for Zn2+-membrane interaction were calculated and the affinity between Zn2+ and SLBs increased with an increase in the POPS content in the membrane. These results have important implications in general understanding of ion-mediated malformations of cell membranes and cell fusion. Also, this work provides an interesting in vitro system for studying metal ions interacting with biomembranes.

研究领域: 生物物理 · 细胞生物学 · 膜科学
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CHEMISTRY OF MATERIALS · 2017 · IF 9.466

Zr-Based MOFs Shielded with Phospholipid Bilayers: Improved Biostability and Cell Uptake for Biological Applications

Jian Yang,Xiaojing Chen,Yongsheng Li,Qixin Zhuang,Peifeng Liu,Jinlou Gu

For practical biomedical applications, the stabilization of nanoscale metal–organic frameworks (NMOFs) in the presence of phosphate is of prime importance but remains a significant challenge because of the inevitable and strong driving force between metal clusters and phosphate species to form metal-phosphate in physiological environments. Through shielding Zr-NMOFs within the continuous phospholipid bilayers (PBLs), herein, we figured out a unique way to protect the vulnerable coordination bonds in their frameworks from the attack of phosphate. To exemplify the facility of constructing PBLs on Zr-NMOFs core, a porphyrinic NMOF of PCN-223 (standing for a platform with broad biological applications) was elaborated using a triethylamine (TEA)-modulated strategy. TEA could not only control the phase transformation of porphyrinic MOFs to achieve pure-phase PCN-223 crystals but also minimize their particles size down to sub-200 nm. Negative-stained TEM, FT-IR and XPS techniques revealed that PBLs could be closely coated onto the surface of nanoPCN-223, thanks to the strong Zr–O–P chemical complexation between Zr-NMOFs and phospholipid. The resultant coated nanoPCN-223 exhibited significantly enhanced phosphatic-resistance in phosphate buffer solution (PBS) and presented exceptional stability in harsh chemical environments. Furthermore, the MOFs-supported PBLs could effectively provide a stable biocompatible interface for subsequent cell culture and improve their biocompatibility, cellular uptake efficiency and real biostability of NMOFs in cellular environments. This study offers an alternative system for forming stable PBLs supported on NMOFs, and represents the first example of stabilizing Zr-NMOFs free from the attack of phosphate species in biological media.

研究领域: 纳米技术 · 生物医学工程 · 材料科学 · 生物材料
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INTERNATIONAL JOURNAL OF PHARMACEUTICS · 2017 · IF 3.649

Carboxymethyl chitosan/phospholipid bilayer-capped mesoporous carbon nanoparticles with pH-responsive and prolonged release properties for oral delivery of the antitumor drug, Docetaxel

Yanzhuo Zhang,Wufu Zhu,Heran Zhang,Jin Han,Lihua Zhang,Qisi Lin,Fengwei Ai

In this article, a new type of carboxymethyl chitosan/phospholipid bilayer-capped mesoporous carbon nanomatrix (CCS/PL/MC) was fabricated as a potential nano-drug delivery system. In this drug delivery system, a mesoporous carbon nanomatrix (MC) acts as the support for loading drug molecules, a positively charged phospholipid (PL) layer works as the inner shell for prolonged drug release and a negatively charged carboxymethyl chitosan (CCS) layer serves as the outer shell for pH-responsive drug release. Docetaxel (DTX) was selected as a model drug. The drug-loaded CCS/PL/MC was synthesized via a combination approach of double emulsion/solvent evaporation followed by lyophilization. The drug-loaded nanoparticles were characterized for their particle size, structure, morphology, zeta (ζ)-potential, specific surface area, porosity, drug loading and solid state. In vitro drug release tests showed that the drug-loaded CCS/PL/MC nanoparticles possess a good pH-sensitivity and prolonged releasing ability with negligible release in gastric media and controlled release in intestinal media. Compared with MC and PL-capped MC, CCS/PL/MC had a greater mucoadhesiveness. Moreover, cellular uptake study indicated that CCS/PL/MC might improve intracellular drug delivery. These results suggest that this hybrid nanocarrier, combining the beneficial features of CCS, PL and MC, is a promising drug delivery system able to improve the oral absorption of antitumor drugs.

