IF 4.5 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2026-10-01 Epub Date: 2026-03-04 DOI: 10.1016/j.bioelechem.2026.109264

Caio C.G. Silva , Alessandro Cacia , Hernán D. Rojas-Mantilla , Maria V.B. Zanoni , Saulo S. Garrido , Felipe Conzuelo

Photobioelectrochemical systems (PBEs) harness the machinery of photosynthetic microorganisms to convert solar energy into electricity. However, the inefficient electron transfer at the cell-electrode interface remains as the key performance limitation. Herein, we report a plasmonic biohybrid strategy to enhance extracellular electron transfer in Chlorella-based photobioelectrodes by integrating gold nanoparticles (AuNPs) localized on the microalgae membrane. Two approaches are investigated, consisting of physical mixing of isolated cells with AuNPs and cultivating microalgae in a growth medium supplemented with AuNPs, with the second approach allowing to obtain about significantly higher photocurrent responses. Optimized bioelectrodes yield photocurrent densities of up to 132 μA cm⁻², 74% higher than bioelectrodes fabricated using unmodified cells. Spectral response analysis reveals a strong resonance at 525 nm, consistent with the plasmonic properties of AuNPs. Importantly, pigment content, growth kinetics, and membrane integrity are preserved, confirming the biocompatibility of the modification. This work presents a facile and effective route to engineer photosynthetic bioelectrodes using nanomaterials, advancing the design of high-performance PBEs for solar-to-electricity conversion.

光生物电化学系统（PBEs）利用光合微生物的机制将太阳能转化为电能。然而，电池-电极界面的低效率电子转移仍然是主要的性能限制。在此，我们报道了一种等离子体生物杂交策略，通过整合定位在微藻膜上的金纳米颗粒（AuNPs）来增强小球藻基光生物电极的细胞外电子转移。研究人员研究了两种方法，一种是将分离细胞与AuNPs物理混合，另一种是在添加了AuNPs的生长培养基中培养微藻，第二种方法可以获得更高的光电流响应。优化后的生物电极产生的光电流密度高达132 μA cm−2，比使用未修饰的细胞制备的生物电极高74%。光谱响应分析显示在525 nm处有强烈的共振，与AuNPs的等离子体特性一致。重要的是，色素含量、生长动力学和膜完整性都得到了保存，证实了改性的生物相容性。这项工作提出了一种简单有效的途径来利用纳米材料设计光合生物电极，推进了高性能PBEs的设计，用于太阳能到电力的转换。

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引用次数: 0

Anthraquinone disulfonate as a stable redox mediator for efficient air-cathodes at neutral pH in dual-chamber microbial fuel cells 二磺酸蒽醌作为双室微生物燃料电池中性pH下高效空气阴极的氧化还原介质

IF 4.5 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2026-10-01 Epub Date: 2026-03-09 DOI: 10.1016/j.bioelechem.2026.109279

Antoine Vautier, James A. Behan, Charlotte Bodin, Florence Geneste, Frédéric Barrière

Microbial Fuel Cells (MFCs) are commonly developed as organic-matter oxidizing bioanodes with abiotic air cathodes. However, O₂ reduction requires active aeration and/or the use of expensive catalysts using noble metals. In this study, 2,7-anthraquinone disulfonate (2,7-AQDS), an organic redox mediator commonly used in aqueous redox flow battery systems (AORFBs), served as a redox-stable intermediate for oxygen reduction. Dual-chamber MFC pilots were developed with 2,7-AQDS in the catholyte under both anoxic and aerobic conditions and compared to pilots with ferricyanide catholytes. In both conditions, cyclic voltammetry studies confirmed similar and efficient electroactivity despite the proximity AQDS formal redox potential to that of acetate oxidation. Mediated air-cathodes achieved open-circuit voltage (OCV) of 510 mV and current densities of 140 μA/cm², nearly double those of air-only cathodes (72 μA/cm²), while delivering a 33% higher power density (12 mW/m² vs. 8 mW/m²). Passive catholyte aeration enabled continuous reoxidation of reduced 2,7-AQDS at 8.8 × 10⁻⁸ mol/s, exceeding the AQDS reduction rate by the bioanode (2.5 × 10⁻¹⁰ mol/s), thus ensuring effective self-regeneration and stable AQDS concentration. These results demonstrate that AQDS coupled with passive oxygen supply sustains biofilm activity with enhances current and power, and allow long-term / low-maintenance MFC operation and organic-matter oxidation.

