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    28 October 2018, Volume 24 Issue 5
    Special Issue for the Best Papers of the Award Winners in Electrochemistry
    Table of Contents
    2018, 24(5):  0. 
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    Preface for the Special Issue of the Award Winners
    Shigang Sun
    2018, 24(5):  407-408.  doi:10.13208/j.electrochem.180140
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          Year 2018 marks the 30th anniversary of the foundation of the Chinese Society of Electrochemistry. The past 30 years have witnessed enormous achievements of the science and technology in electrochemistry in China. The international academic communications become more and more frequent while the research quality ranks in the worldwide forefront, which make China plays more and more important roles in the international community of electrochemistry. With the stern support of domestic researchers and international colleagues, the Chinese professional academic journal,Journal of electrochemistry, has kept growing up and becoming one of the top journals in the science and technology of China.   
          The 19th Chinese National Conference of Electrochemistry was held in Shanghai in 2017. Surrounding the fundamentals, applications and frontiers in the development of electrochemical science and technology, the Conference presented the newest progresses and achievements, discussed in depth on the opportunities, challenges and prospects of electrochemistry, and enhanced the scientific collaborations as well as the technical transformations. It is believed that the every-two-year National Conference will push forwards the development and progress of electrochemistry in Chinese.   
          Series awards were granted in the 19th National Conference of Electrochemistry. The Outstanding Achievement Award was awarded to Prof. Er-kang Wang from Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, for his solid achievements and contributions to electrochemistry science. The Electrochemistry Contribution Award were awarded to Prof. Yong Yang from Xiamen University and Prof. Hua-Min Zhang from Dalian Institute of Chemical Physics. The Electrochemistry Award for Young Scientists were winned by Prof. Yong-Gang Wang from Fudan University, Prof. Xiao-Qing Huang from Soochow University, Shao-Jun Guo from Peking University, and Prof. Jin-Song Hu from Institute of Chemistry, Chinese Academy of Sciences.   
           To encourage and support Chinese scholars, especially the young researchers, to publish their high-quality papers in Journal of Electrochemistry, and to promote the quality of the academic journal of our own, Prof. Zhao-Wu Tian, the member of Chinese Science Academy as well as the Honorary Editor-in-Chief, proposed to set up the “Excellent Paper Awards” of Journal of Electrochemistry. This time the Excellent Paper Awards were delivered to Prof. Zi-Dong Wei from Chongqing University, Prof. Bing-Wei Mao from Xiamen University, Prof. Lin Zhuang from Wuhan University, Prof. Xing-Xing Chen from University of Science and Technology Liaoning, and Prof. Zhan-Ao Tan from North China Electric Power University. 
           To promote the academic exchange and to improve the journal quality, the editorial office invited eight award winners to contribute their newest research work to this special issue of Journal of Electrochemistry. We believe it reflects the representative progresses of electrochemistry in energy, environment and material domains. We wish the publication of the special issue would present the extensive readers the state-of-art, prospects as well as the scientific problems and challenges, can promote the academic effect of the Journal of Electrochemistry, and would push forwards the development of electrochemical science and technology in China.
           Here I would like to thank the authors, the reviewers and the editors for their hard work and selfless contributions! I would also like to say thanks to the extensive electrochemical researchers for your persistent supports to Journal of Electrochemistry!
    Design Strategies toward Highly Active Electrocatalysts for Oxygen Evolution Reaction
    TANG Tang, JIANG Wen-jie, NIU Shuai, HU Jin-song
    2018, 24(5):  409-426.  doi:10.13208/j.electrochem.180146
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    Electrocatalytic water splitting is pivotal for efficient and economical production of hydrogen and oxygen gasses. However, the efficiency of the whole device is largely limited by the oxygen evolution reaction (OER) at the anode due to its sluggish kinetics. Thus, it is imperative to develop inexpensive, highly active OER catalysts to lower the reaction barriers. By examining the underlying critical factors for OER performance, this review outlines general principles for designing efficient nanosized OER catalysts, including (1) enhancing the intrinsic activity of active site by electronic modulation, crystallinity modulation, phase control, defect engineering and spin state engineering; (2) designing appropriate micro/meso/macro structure with high electrical conductivity and mechanical stability to maximize the quantity of accessible active sites, and to promote electron transfer during OER process, as well as to achieve high durability especially at high current density. A series of highly efficient OER catalysts developed by our and other groups are then exemplified to demonstrate the guidance of these principles. At last, some perspectives are highlighted in the further development of efficient OER electrocatalysts, of which can contribute greatly to the achievement in large-scale commercialization of electrocatalytic water-splitting technology.
