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ANALYTICAL CHEMISTRY · 2022 · IF 8.008

Spatiotemporal-Resolved Hyperspectral Raman Imaging of Plasmon-Assisted Reactions at Single Hotspots

Xueqin Chen,Yan Gao,Jiayin Zhan,Qing Xia,Zixuan Chen,Jun-Jie Zhu

Raman spectroscopy facilitates the study of reacting molecules on single nanomaterials. In recent years, the temporal resolution of Raman spectral measurement has been remarkably reduced to the millisecond level. However, the classic scan-based imaging mode limits the application in the dynamical study of reactions at multiple nanostructures. In this paper, we propose a spatiotemporal-resolved Raman spectroscopy (STRS) technology to achieve fast (∼40 ms) and high spatial resolution (∼300 nm) hyperspectral Raman imaging of single nanostructures. With benefits of the outstanding electromagnetic field enhancement factor by surface plasmon resonance (∼1012) and the snapshot hyperspectral imaging strategy, we demonstrate the observation of stepwise Raman signals from single-particle plasmon-assisted reactions. Results reveal that the reaction kinetics is strongly affected by not only the surface plasmon-polariton generation but also the density of Raman molecules. In consideration of the spatiotemporal resolving capability of STRS, we anticipate that it provides a potential platform for further extending the application of Raman spectroscopy methods in the dynamic study of 1D or 2D nanostructures.

研究领域: 纳米科学 · 光谱学 · 化学动力学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

In-situ imaging and time-resolved investigation of local pH in electrocatalytic CO2 reduction

Zezhong Xie,Qiushi Wang,Rongge Yang,Jingnan Zhang,Shanqiang Ou,Gangfeng Ouyang,Mingyang Li,Jianxin Shi,Yexiang Tong

Local pH near the catalyst surface exerts a substantial influence on both catalytic selectivity and activity in electrocatalytic CO 2 reduction (CO 2 RR). While the investigation of local pH remains challenging in the aspect of in-situ imaging and monitoring. In this study, a novel lateral-type surface-enhanced Raman spectroscopy (L-SERS) system with a wide pH testing range from acidic to alkaline, is developed for the in-situ observation of local pH distributions with high spatial and temporal resolution during CO 2 RR. Excellent in-situ imaging of local pH near the catalyst surface is obtained, showing good consistency with simulation results. Besides, the gradual pH elevation and stabilization can be monitored via this time-resolved local pH investigation. This study presents a direct visualization of local pH distribution and variation at the Nernst layer during CO 2 RR, providing direct evidence in local pH for the feasibility of acidic electrolyte and offering theoretical guidance for optimizing CO 2 RR conditions.

研究领域: 化学 · 材料科学 · 电化学
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

High Spatiotemporal Resolution Biomimetic Thermoreceptors Realizing by Jointless p-n Integration Thermoelectric Composites

Chengzhi Chen,Zijian Liu,Liangchao Guo,Bingchen Huo,Qi Sun,Lirong Liang,Chunyu Du,Guangming Chen

Human body temperature is a critical physiological indicator, reflecting metabolism and temperature regulation. Biomimetic temperature sensors with high temporal and spatial resolution are highly desired to emulate human skin's temperature perception capabilities. Here, a selective filtration method is proposed to fabricate a jointless p-n thermoelectric module, integrating p-type and n-type materials with minimal interfacial barriers. The structure enables rapid response, minimal signal variation, and a robust linear relationship between open circuit voltage and temperature difference, making it suitable as a biomimetic thermoreceptor for enhancing humanoid robots with intelligent sensing capabilities. A smart thermoelectric sensing system with a high temporal and spatial resolution is developed using with jointless p-n module as the sensing element. In temporal thermal sensing, the sensing system can timely and effectively identify the heat source, with a fast response time of <0.1 s. In addition, in spatial thermal sensing, the system reliably detects thermal stimuli within discrete regions of each measuring area of <1 × 1 cm 2 . This study provides an effective strategy for temperature sensors in thermoelectric sensing and biomimetic thermoreceptor applications.