微生物燃料电池（mfc）通常被开发为有机物氧化生物阳极和非生物空气阴极。然而，O2还原需要主动曝气和/或使用昂贵的贵金属催化剂。在本研究中，2,7-蒽醌二磺酸盐（2,7- aqds）作为水氧化还原液流电池系统（AORFBs）中常用的有机氧化还原介质，作为氧还原的氧化还原稳定中间体。在缺氧和有氧条件下培养具有2,7- aqds的双室MFC飞行员，并与具有铁氰化阴极的飞行员进行比较。在这两种情况下，循环伏安法研究证实，尽管AQDS形式氧化还原电位与醋酸氧化电位接近，但电活性相似且有效。介质空气阴极的开路电压（OCV）为510 mV，电流密度为140 μA/cm2，几乎是纯空气阴极（72 μA/cm2）的两倍，而功率密度（12 mW/m2 vs. 8 mW/m2）提高了33%。被动阴极曝气使还原的2,7-AQDS以8.8 × 10−8 mol/s的速度连续再氧化，超过了生物阳极对AQDS的还原速率（2.5 × 10−10 mol/s），从而保证了有效的自再生和稳定的AQDS浓度。这些结果表明，AQDS与被动供氧相结合，可以在增强电流和功率的情况下维持生物膜的活性，并允许长期/低维护的MFC运行和有机物氧化。

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引用次数: 0

Developing fast scan cyclic voltammetry at carbon fiber microelectrodes to quantify short chain fatty acids in situ 碳纤维微电极快速扫描循环伏安法原位定量短链脂肪酸。

IF 4.5 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2026-10-01 Epub Date: 2026-03-04 DOI: 10.1016/j.bioelechem.2026.109266

Terdha Narla , Uma Nudurupati, Yangguang Ou

Acetic, propionic, and butyric acids are short chain fatty acids (SCFAs) and the most abundant metabolites produced by gut bacteria. To uncover mechanistic insights of their function throughout the body, it is critical to measure rapid SCFA fluxes in sites of action such as brain, muscle, and skin. Current approaches have focused on fecal and plasma measurements, where SCFA levels are low and not representative of tissue-specific concentrations or fluxes. Thus, a rapid, in situ methodology is needed. Fast scan cyclic voltammetry (FSCV) at carbon fiber microelectrodes (CFMs) has the spatiotemporal resolution to fill this need. However, the electrochemical response of CFMs to SCFAs have not been explored until now. By coupling FSCV at CFMs with flow injection analysis of each SCFA, we demonstrate there are distinct peaks in the cyclic voltammograms for each fatty acid. Some of these peaks display faradaic behavior in scan rate, holding potential, and switching potential experiments. Interestingly, we identify several peaks that are concentration-sensitive and therefore are promising quantifiable markers of SCFA dynamics and fluxes. This work lays the foundation in understanding the response of CFMs to fatty acids and demonstrate the utility of FSCV at CFMs for the in situ quantitation of SCFAs.

乙酸、丙酸和丁酸是短链脂肪酸（SCFAs），是肠道细菌产生的最丰富的代谢物。为了揭示其在全身功能的机制，测量脑、肌肉和皮肤等作用部位的快速SCFA通量至关重要。目前的方法主要集中在粪便和血浆测量，其中SCFA水平较低，不能代表组织特异性浓度或通量。因此，需要一种快速的就地方法。碳纤维微电极（CFMs）的快速扫描循环伏安法（FSCV）具有满足这一需求的时空分辨率。然而，cfm对scfa的电化学响应目前还没有研究。通过将cfm的FSCV与每种SCFA的流动注射分析相结合，我们发现每种脂肪酸的循环伏安图中都有不同的峰。其中一些峰在扫描速率、保持电位和开关电位实验中显示出法拉第行为。有趣的是，我们发现了几个对浓度敏感的峰，因此是有希望的SCFA动态和通量的可量化标记。这项工作为理解cfm对脂肪酸的反应奠定了基础，并证明了FSCV在cfm中用于scfa原位定量的实用性。

