Journal of the American Chemical Society
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2025
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IF 15.6
Pei Liu,Mengmeng Zheng,Yue Wang,Xiang-Yu Kong,Yingjie Zhao,Mengru Zhang,Qun Xu,Lei Jiang,Liping Wen
The process of photosynthesis in green plants and energy conversion in certain archaea are inseparable from photoregulated ion pumping. Two-dimensional (2D) nanofluidic membranes, emerging as competitive candidates for constructing ion pumps, present intriguing prospects for harvesting light energy. However, the inevitable presence of defects during the synthesis of 2D materials underscores the critical need to understand their impact on ion transport dynamics within nanofluidic systems. Here, we present a chemically engineered asymmetric nanofluidic membrane (ANM) by intercalating molybdenum trioxide (MoO3) with controlled oxygen vacancies into graphene oxide laminates, systematically investigating the defect chemistry-governed photo-activated ion transport. Upon photoexcitation, MoO3 nanosheets exhibit tunable surface plasmon resonance (SPR) through photochemical H+ intercalation, leading to an augmentation of oxygen vacancies and an elevated concentration of free electrons. These vacancies enrich MoO3 with excess localized surface electrons, enabling tunable SPR that creates negative charge centers and significantly enhances space charge through defect-induced polarization. Density functional theory (DFT) calculations reveal the atomic-level mechanism of vacancy-enhanced cation transport, showing a notable 188% increase in the adsorption energy of K+ at MoO3 surfaces with two vacancy sites compared to one vacancy (−13.66 vs −4.74 eV). Under asymmetric photo irradiation, the system achieves a peak power density of approximately 439.2 W/cm2 in equilibrium ionic solutions, realizing a photonic-to-ionic energy conversion efficiency of 7.98 × 10–4% via synergistic effects of defects and plasmonics. Our research pioneers the elucidation of the regulation and underlying mechanisms of intrinsic defects on active ion transport within nanofluidic membranes, while fostering a novel perspective on photon–electron–ion interplay within nanofluidic environments.
研究领域:
纳米流体学
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能量转换
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材料科学
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物理化学
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光子学
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电化学
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凝聚态物理
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2019
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IF 8.456
Junji Li,Xiao-Yang Tian,Li-Ping Zong,Qiang Zhang,Xue-Ji Zhang,Robert Marks,Serge Cosnier,Dan Shan
Glycopolymers have emerged as powerful and versatile glycan analogues for the investigation of cellular signal transduction. In this study, a layer of the glycopolymer-brush (GlyB) interface was functionalized on the surface of gold substrates. In order to enhance the capability and accessibility of this transducer interface, a combined protocol of copper(0)-mediated living radical polymerization (Cu(0)-LRP) with subsequent “CuAAC” click reaction was utilized to synthesize a set of novel glycopolymer precursors with a tunable scaffold structure and pyranose ligands. The resulting glycopolymer exhibited a fine-tuned molecular weight with a minor dispersity of 1.27. Through surface plasmon resonance (SPR) analysis, various GlyB interfaces exhibiting different saccharide moieties (glucose, mannose, and galactose) were examined to study their adhesion or antiadhesion potential toward three types of proteins, concanavalin A, bovine serum albumin, and peanut agglutinin (PNA). The strong affinity between poly(galactose) and PNA was further employed to construct a proof-of-concept aggregation-mediated sensing system. This minimal naked-eye sensor that consisted of only two substances, namely, gold nanoparticles and glycopolymers, was characterized and tested for its potential in protein quantification.
研究领域:
材料科学
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聚合物化学
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生物技术
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分析化学
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 17
·6992-7000
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IF 3.288
Tehseen Nawaz,Muhammad Ahmad,Jieying Yu,Shiqi Wang,Tianxin Wei
Novel bifunctional group monomer itaconic acid (IA) based molecularly imprinted polymers (MIPs) were successfully prepared with hydrogen bonding interactions by applying a facile combination of a reversible addition chain transfer mechanism (RAFT) and surface plasmon resonance (SPR). UV photo-polymerization in synergy with 2-methyl-2-[(dodecylsulfanylthiocarbonyl)sulfanyl]propanoic acid (TTCA) as a chain transfer reagent was employed for MIP film synthesis on an SPR sensor chip for the detection of progesterone using ethylene glycol dimethacrylate (EGDMA) as a cross linker. In addition, the ratio of template to bifunctional group monomer to cross linker was optimized (1 : 2 : 12) by real-time SPR monitoring. The modified surface of the biosensor was characterized by contact angle measurements, frontier transfer infrared spectroscopy (FTIR) and scanning electron microscopy (SEM). The resulting itaconic acid based MIP (IA based MIP) biosensor showed a high adsorption capacity and excellent selectivity in comparison to other analogues and non-imprinted polymer (NIP) film. Through 8 adsorption–desorption cycles, the high recoverability of IA based MIP film was confirmed. These features suggested that IA based MIPs are ideal candidates for biosensor use owing to the bifunctionality of the monomer. Consequently, within the concentration range of 1 × 10−18 to 1 × 10−8 mol L−1, the coupling angle change of SPR versus the negative logarithm of concentration showed excellent linearity: R2 = 0.99. Based on a linear equation, IA based MIPs showed excellent values for the limit of detection (LOD) and limit of quantification (LOQ), i.e. 0.28 × 10−19 mol L−1 and 0.92 × 10−19 mol L−1, respectively. Furthermore, the influence of the matrix on the biosensor was successfully analyzed in real samples with satisfactory outcomes, displaying identical behavior to ideal samples. Hence, IA based MIPs in combination with an SPR sensor chip demonstrated potential applications for rapid and highly effective sensing even in complicated matrices.
研究领域:
分析化学
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生物传感器
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高分子科学
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材料科学
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生物技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Nini Luo,Yue Shu,Chuanlong Zhu,Xiaoxue Cheng,Lixue Chen,Jiang Wang,Rui Liu,Huangxian Ju,Wei Cheng,Qianfeng Xia
The abnormal protein phosphorylation is closely related to a series of diseases including cancers, neurodegeneration, and other immune/inflammatory disorders. However, a simple, accurate, and pragmatic methodology for the direct detection of phosphorylation levels of target proteins is largely unavailable. Herein, a surface plasma resonance (SPR) biosensor was developed to detect phosphorylated protein based on significant SPR enhancement using UiO-66 and its high affinity for phosphate residues. Furthermore, the pH of the incubation buffer and the NaOH concentration in the washing solution to eliminate nonspecific adsorption of nanoparticles on the chip surface were optimized to adjust the surface charges of UiO-66. This improved the specificity and sensitivity of the proposed method. The designed biosensor could distinguish 1% phosphorylated peptides from non-phosphorylated peptides background. Moreover, the method could directly analyze the phosphorylation level of target protein in complex samples such as cell or tissue extracts without requiring a purification step in a single workflow. This simple and robust biosensor is a sensitive, accurate, and pragmatic toolbox to detect phosphorylated proteins without destroying the protein structure and can significantly facilitate phosphoproteomics and clinical diagnosis research.
研究领域:
生物传感
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蛋白质组学
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生物医学工程
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分析化学
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分子生物学
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临床诊断
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DOI
高影响因子
危险品化学品经营许可证（带存储）