CAS / MDL: 64-17-5
研究领域: 材料科学 · 生物医学工程 · 机器人学
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Cell Metabolism · 2022 · IF 31.373

Ultrasensitive sensors reveal the spatiotemporal landscape of lactate metabolism in physiology and disease

Xie Li,Yinan Zhang,Lingyan Xu,Aoxue Wang,Yejun Zou,Ting Li,Li Huang,Weicai Chen,Shuning Liu,Kun Jiang,Xiuze Zhang,Dongmei Wang,Lijuan Zhang,Zhuo Zhang,Zeyi Zhang,Xianjun Chen,Wei Jia,Aihua Zhao,Xinfeng Yan,Haimeng Zhou,Linyong Zhu,Xinran Ma,Zhenyu Ju,Weiping Jia,Congrong Wang,Joseph Loscalzo,Yi Yang,Yuzheng Zhao

Summary Despite its central importance in cellular metabolism, many details remain to be determined regarding subcellular lactate metabolism and its regulation in physiology and disease, as there is sensitive spatiotemporal resolution of lactate distribution, and dynamics remains a technical challenge. Here, we develop and characterize an ultrasensitive, highly responsive, ratiometric lactate sensor, named FiLa, enabling the monitoring of subtle lactate fluctuations in living cells and animals. Utilizing FiLa, we demonstrate that lactate is highly enriched in mammalian mitochondria and compile an atlas of subcellular lactate metabolism that reveals lactate as a key hub sensing various metabolic activities. In addition, FiLa sensors also enable direct imaging of elevated lactate levels in diabetic mice and facilitate the establishment of a simple, rapid, and sensitive lactate assay for point-of-care clinical screening. Thus, FiLa sensors provide powerful, broadly applicable tools for defining the spatiotemporal landscape of lactate metabolism in health and disease.

研究领域: 细胞生物学 · 代谢 · 生物医学工程 · 疾病模型
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Nature Communications · 2017 ·Vol. 8 ·期 1 ·1-10 · IF 12.124

Imaging the transient heat generation of individual nanostructures with a mechanoresponsive polymer

Chen Xueqin,Xia Qing,Cao Yue,Min Qianhao,Zhang Jianrong,Chen Zixuan,Chen Hong-Yuan,Zhu Jun-Jie

Measuring the localized transient heat generation is critical for developing applications of nanomaterials in areas of photothermal therapy (PTT), drug delivery, optomechanics and biological processes engineering. However, accurate thermometry with high spatiotemporal resolution is still a challenge. Here we develop a thermosensitive polymer-capped gold nanorod (AuNRs@pNIPAAm), which has temperature-dependent local surface plasmon resonance spectra due to the submolecular conformational change of pNIPAAm molecules. We measure the conformational dynamics on individual gold nanorods at the milliseconds level by the developed spatiotemporal resolution plasmonic spectroscopy (SRPS) and find that it has a fast (<4 ms), linear and reversible mechanoresponse to temperature changes as small as 80 mK. The rapid and highly sensitive thermosensitive AuNRs@pNIPAAm opens a new way to achieve spatiotemporal thermometry for potential applications in PTT and other biological research.

CAS / MDL: 109-99-9 64-17-5 67-64-1
研究领域: 纳米技术 · 生物医学工程 · 材料科学 · 光学
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-10 · IF 15.7

Disentangling extracellular current of electroactive bacteria with oblique-incidence reflection difference imaging

Qian Shiwu,Wang Chenyu,Fang Changxiang,Li Meng,Qiao Yan,Hu Weihua

Understanding the extracellular electron transfer (EET) process of electroactive bacteria is of great significance. It is critical yet challenging to differentiate the partial currents from direct (DET) and mediated electron transfer (MET) pathways in the integrated EET current. Herein the EET current of model exoelectrogen is successfully disentangled by using spatiotemporally-resolved oblique-incidence reflection difference (OIRD) technique coupled with polyaniline (PANI)-based dual electrode. The PANI film serves as an electron acceptor to translate the charge information into OIRD signals, enabling mapping of EET current. Upon complete reduction of PANI, the local EET current is switched off, and the soluble mediators are forced to discharge on the nearby PANI electrode, enabling measuring of MET current. In such a way, the DET and MET currents are measured and the average currents from each bacterium are quantified. As-reported method enables successful disentangling the EET current and may offer valuable insights to related research.