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引用次数: 0

Nanotip acetylcholine biosensor reveals cholinergic differentiated SH-SY5Y cells release partial vesicle content during exocytosis 纳米尖端乙酰胆碱生物传感器显示胆碱能分化的SH-SY5Y细胞在胞吐过程中释放部分囊泡内容物

IF 4.5 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2026-10-01 Epub Date: 2026-02-26 DOI: 10.1016/j.bioelechem.2026.109260

Yuanmo Wang , Ajay Pradhan , Pankaj Gupta , Jörg Hanrieder , Henrik Zetterberg , Ann-Sofie Cans

Acetylcholine (ACh) is a central neurotransmitter in cognitive function, motor control, and synaptic modulation, yet its electrochemical inactivity and the rapid kinetics of exocytosis have hindered real-time quantal measurements. Micrometer-scale enzymatic ACh biosensors previously enabled sub-millisecond extracellular recordings but were too large for synaptic positioning and intracellular recordings. Here we present a short, ultrafast and low-noise amperometric ACh biosensor based on a needle-shaped carbon fiber nanotip electrode functionalized with gold nanoparticles and enzymes. The miniaturized geometry allows precise placement at neurite release sites and minimally invasive insertion into the cell cytoplasm, enabling high-temporal resolution monitoring of presynaptic exocytosis together with quantification of intracellular ACh vesicle content. We applied this platform to differentiated human cholinergic SH-SY5Y neuroblastoma cells, an established yet underutilized cell model for cholinergic signaling. The nanotip sensor successfully captured amperometric spikes from both intracellular vesicle burst events and presynaptic ACh release. Intracellular events released a larger amount of ACh than presynaptic exocytosis events, indicating a predominance of partial exocytosis mode in these cells. These results demonstrate the nanotip ACh biosensor as a unique tool for probing fusion pore dynamics at subcellular resolution and for providing quantitative insight into the quantal nature of cholinergic signaling in human neuronal models.

乙酰胆碱（ACh）是认知功能、运动控制和突触调节的中枢神经递质，但它的电化学不活性和胞吐的快速动力学阻碍了实时量子测量。微米级的酶促ACh生物传感器以前可以进行亚毫秒级的细胞外记录，但对于突触定位和细胞内记录来说太大了。本文提出了一种短、超快、低噪声的基于针状碳纤维纳米电极的ACh生物传感器，该电极具有金纳米粒子和酶的功能。小型化的几何结构允许精确放置在神经突释放位点，并微创插入细胞质，从而实现突触前胞吐的高时间分辨率监测以及细胞内ACh囊泡含量的定量。我们将该平台应用于分化的人胆碱能SH-SY5Y神经母细胞瘤细胞，这是一种已建立但未充分利用的胆碱能信号传导细胞模型。纳米尖端传感器成功捕获了细胞内囊泡破裂事件和突触前乙酰胆碱释放的电流峰值。细胞内事件比突触前胞吐事件释放更多的乙酰胆碱，表明这些细胞以部分胞吐模式为主。这些结果表明，纳米尖端ACh生物传感器是一种独特的工具，可以在亚细胞分辨率下探测融合孔动力学，并为人类神经元模型中胆碱能信号的量子性质提供定量的见解。

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引用次数: 0

Electrochemistry of redox enzymes: from functional enzyme immobilization to enzymatic bio-electrochemical devices (tutorial) 氧化还原酶的电化学：从功能酶固定化到酶生物电化学装置（教程）

IF 4.5 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2026-10-01 Epub Date: 2026-03-04 DOI: 10.1016/j.bioelechem.2026.109265

A. Guessab, I. Mazurenko, E. Lojou, A. de Poulpiquet

Electrochemistry of redox enzymes is a multidisciplinary field, and students who join labs specialized in bio-electrochemistry have various backgrounds: chemistry, biology, biotechnologies, nanotechnologies, physics, etc., so that their level in the involved disciplines is often heterogeneous, and they sometimes lack the basic knowledge about either of the fields concerned by their project (physical chemistry, electrochemistry, enzymology, etc.). Projects that gather experienced researchers from these different areas also sometimes suffer from a lack of understanding between the partners. This tutorial, which follows a lecture given at the first winter school of the French group of bio-electrochemistry (GFB), aims at guiding newcomers in the field and provides advice for more in-depth and specialized literature. It seeks to provide a solid theoretical and experimental foundation. Redox enzymes and the basic methods of immobilization at the electrode are introduced. The mechanisms of direct and mediated electron transfers are explained. An important electrochemical method, cyclic voltammetry, is explained, and the article describes how to extract information about enzyme/electrode and catalytic reactions. Finally, the tutorial presents two enzymatic bio-electrochemical devices, enzymatic fuel cells and enzymatic biosensors, and provides a guide for their electrochemical characterization.

