目录 | 《电化学》2023年第6期（界面设计与电化学传感专辑）文章速览

专辑介绍：《电化学》期刊2023年出版《界面设计与电化学传感专辑》，由清华大学李景虹院士、华东师范大学田阳教授、青岛大学许元红教授、华东师范大学张立敏教授共同担任客座编辑。

封面：金属有机框架作为一类新型的多孔晶体材料，由于具有比表面积大、化学稳定性好、结构可调节等优点，在电化学和电化学发光免疫分析中得到了广泛应用。（文献号 2218003）

本期为全英文，收录6篇界面设计与电化学传感方向的综述和研究论文。扫描或识别二维码，免费查看、下载文献的PDF全文。

李景虹, 田阳, 许元红, 张立敏. “界面设计与电化学传感”专辑序言[J]. 电化学, 2023, 29(6): 2218000.

DOI: 10.13208/j.electrochem.2218000

作者聚焦

Author Spotlight

DOI: 10.13208/j.electrochem.2218111

覃晓丽, 詹子颖, Sara Jahanghiri, Kenneth Chu, 张丛洋, 丁志峰. 金属有机框架材料在电化学/电化学发光免疫分析中的应用[J]. 电化学, 2023, 29(6): 2218003.

Xiao-Li Qin, Zi-Ying Zhan, Sara Jahanghiri, Kenneth Chu, Cong-Yang Zhang, Zhi-Feng Ding. Metal-Organic Frameworks for Electrochemical and Electrochemiluminescent Immunoassay[J]. Journal of Electrochemistry, 2023, 29(6): 2218003.

DOI: 10.13208/j.electrochem.2218003

Development of ultrasensitive, highly accurate and selective immunosensors is significant for the early diagnosis, screening, and monitoring of diseases. Electrochemical and electrochemiluminescent (ECL) immunoassays have both attracted great attention and become a current research hotspot due to their advantages such as good stability, high sensitivity and selectivity, wide linear range, and good controllability. Metal-organic frameworks (MOFs), as a new class of porous crystalline materials, have been widely applied in electrochemical and ECL immunosensors owing to their large specific surface area, good chemical stability, as well as adjustable pore size and nanoscale framework structures. Various MOF nanomaterials with different properties for the development of high-performance electrochemical and ECL immunosensors can be achieved, because they can be applied as sensitive platforms for immobilizing biological recognition molecules, enriching the trace analytes and signal molecules, amplifying the signal and enhancing the sensitivity of the electrochemical or ECL immunoassays. This review summarizes various types of MOFs-based immunosensors and their assays application, in which MOFs act as electrode matrices, signal probes (either as electroactive labels or as emitter labels), carriers or catalytic labels for sensitive electrochemical and ECL detections. Moreover, challenges and future opportunities for the development of the functionalized MOFs are discussed to provide a guidance on the design and fabrication of high-performance MOFs-based immunosensors in the future.

静超, 龙亿涛. 暗场显微镜下的彩色“纳米星”[J]. 电化学, 2023, 29(6): 2218006.

Chao Jing, Yi-Tao Long. Colorful “Stars” in the Dark[J]. Journal of Electrochemistry, 2023, 29(6): 2218006.

DOI: 10.13208/j.electrochem.2218006

Plasmonic nanoparticles such as Au and Ag with localized surface plasmon resonance (LSPR) property exhibit unique scattering and absorption features. The plasmonic scattering and absorption bands are mainly located at visible light region which can be easily applied in visual detections. By modulating the size, shape and composition of gold and silver colloid solutions, plenty of colorimetric methods have been designed for the detection of metal ions, biomolecules and environmental contaminants. For many years, the LSPR-based measurements are implemented in reagent tubes. Since 2000, the plasmon resonance scattering (PRS) light of metal nanoparticles captured by dark-field microscopy enables the investigation at the nanoscale dimension. Mono-dispersed nanoparticles under a dark-field microscope showed distinct scattering light spots, like colorful stars in the dark sky. The PRS light of a single nanoparticle opens a new way for ultra-sensitive sensing which eliminates the average effects in bulk and provides more accurate reaction information. Thus, individual nanoparticles with specific scattering colors are excellent nanoprobes in the applications of biology, physics, and chemistry. In this review, the plasmonics based colorimetric nanosensors are presented. Particularly, the application of in-situ PRS in the dynamically monitoring of electrocatalytic reactions is highlighted. We firstly introduce a short history of the discovery and development of plasmonic nanoparticles from the ancient artwork to the modern characterization techniques. Some factors including morphology, and dielectric constants that are correlated to the LSPR bands and scattering light colors are listed. Secondly, we demonstrate the use of single plasmonic nanoparticles as visualized color-coded nanoprobes. As the morphology of particles has strong effect on the PRS light, elegant sensors have been conceived by the etching and growth of nanoparticles with different sizes and shapes. On the other hand, the real-time monitoring of particle structure evolution could also reveal the mechanism of the material fabrication at the nanoscale. In addition, core-satellite nanostructures with various linkers are proposed as ultra-sensitive sensors according to the inter-particle coupling effect. Subsequently, we summarize several advanced techniques for nanoscale signal extraction and amplifications. For instance, to expand the application of colorimetric nanosensors, converting the colors into RGB values could clearly distinguish the subtle color changes. Combining with high-throughput signal processing method, thousands of nanoparticles can be rapidly analyzed, which can greatly enhance the measurement efficiency. Except the PRS color, the PRS intensity could also provide abundant information and is easier to be captured. A facile method by converting the PRS intensity of single nanoparticles into visible colors is presented, which is mighty suitable for the in-situ monitoring of fast electrochemical process with high time resolution.