CAS / MDL: 62-53-3
研究领域: 微生物电化学 · 生物电化学 · 纳米技术 · 电分析化学
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Microsystems & Nanoengineering · 2024 ·Vol. 10 ·期 1 ·1-11 · IF 7.3

MRI and CT compatible asymmetric bilayer hydrogel electrodes for EEG-based brain activity monitoring

Ren Guoqiang,Zhang Mingxuan,Zhuang Liping,Li Lianhui,Zhao Shunying,Guo Jinxiu,Zhao Yinchao,Peng Zhaoxiang,Lian Jiangfan,Liu Botao,Ma Jingyun,Hu Xiaodong,Zhang Zhewei,Zhang Ting,Lu Qifeng,Hao Mingming

The exploration of multi-dimensional brain activity with high temporal and spatial resolution is of great significance in the diagnosis of neurological disease and the study of brain science. Although the integration of electroencephalogram (EEG) with magnetic resonance imaging (MRI) and computed tomography (CT) provides a potential solution to achieve a brain-functional image with high spatiotemporal resolution, the critical issues of interface stability and magnetic compatibility remain challenging. Therefore, in this research, we proposed a conductive hydrogel EEG electrode with an asymmetrical bilayer structure, which shows the potential to overcome the challenges. Benefiting from the bilayer structure with different moduli, the hydrogel electrode exhibits high biological and mechanical compatibility with the heterogeneous brain-electrode interface. As a result, the impedance can be reduced compared with conventional metal electrodes. In addition, the hydrogel-based ionic conductive electrodes, which are free from metal conductors, are compatible with MRI and CT. Therefore, they can obtain high spatiotemporal resolution multi-dimensional brain information in clinical settings. The research outcome provides a new approach for establishing a platform for early diagnosis of brain diseases and the study of brain science.

研究领域: 神经科学 · 医学成像 · 生物医学工程 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

A multisensory-feedback tactile glove with dense coverage of sensing arrays for object recognition

Ye Qiu,Zhiqiang Wang,Pengcheng Zhu,Binbin Su,Chang Wei,Ye Tian,Zheng Zhang,Hao Chai,Aiping Liu,Lihua Liang,Huaping Wu

Somatosensory networks that provide sophisticated sensory feedback and enable the dexterous manipulation of the human grasp remain difficult to replicate in robots, which is attributed to the grand challenge of densely covering the hand with tactile arrays. Here, a multisensory tactile glove is reported that is capable of object recognition with dense coverage of pressure and temperature sensing arrays. The synergistic effect of the multimodal configuration allows the tactile arrays to perceive contact pressure and thermal conductivity of an object involved in grasping motion, thus enhancing the accuracy via the combination of the mechanical features with thermal properties. By leveraging the multiple scanning technology and wireless transmission system, the tactile glove achieves a recognition accuracy of 94.2% in differentiating 20 types of objects with a modified deep learning algorithm. The large-area sensing arrays with high spatiotemporal resolution and multimodal sensing capabilities, which paves the way for the development of robot grasping tools, human–machine interfacing, and advanced prosthetics.

研究领域: 机器人学 · 人机交互 · 可穿戴传感器 · 假肢技术 · 人工智能
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Nanoscale · 2019 ·Vol. 11 ·期 22 ·10702-10708 · IF 6.97

A single nanowire sensor for intracellular glucose detection

Quan-Lan Liao,Hong Jiang,Xin-Wei Zhang,Quan-Fa Qiu,Yun Tang,Xiao-Ke Yang,Yan-Ling Liu,Wei-Hua Huang

Glucose metabolism plays an important role in cell energy supply, and quantitative detection of the intracellular glucose level is particularly important for understanding many physiological processes. Glucose electrochemical sensors are widely used for blood and extracellular glucose detection. However, intracellular glucose detection cannot be achieved by these sensors owing to their large size and consequent low spatial resolution. Herein, we developed a single nanowire glucose sensor for electrochemical detection of intracellular glucose by depositing Pt nanoparticles (Pt NPs) on a SiC@C nanowire and further immobilizing glucose oxidase (GOD) thereon. Glucose was converted by GOD to an electroactive product H2O2 which was further electro-catalyzed by Pt NPs. The glucose nanowire sensor is endowed with a high sensitivity, high spatial-temporal resolution and enzyme specificity due to its nanoscale size and enzymatic reaction. This allows the real-time monitoring of the intracellular glucose level, and the increase of the intracellular glucose level induced by a novel potential hypoglycemic agent, reinforcing its potential application in lowering the blood glucose level. This work provides a versatile method for the construction of enzyme-modified nanosensors to electrochemically detect intracellular non-electroactive molecules, which is of great benefit for physiological and pathological studies.