氧化还原酶的电化学是一个多学科领域，加入生物电化学实验室的学生有不同的背景：化学、生物学、生物技术、纳米技术、物理学等，因此他们在所涉及的学科中的水平往往是异质的，有时他们缺乏项目所涉及的任何一个领域（物理化学、电化学、酶学等）的基础知识。从这些不同领域聚集经验丰富的研究人员的项目有时也会因合作伙伴之间缺乏理解而受到影响。本教程是继法国生物电化学小组（GFB）第一届冬季学校的讲座之后编写的，旨在指导该领域的新手，并为更深入和专业的文献提供建议。它力求提供一个坚实的理论和实验基础。介绍了氧化还原酶及其电极固定化的基本方法。解释了直接和间接电子转移的机理。介绍了一种重要的电化学方法——循环伏安法，并介绍了如何提取酶/电极和催化反应的信息。最后，本教程介绍了两种酶生物电化学装置，酶燃料电池和酶生物传感器，并提供了它们的电化学表征指南。

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引用次数: 0

Proof-of-concept bioelectrochemical characterization of Mycolicibacterium smegmatis for diagnostic applications 耻垢分枝杆菌诊断应用的概念验证生物电化学表征

IF 4.5 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2026-10-01 Epub Date: 2026-03-09 DOI: 10.1016/j.bioelechem.2026.109277

Sunday Olakunle Oguntomi , Abhipsa Sahu , Yili Yang , Enrico Marsili

Elevated urease activity in tuberculosis-infected individuals is often suggestive of bacterial virulence by promoting survivability and establishment of the causative pathogen (Mycobacterium tuberculosis) in the host. Thus, heightened urease activity could be a promising biomarker for screening pathogenic mycobacterial strains. In this proof-of-concept study, we evaluate the suitability of electrochemical techniques for direct screening of mycobacterial strains based on urease activity. Mycolicibacterium smegmatis wildtype (WT), a derived knockout mutant of the LCP protein family (∆0107) with high urease activity, and its complement strain (c-0107) were coated in polydopamine (PDA) and immobilized on a screen-printed electrode (SPE) for microscopy and electrochemical characterization, in presence of exogenous redox mediators: potassium ferricyanide, anthraquinone, and riboflavin. Microscopy showed compatibility of PDA as a coating material for mycobacterial cells. Electrochemical analysis results indicated enhanced M. smegmatis electroactivity in the presence of anthraquinone, with higher current output in the strain with high urease activity. Experiments at different urea concentrations suggest that urea is not required for this screening approach. This work shows that electrochemical data can potentially distinguish mycobacterial strains based on urease activity. It also lays a groundwork in the model mycobacteria M. smegmatis, which could facilitate development of assays for pathogenic mycobacterial species.

结核菌感染个体的脲酶活性升高，通常通过促进宿主的生存能力和致病病原体（结核分枝杆菌）的建立，提示细菌的毒力。因此，提高脲酶活性可能是筛选致病性分枝杆菌菌株的一个有希望的生物标志物。在这项概念验证研究中，我们评估了基于脲酶活性的电化学技术直接筛选分枝杆菌菌株的适用性。在外源性氧化还原介质铁氰化钾、蒽醌和核黄素的存在下，将LCP蛋白家族（∆0107）的敲除突变体——耻毛分枝杆菌野生型（WT）及其补体菌株（c-0107）包被聚多巴胺（PDA），并固定在屏幕印刷电极（SPE）上进行显微镜和电化学表征。显微镜显示PDA作为分枝杆菌细胞包衣材料的相容性。电化学分析结果表明，蒽醌的存在增强了耻垢分枝杆菌的电活性，且菌株具有较高的脲酶活性。不同尿素浓度的实验表明，这种筛选方法不需要尿素。这项工作表明电化学数据可以根据脲酶活性潜在地区分分枝杆菌菌株。这也为建立耻垢分枝杆菌模型奠定了基础，为开发致病性分枝杆菌的检测方法奠定了基础。