陈涛, 许元红, 李景虹. 基于电化学阻抗谱的致病菌检测传感器的研究进展[J]. 电化学, 2023, 29(6): 2218002.

Tao Chen, Yuan-Hong Xu, Jing-Hong Li. Recent Advances in Electrochemical Impedance Spectroscopy-Based Pathogenic Bacteria Sensing[J]. Journal of Electrochemistry, 2023, 29(6): 2218002.

DOI: 10.13208/j.electrochem.2218002

Pathogenic bacteria have been throwing great threat on human health for thousands of years. Their real-time monitoring is in urgent need as it could effectively halt the spread of pathogenic bacteria and thus reducing the risk to human health. Up till now, diverse technologies such as electrochemistry, optics, piezoelectricity and calorimetry have been developed for bacteria sensing. Therein, electrochemical impedance spectroscopy (EIS)-based sensors show great potential in point-of-care bacterial analysis because of their low-cost, short read-out time, good reproducibility, and portable equipment construction. In this review, we will primarily summarize the typical applications of electrochemical impedance technology in bacteria sensing based on different electrodes in the last three years. As we know, the electrode materials play an extremely important role in the construction of EIS-based sensors because not only the immobilization of bio-recognition elements for bacteria, but also the sensitivity, economical efficiency and portability of the as-prepared sensors are mainly determined by the electrode materials. Therefore, in order to provide new researchers a clear preparation process for EIS-based sensors fabricated with different electrodes, we try to classify the EIS-based sensors according to the different electrode platforms. Moreover, present difficulties, future directions and perspectives for their applications are also discussed. It can provide guidance in future study of novel EIS-based sensors for rapid, sensitive and accurate sensing of diverse pathogenic bacteria.

刘原东, 李佳润, 张立敏, 田阳. 基于线性范围可调的适配体功能化微电极的鼠脑中钾离子的活体分析[J]. 电化学, 2023, 29(6): 2218004.

Yuan-Dong Liu, Jia-Run Li, Li-Min Zhang, Yang Tian. An Aptamer-Based Microelectrode with Tunable Linear Range for Monitoring of K⁺ in the Living Mouse Brain[J]. Journal of Electrochemistry, 2023, 29(6): 2218004.

DOI: 10.13208/j.electrochem.2218004

Potassium ion (K⁺) is widely involved in several physiopathological processes, and its abnormal changes are closely related to the occurrence of brain diseases of cerebral ischemia. In vivo acquirement of K⁺ variation is significant to understand the roles of K⁺ playing in brain functions. A microelectrode based on single-stranded DNA aptamers was developed for highly selective detection of K⁺ in brain, in which the aptamer probes were designed to contain an aptamer part for specific recognition of K⁺, an alkynyl group used for stable confinement of aptamer probe on the gold surface, and an electrochemical redox active ferrocene group to generate current response signal. The response range of the microelectrodes could be rationally tuned by varying the chain length of the aptamer probe. The optimized electrode, LAC, displayed high selectivity for in vivo detection of K⁺, and suitable linear range from 10 μmol·L^-1-10 mmol·L^-1, which could fulfill the requirement of K⁺ detection in brain. Eventually, the microelectrodes were successfully applied for the detection of K⁺ in the living mouse brains followed by hypoxic.

胡琼, 李诗琪, 梁伊依, 冯文星, 骆怡琳, 曹晓静, 牛利. 基于硼酸盐亲和辅助电化学调控ATRP的癌胚抗原超灵敏电化学适体传感研究[J]. 电化学, 2023, 29(6): 2218001.