研究领域: 生物化学 · 纳米技术 · 电化学 · 细胞生物学
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ACS Nano · 2022 · IF 18.027

Self-illuminating NIR-II bioluminescence imaging probe based on silver sulfide quantum dots

Mohammad Javad Afshari,Cang Li,Jianfeng Zeng,Jiabin Cui,Shuwang Wu,Mingyuan Gao

Bioluminescence (BL) imaging has emerged to tackle the potential challenges of fluorescence (FL) imaging including the autofluorescence background, inhomogeneous illumination over a wide imaging field, and the light-induced overheating effect. Taking advantage of the bioluminescence resonance energy transfer (BRET) mechanism between a conventional luciferin compound and a suitable acceptor, the visible light of the former can be extended to photons with longer wavelengths emitting from the latter. Although BRET-based self-illuminating imaging probes have already been prepared, employing potentially cytotoxic elements as the acceptor with the emission wavelengths which hardly reach the first near-infrared (NIR-I) window, has limited their applications as safe and high performance in vivo imaging agents. Herein, we report a biocompatible, self-illuminating, and second near-infrared (NIR-II) emissive probe to address the cytotoxicity concerns as well as improve the penetration depth and spatiotemporal resolution of BL imaging. To this end, NanoLuc luciferase enzyme molecules were immobilized on the surface of silver sulfide quantum dots to oxidize its luciferin substrate and initiate a single-step BRET mechanism, resulting in NIR-II photons from the quantum dots. The resulting dual modality (BL/FL) probes were successfully applied to in vivo tumor imaging in mice, demonstrating that NIR-II BL signals could be easily detected from the tumor sites, giving rise to ∼2 times higher signal-to-noise ratios compared to those obtained under FL mode. The results indicated that nontoxic NIR-II emitting nanocrystals deserve more attention to be tailored to fill the growing demands of preparing appropriate agents for high quality BL imaging.

研究领域: 生物医学工程 · 分子生物学 · 纳米技术 · 成像科学 · 癌症研究
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MICROCHEMICAL JOURNAL · 2024 · IF 4.9

A novel electrochemical microneedle sensor for highly sensitive real time monitoring of glucose

Tao Ming,Tingting Lan,Mingxing Yu,Xu Duan,Shuhan Cheng,Hong Wang,Juan Deng,Deling Kong,Shuang Yang,Zhongyang Shen

Glucose is one of the most significant biomarkers due to its association with numerous diseases related to blood glucose concentration. In this study, a novel electrochemical microneedle sensor (EMS) for highly sensitive, high spatiotemporal resolution, real time glucose monitoring is developed. Initially, the sensor is modified by electrochemically depositing gold nanoparticles to enhance its conductivity. Subsequently, a platinum sensing layer is deposited onto the sensor to realize the detection of hydrogen peroxide. Glucose oxidase (GOx) is then immobilized onto the sensor by immersing it in an O-phenylenediamine solution and electro-polymerizing O-phenylenediamine. A polyurethane-based biological protective film is applied to protect the electrode from interference by large proteins and cell deposition in body fluid. The prepared EMS demonstrates excellent selectivity for glucose detection (0.818 μA/mM) over a broad range (0 to 20 mM). Furthermore, clinical serum glucose testing experiments verified the sensor’s performance, showcasing its potential for biomedical research and clinical practice. This EMS offers a less invasive and more convenient method for highly sensitive, high spatiotemporal resolution, real time glucose monitoring. Moreover, this electrochemical implantable sensor provides a minimally invasive and convenient solution for continuous monitoring of other biomarkers.

CAS / MDL: 64-17-5 7447-40-7
研究领域: 生物医学工程 · 分析化学 · 传感器与执行器 · 医疗器械 · 糖尿病管理
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