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引用次数: 0

Optimization of a MWCNTs-AuNPs composite-modified electrochemical immunosensor with anti-fouling property for highly sensitive and rapid detection of BNP in myocardial infarction-induced heart failure diagnosis MWCNTs-AuNPs复合修饰抗污染电化学免疫传感器在心肌梗死性心力衰竭诊断中的高灵敏度和快速检测

IF 4.5 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Bioelectrochemistry

Pub Date : 2026-10-01 Epub Date: 2026-02-28 DOI: 10.1016/j.bioelechem.2026.109258

Jiaru Fu , Dewei Huang , Bolu Sun , Chengwen Li , Yuqiong Wu , Huajie Li , Jiali Kang , Haiying He , Xiangdong Wang , Yaru Zhang , Xuanxiu Da , Mian Chen , Lin Yang

Brain natriuretic peptide (BNP) is a sensitive biomarker for acute heart failure (AHF). Rapid, sensitive, and anti-fouling BNP detection in serum remains clinically unmet. Herein, a novel electrochemical immunosensor with synergistic signal amplification and anti-fouling ability was constructed via layered AuNPs/MWCNTs-AuNPs modification. Bottom AuNPs mitigate MWCNTs agglomeration and enable stable Anti-BNP immobilization via AuS bonds, MWCNTs enhance conductivity, and top AuNPs amplify signals, forming an efficient electron-transport network. A nitrocellulose (NC) membrane was laminated for anti-fouling via rapid contaminant sieving. Under optimization, the sensor shows a linear range of 7.81–8 × 10³ pg/mL for BNP, with a detection limit of 8.14 × 10⁻² pg/mL (3σ, n = 11), outperforming ELISA. It exhibits excellent selectivity (vs. cTn-I, glucose, IL-6), repeatability (RSD = 2.3%), and stability (92.4% retention over 30 days). Serum recovery rates of 102–105% confirm anti-fouling reliability. This cost-effective platform promises POCT for AHF and underpins anti-fouling biosensor development.

脑钠肽（BNP）是急性心力衰竭（AHF）的敏感生物标志物。快速、灵敏、抗污染的血清BNP检测仍未在临床上实现。本文通过层状AuNPs/MWCNTs-AuNPs修饰，构建了一种具有协同信号放大和防污能力的新型电化学免疫传感器。底部AuNPs可减轻MWCNTs团聚并通过AuS键实现稳定的Anti-BNP固定化，MWCNTs可增强电导率，顶部AuNPs可放大信号，形成高效的电子传递网络。采用快速过滤的方法制备了一种硝基纤维素（NC）防污膜。优化后，该传感器对BNP的检测线性范围为7.81 ~ 8 × 103 pg/mL，检出限为8.14 × 10-2 pg/mL (3σ, n = 11)，优于ELISA。它具有优良的选择性（相对于ctn - 1、葡萄糖、IL-6）、重复性（RSD = 2.3%）和稳定性（30天内保留率为92.4%）。102-105%的血清回收率证实了抗污染的可靠性。这个具有成本效益的平台为AHF提供了POCT，并支持了防污生物传感器的开发。

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引用次数: 0

Ultrafast optical nonlinearities and refraction enhanced optical limiting performance of azonaphthalene dyes 超快光学非线性和折射增强了偶氮萘染料的光学极限性能

IF 4.7 3区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Photochemistry and Photobiology A-chemistry

Pub Date : 2026-09-01 Epub Date: 2026-03-06 DOI: 10.1016/j.jphotochem.2026.117157

Deshun Li , Xuanming Liang , Xingzhi Wu , Honglin Shang , Jie Zhang , Yu Fang , Yongqiang Chen , Fei Wang , Quanying Wu , Yinglin Song