Qiong Hu, Shi-Qi Li, Yi-Yi Liang, Wen-Xing Feng, Yi-Lin Luo, Xiao-Jing Cao, Li Niu. Boronate Affinity-Assisted Electrochemically Controlled ATRP for Ultrasensitive Electrochemical Aptasensing of Carcinoembryonic Antigen[J]. Journal of Electrochemistry, 2023, 29(6): 2218001.

DOI: 10.13208/j.electrochem.2218001

As an acidic glycoprotein, carcinoembryonic antigen (CEA) is of great value as a broad-spectrum tumor marker in the differential diagnosis and surveillance of malignant tumors. In this work, we report an electrochemical aptasensor for the ultrasensitive and highly selective detection of CEA, taking advantage of the dual amplification by the boronate affinity-assisted electrochemically controlled atom transfer radical polymerization (BA-eATRP). Specifically, the BA-eATRP-based electrochemical aptasensing of CEA involves the capture of target antigens by nucleic acid aptamers, the covalent crosslinking of ATRP initiators to CEA antigens via the selective interactions between the phenylboronic acid (PBA) group and the cis-diol group of the monosaccharide residues, and the collection of the ferrocene (Fc) reporters via the eATRP of ferrocenylmethyl methacrylate (FcMMA). As CEA is decorated with hundreds of cis-diol groups, the BA-based crosslinking can result in the labeling of each CEA with hundreds of ATRP initiators; furthermore, the eATRP of FcMMA results in the surface-initiated growth of long-chain ferrocenyl polymers, leading to the tethering of each ATRP initiator-conjugated site with hundreds to thousands of Fc reporters. Such that, the BA-eATRP can result in the efficient labeling of each CEA with a plenty of Fc reporters. Under the optimized conditions, the BA-eATRP-based strategy enables the highly selective aptasensing of CEA at a concentration as low as 0.34 pg·mL^-1, with a linear range of 1.0-1,000 pg·mL^-1. Besides, this aptasensor has been successfully applied to the quantitative analysis of CEA in human serum. The BA-eATRP-based electrochemical aptasensor is cost-effective and simple in operation, holding broad application prospect in the ultrasensitive and highly selective detection of CEA.

张生雅, 姚敏, 王泽, 刘天娇, 张蓉芳, 叶慧琴, 冯彦俊, 卢小泉. 通过扫描光电化学显微镜研究超分子光敏剂-二氧化钛薄膜系统的光诱导电子转移[J]. 电化学, 2023, 29(6): 2218005.

Sheng-Ya Zhang, Min Yao, Ze Wang, Tian-Jiao Liu, Rong-Fang Zhang, Hui-Qin Ye, Yan-Jun Feng, Xiao-Quan Lu. Scanning Photoelectrochemical Microscopic Study in Photoinduced Electron Transfer of Supramolecular Sensitizers-TiO2 Thin Films Systems[J]. Journal of Electrochemistry, 2023, 29(6): 2218005.

DOI: 10.13208/j.electrochem.2218005

Crafting charge transfer channels at titanium dioxide (TiO2) based photoanodes remain a pressing bottleneck in solar-to-chemical conversion technology. Despite the tremendous attempts, TiO2 as the promising photoanode material still suffers from sluggish charge transport kinetics. Herein, we propose an assembly strategy that involves the axial coordination grafting metalloporphyrin-based photosensitizer molecules (MP) onto the surface-modified TiO2 nanorods (NRs) photoanode, forming the composite MP/TiO2 NRs photoelectrode. As expected, the resulted unique MPB/TiO2 NRs photoelectrode displays significantly improved photocurrent density as compared to TiO2 NRs alone and MPA/TiO2 NRs photoelectrode. Scanning photoelectrochemical microscopy (SPECM) and intensity modulated photocurrent spectroscopy (IMPS) were employed to systematically evaluate the continuous photoinduced electron transfer (PET) dynamics for MP/TiO2 NRs photoelectrode. According to the data fitting, it is found that the photoelectron transfer rate (keff) constant for the MPB/TiO2 NRs is about 2.6 times higher than that for the pure TiO2 NRs under light irradiation. The high kinetic constant for the MPB/TiO2 NRs was ascribed to that the conjugated molecules MPB of D-A structure can effectively accelerate intramolecular electrons transfer as well as promote electrons taking part in the reduction reaction of I^3- to I^- in the novel charge transfer channel. The results demonstrated in this study are expected to shed some light on investigating the mechanism in the charge transfer process of artificial photosynthesis and constructing efficient photoelectrodes.

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