研究领域: 药剂学 · 纳米医学 · 肿瘤学
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ANALYTICAL CHEMISTRY · 2021 · IF 6.986

Antibody-Free Determinations of Low-Mass, Soluble Oligomers of Aβ42 and Aβ40 by Planar Bilayer Lipid Membrane-Based Electrochemical Biosensor

Yuemei Duan,Jia Chen,Yan Jin,Qiuyun Tu,Shuhui Wang,Juan Xiang

Alzheimer’s disease (AD) is the most common neurodegenerative disease among the elderly. Abnormal aggregates of both β-amyloid peptide (Aβ) subtypes, Aβ42 and Aβ40, are the typical neuropathology hallmarks of AD. However, because of the lack of specific recognition elements such as an antibody and aptamer, it is difficult to differentiate and determine the oligomers of Aβ42 and Aβ40 in clinic. In this paper, we developed a planar bilayer lipid membrane (BLM)-based electrochemical biosensor. According to the dynamic differences on oligomer-induced BLM damage, both low-mass, soluble oligomers of Aβ42 and Aβ40 (L-Aβ42O and L-Aβ40O) were measured in turn by electrochemical impedance spectroscopy. The BLM was supported by a porous 11-mercaptoundecanoic acid layer on a gold electrode, which amplified the impedance signal corresponding to the membrane damage and improved the detection sensitivity. The weakly charged surface of the BLM ensured the low non-specific adsorption of coexisting proteins in cerebrospinal fluid (CSF). Using the electrochemical biosensor, L-Aβ42O was determined within 20 min, with a linear range from 5 to 500 pM and a detection limit of 3 pM. Meanwhile, L-Aβ40O was determined within 60 min, with a linear range from 60 pM to 6.0 nM and a detection limit of 26 pM. The recoveries in oligomer-spiked artificial CSF and human CSF samples confirmed the accuracy and applicability of this proposed method in clinic. This work provides an antibody-free, highly selective, and sensitive method for simultaneous detections of L-Aβ42O and L-Aβ40O in real CSF samples, which is significant for the early diagnosis and prognosis of AD.

研究领域: 神经科学 · 生物医学工程 · 分析化学
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CHEMICAL ENGINEERING JOURNAL · 2025 · IF 13.2

Polyphenol-based coacervate droplets as building blocks for protocells and prototissues

Qi Xie,Wei Chen,Zijian Huang,Yuan Gao,Haoyu Zhang,Zhanhao Zhou,Samira Batur,Chuansheng Fu,Jiao Zhang,Conglian Yang,Junjun Liu,Li Kong,Zhiping Zhang

Despite the nascent stage of research into protocells and prototissues, their substantial potential has increasingly positioned them as a focal point in recent years. The bottom-up reconstruction of life systems is gradually garnering widespread attention. In this study, a type of protocells and corresponding prototissues based on polyphenol coacervate droplets were developed via hydrogen bond interactions. The droplets exhibited properties reminiscent of cytoplasm, enriching a wide range of substances. Upon further modification with lipid bilayers, the protocells not only achieved a structural resemblance to natural cells, but also effectively maintained the stability. Prototissues formed by the orderly aggregation of protocells can not only encapsulate living cells, but also maintain the structural integrity and function of both artificial and living cells. At the macroscopic level, the prototissues were injectable, customizable in shape, bioadhesive, and capable of long-term retention in vivo. Moreover, the prototissues showed no obvious inflammatory responses. Polyphenol-based protocells and tissues with unique characteristics may offer new insights for research and applications in organoids, transplantation, and medical devices.