Azo molecules represent a pivotal class of near-infrared dyes with extensive applications in energy storage/conversion and smart materials. While their nonlinear absorption (NLA) effects have garnered significant attention, the optical limiting (OL) mechanisms and performance of these molecules remain underexplored. This study investigates the near-infrared broadband nonlinear absorption and OL mechanisms of two azo derivatives (AZON-1 and AZON-2) using Z-scan measurement (620–900 nm) and transient absorption spectroscopy. The impact of molecular planarity differences on nonlinear optical responses is analyzed. Ultrafast dynamics are elucidated through transient absorption measurements. These measurements uncover photophysical mechanisms. Notably, AZON-2 exhibits intensity-dependent transitions from saturation absorption (SA) to reverse saturation absorption (RSA) at 620 nm, attributed to the interplay between SA and excited-state absorption (ESA). Both samples demonstrate robust NLA across 620–900 nm, primarily originating from ESA and two-photon absorption (TPA). The nonlinear responses under 650 nm laser irradiation in OL experiment are simulated. These results are validated via Z-scan techniques and correlated with DFT-derived molecular structure-property relationships. AZON-1 exhibits a low OL threshold of 11 mJ/cm² at 650 nm with an effective NLA coefficient of 2 × 10⁻¹³ m/W, basically consistent with the Z-scan results. For AZON-2, a synergistic SA-RSA fitting model reveals that cooperative SA-RSA effects enhance OL response speed. This work advances the understanding of nonlinear optical properties in azo derivatives, enriching experimental paradigms and providing design guidelines for organic materials with superior nonlinear optical performance.

偶氮分子是一类关键的近红外染料，在能量存储/转换和智能材料中有着广泛的应用。虽然它们的非线性吸收（NLA）效应引起了极大的关注，但这些分子的光学限制（OL）机制和性能仍未得到充分的研究。本文利用z扫描测量（620 ~ 900 nm）和瞬态吸收光谱研究了两种偶氮衍生物（AZON-1和AZON-2）的近红外宽带非线性吸收和OL机制。分析了分子平面度差异对非线性光学响应的影响。通过瞬态吸收测量阐明了超快动力学。这些测量揭示了光物理机制。值得注意的是，AZON-2在620 nm处表现出从饱和吸收（SA）到反向饱和吸收（RSA）的强度依赖转变，这归因于SA和激发态吸收（ESA）之间的相互作用。两个样品在620-900 nm范围内都表现出强大的NLA，主要来自欧空局和双光子吸收（TPA）。模拟了650 nm激光辐照下OL实验的非线性响应。这些结果通过z扫描技术得到验证，并与dft衍生的分子结构-性质关系相关联。AZON-1在650 nm处表现出11 mJ/cm2的低OL阈值，有效NLA系数为2 × 10−13 m/W，与z扫描结果基本一致。对于AZON-2，协同SA-RSA拟合模型表明，协同SA-RSA效应提高了OL响应速度。这项工作促进了对偶氮衍生物非线性光学性质的理解，丰富了实验范式，并为具有优异非线性光学性能的有机材料的设计提供了指导。

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引用次数: 0

Theoretical investigation of crystal structure transformation regulating differential luminescence: The dominant role of the S1-T2 pathway 晶体结构转变调控差分发光的理论研究：S1-T2通路的主导作用

IF 4.7 3区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Photochemistry and Photobiology A-chemistry

Pub Date : 2026-09-01 Epub Date: 2026-02-27 DOI: 10.1016/j.jphotochem.2026.117152

Shao-Wen Luo, Yue Ren , Ming-Yang Li

Thermally activated delayed fluorescence (TADF) and organic room temperature phosphorescence (RTP) are triplet-involved emission process governed by the competition between intersystem crossing (ISC) and reverse intersystem crossing (RISC). However, the selective regulation of this competition by molecular packing motifs remains poorly understood. Here, a multiscale theoretical study is conducted on two polymorphs (GY and OR) of TPA-CHO to elucidate the mechanism underlying TADF-RTP conversion. Our results demonstrate that the S₁-T₂ pathway, rather than the conventional S₁-T₁ channel, plays a decisive role in the excited-state population transfer across different aggregation conditions. The GY crystal favors TADF due to the reduced S₁-T₂ energy gap and low activation energy, enabling efficient RISC, while the OR crystal exhibits RTP behavior driven by enhanced spin-orbit coupling that accelerates ISC. Distinct intermolecular interactions in the two crystal phases further suppress non-radiative decay. This work establishes a clear crystal-regulated photophysical mechanism and provides theoretical insight into the rational control of TADF and RTP emission.

热激活延迟荧光（TADF）和有机室温磷光（RTP）是受系统间交叉（ISC）和反向系统间交叉（RISC）竞争支配的三重参与发射过程。然而，分子包装基序对这种竞争的选择性调节仍然知之甚少。本文对TPA-CHO的两种多晶型（GY和OR）进行了多尺度理论研究，以阐明TADF-RTP转化的机制。我们的研究结果表明，在不同聚集条件下激发态种群转移中起决定性作用的是S1-T2途径，而不是传统的S1-T1通道。GY晶体由于减小了S1-T2的能隙和较低的活化能而有利于TADF，从而实现了高效的RISC，而OR晶体由于增强的自旋-轨道耦合而表现出RTP行为，从而加速了ISC。两个晶体相中不同的分子间相互作用进一步抑制了非辐射衰变。本工作建立了清晰的晶体调控光物理机制，为TADF和RTP发射的合理控制提供了理论见解。

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引用次数: 0

Visible-light-driven synthesis of DNA-templated gold nanoparticles in biocompatible PEGDA-chitosan nanocomposites 生物相容性聚乙二醇-壳聚糖纳米复合材料中dna模板金纳米颗粒的可见光合成

IF 4.7 3区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Photochemistry and Photobiology A-chemistry

Pub Date : 2026-09-01 Epub Date: 2026-03-03 DOI: 10.1016/j.jphotochem.2026.117160

Elaf Algrairy , Lotfi Beji , Haja Tar , Noura Kouki , Abrar S. Alnafisah , Fahad M. Alminderej , Lotfi M. Aroua

A novel, rapid, and eco-friendly photochemical method is presented for the synthesis of gold nanoparticles (AuNPs) and their direct integration into a biocompatible polymer matrix. The technique utilizes a visible-light-absorbing benzophenone derivative(BP-d) as a photoinitiator, triethylamine (TEA) as a co-initiator, and calf thymus DNA (ct-DNA) as a multifunctional template that prevents aggregation, facilitates electron transfer, and provides a scaffold for controlled nucleation. The photochemical mechanism was first tested in an aqueous system, where kinetic analysis revealed that ct-DNA significantly enhances reaction efficiency, enabling the formation of stable AuNPs within 40 s under visible-light irradiation (λ_irr = 419 nm). The optimized BP-d/TEA/ct-DNA system was then employed to initiate photopolymerization within a polyethylene glycol diacrylate (PEGDA)–chitosan matrix, yielding a cross-linked, polymer-confined nanocomposite via a one-pot process. Transmission electron microscopy (TEM) showed quasi-spherical AuNPs with a narrow size distribution (average diameter ≈ 5.9 nm) evenly dispersed within the polymer network. At the same time, Fourier-transform infrared (FTIR) spectroscopy confirmed the formation of a cohesive matrix stabilized by steric and electrostatic interactions. By integrating visible-light photochemistry with biomolecular templating and polymer confinement, this work provides a scalable and sustainable platform for the precise production of Au–polymer nanocomposites. Evaluation of catalytic activity and biological performance is outside the scope of this study and will be addressed in future research.

提出了一种新型、快速、环保的光化学方法，用于合成金纳米颗粒（AuNPs）并将其直接整合到生物相容性聚合物基质中。该技术利用吸收可见光的二苯甲酮衍生物（BP-d）作为光引发剂，三乙胺（TEA）作为共引发剂，小牛胸腺DNA （ct-DNA）作为多功能模板，防止聚集，促进电子转移，并为受控成核提供支架。首先在水体系中测试了光化学机理，动力学分析表明，ct-DNA显著提高了反应效率，在可见光照射（λirr = 419 nm）下，40 s内形成稳定的AuNPs。然后利用优化后的BP-d/TEA/ct-DNA体系在聚乙二醇二丙烯酸酯(PEGDA) -壳聚糖基质中引发光聚合，通过一锅工艺得到交联的聚合物约束纳米复合材料。透射电镜（TEM）显示，AuNPs呈准球形，尺寸分布窄（平均直径≈5.9 nm），均匀分布在聚合物网络中。同时，傅里叶变换红外光谱（FTIR）证实形成了一个由空间和静电相互作用稳定的内聚矩阵。通过将可见光光化学与生物分子模板和聚合物约束相结合，这项工作为精确生产金聚合物纳米复合材料提供了一个可扩展和可持续的平台。催化活性和生物性能的评价超出了本研究的范围，将在未来的研究中加以解决。

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