研究领域: 合成生物学 · 生物物理学 · 材料科学 · 生物工程 · 细胞生物学 · 组织工程
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BIOSENSORS & BIOELECTRONICS · 2021 · IF 10.618

A sandwich-based evanescent wave fluorescent biosensor for simple, real-time exosome detection†

Shuting Li,Liye Zhu,Longjiao Zhu,Xiaohong Mei,Wentao Xu

Exosomes are regarded as a promising biomarker for the noninvasive diagnosis and treatment of diseases. The value of exosomes for medical research has promoted the search for a fast, efficient, and sensitive detection method. This study reported a sandwich-based evanescent wave fluorescent biosensor (S-EWFB) for exosome detection. A two-step strategy was implemented to take advantages of the simple binding of fluorescent probes with exosomes via the hydrophobic interaction between the cholesteryl and phospholipid bilayer membrane , as well as real-time detection on an evanescent wave liquid-solid interface based on CD63 aptamer-specific capture to form an exosome@fluorescence probe/aptamer sandwich structure. The one-to-many connection between exosomes and signal molecules and the aptamer-modified evanescent wave optical fiber detection platform reduced the detection limit of exosomes to 7.66 particles/mL, with a linear range of 47.5–4.75 × 10 6 particles/mL. The entire detection process was simple, rapid, and real-time and lasted about 1 h while requiring no separation and purification . Additionally, this platform showed excellent surface regeneration capability and exhibited good performance during the analysis of tumor and non-tumor-derived exosomes.

研究领域: 生物传感 · 生物医学工程 · 纳米技术 · 分子生物学 · 癌症研究
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Advanced Science · 2024 · IF 14.3

Artificial Neutrophils Against Vascular Graft Infection

Wentao Jiang,Huizi Xu,Zheng Gao,Ziyu Wu,Zichun Zhao,Jun Wang,Yawen Wu,Haifeng Ke,Chun Mao,Mimi Wan,Min Zhou

Efficient neutrophil migration to infection sites plays a vital role in the body's defense against bacterial infections and natural immune responses. Neutrophils have a short lifespan and cannot be mass-cultured in vitro. Therefore, developing more stable artificial neutrophils (AN) in a controllable manner has become a research focus. However, existing AN lack chemotaxis, which is the ability to migrate toward high-signal-concentration positions in a dynamic blood- flow environment. Supplying AN with chemotaxis is key to designing AN that are more similar to natural neutrophils in terms of morphology and function. In this study, micrometer-sized, spherical, biocompatible AN are developed. These AN consist of zeolitic imidazolate framework-8 nanoparticles encapsulating two enzymes, coacervate droplet frameworks, and outer phospholipid bilayers carrying enzymes. The AN exhibit responsiveness to elevated hydrogen peroxide levels at inflammation sites, actively chemotaxing toward these sites along concentration gradients. They also demonstrate effective combat against Staphylococcus aureus infections. The capabilities of the AN are further validated through in vitro experiments and in vivo evaluations using vascular graft infection models. This study replicates natural neutrophils in terms of chemical composition, functionality, and physiological impact. It introduces new ideas for advancing the development of advanced artificial cells.

研究领域: 生物医学工程 · 免疫学 · 纳米技术 · 传染病
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COLLOIDS AND SURFACES B-BIOINTERFACES · 2022 · IF 5.999

The spatial arrangement of astaxanthin in bilayers greatly influenced the structural stability of DPPC liposomes

Lijun Ding,Jie Yang,Kangrui Yin,Hao Cheng,Jing Li,Changhu Xue

Liposomes are regarded as the ideal nanocarrier for concurrent or separate delivery of nutraceuticals in the food industries. Precise control of the structural stability is essential for the processing, storage, and nutrition delivery of liposomes. Astaxanthin was found to significantly affect the membrane stability of liposomes by inserting into the phospholipid bilayers in a similar way to cholesterol. Compared with cholesterol, astaxanthin could significantly improve the phase transition temperature, membrane fluidity , and membrane compactness of liposomes. Additionally, the membrane stability was well modulated by controlling the distribution patterns of astaxanthin (monomers, H- and J-aggregates) in bilayers. For instance, astaxanthin H-aggregates could endow the liposomal membrane with highest rigidity and compactness. Additionally, astaxanthin aggregates, especially J-aggregates could greatly improve storage stability of liposomes, thus providing a novel strategy to regulate and optimize the stability of liposomes for their diversified applications.

CAS / MDL: 472-61-7
研究领域: 纳米技术 · 食品科学 · 药学
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