    Recent Process in Transition-Metal-Oxide Based Catalysts for Oxygen Reduction Reaction
    WANG Yao, WEI Zi-dong
    2018, 24(5):  427-443.  doi:10.13208/j.electrochem.180147
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    Transition metal oxides (TMOs) based catalysts have become the most promising catalysts to be employed in anion exchange membrane fuel cell for the sluggish oxygen reduction reaction (ORR). However, their ORR activity is still far from that of the Pt-based catalysts. Therefore, it is important to develop high performance TMO based catalysts. Electrical conductivity and intrinsic activity have been regarded as the two keys to affect the ORR activity of the TMOs based catalysts. In this review, we focused on the recent progresses in the fundamental viewpoints on the electrical conductivity and intrinsic activity of the TMOs based ORR catalysts. Accordingly, the strategies to enhance the electrical conductivity and intrinsic activity are also summarized. The electrical conductivity could be reinforced in two ways. On the one hand, by coupling with the conductive materials, the external electrical conductivity of TMOs based catalysts could be elevated strongly. On the other hand, the intrinsic electrical conductivity of TMOs based catalysts could be enhanced by introducing oxygen vacancies or doping other cations or anions into TMOs. For the intrinsic activity of the TMOs based ORR catalysts, the crystal structure modulation for TMOs based catalysts is presented. Besides, the ORR descriptor of TMOs based catalysts, which is important for the future catalysts design, is also concluded in this review. And the conclusions and some future perspectives are also outlined. Although many strategies have been proposed to evaluate the electrical conductivity of TMOs based catalysts, there is still room for the further enhancement when the durability of TMOs based catalysts has been taken into consideration. And the ORR mechanism of TMOs based catalysts also should be further explored. Hence, there is a challenging but desired avenue for the development of the high performance TMOs based catalysts which are expected to be applied into anion exchange membrane fuel cell.
    The New Application of Battery-Electrode Reaction: Decoupled Hydrogen Production in Water Electrolysis
    MA Yuan-yuan, GUO Zhao-wei, WANG Yong-gang, XIA Yong-yao
    2018, 24(5):  444-454.  doi:10.13208/j.electrochem.180143
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    Hydrogen has been considered as a promising alternative to unsustainable fossil fuels because of its high calorific value, clean and abundant resources. Water electrolysis combined with renewable energy is regarded as the best way for hydrogen production, which will become the foundation of future hydrogen economy. For the past few years, many efforts have been employed to develop the cheap and high-performance catalyst for hydrogen evolution reaction and oxygen evolution reaction. However,the coupled hydrogen and oxygen evolution and the use of the expensive membrane have greatly restricted the flexibility of the conventional water electrolysis, and hindered the utilization of renewable energy. Recently, our group has introduced the battery-electrode as a solid-state redox mediator to separate the hydrogen and oxygen productions during water electrolysis in space and time, providing a flexible and membrane-free architecture for water splitting. This decoupled architecture also facilitates the conversion of renewable energy to hydrogen. This review highlights the research progresses, and analyzes the advantages and challenges to this new architecture.
    Recent Advances in Non-Noble Metal Nanomaterials for Oxygen Evolution Electrocatalysis
    ZHAO Dan-dan, ZHANG Nan, Bu Ling-zheng, SHAO Qi, HUANG Xiao-qing
    2018, 24(5):  455-465.  doi:10.13208/j.electrochem.180144
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    Hydrogen is a kind of renewable energies with the merits of environmentally friendly, abundance and high weight energy density, which can replace the fossil energy. The electrolysis of water is regarded as the most effective way to generate hydrogen. Owing to the sluggish kinetics and large overpotential of the anode oxygen evolution reaction (OER), the efficiency of the cathode hydrogen evolution reaction is greatly limited. Therefore, it is highly desirable to explore efficient, stable and low cost electrocatalysts to reduce the overpotential of OER and improve the efficiency of hydrogen evolution. Based on the natural characteristics of non-noble metal catalysts and their excellent OER activities in high hydroxyl ion (OH-) concentrations, the OER mechanism in alkaline conditions and the methods for OER performance evaluation are firstly introduced in this review. Then the recent research progresses in non-noble metal nanomaterial electrocatalysts for OER are mainly illustrated. Finally, some perspectives are highlighted with the in-depth insights of catalytic mechanism, the designs of bifunctional and novel non-noble metal catalysts.
    Recent Progress in Organic Redox Flow Batteries
    XIA Li-xing, LIU Hao, LIU Lin, TAN Zhan-ao
    2018, 24(5):  466-487.  doi:10.13208/j.electrochem.180142
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    Redox flow batteries (RFBs) are promising candidate for balancing instability of grids caused by integration of intermittent renewable energies such as solar energy and wind energy. Along with wide deployments in solar energy and wind energy due to abundance and declining installation cost, it can be predicted that RFBs will enter a period of rapid development. Basically,RFBs are electrochemical energy storage devices that decouple energy and power of the system by storing liquid electrolyte in tanks outside battery system itself. Such a unique framework makes RFBs flexible and fulfills the various demands of grids. During battery operation, redox-active species are energy-conversion carriers by changing molecular valence states, and thus, are critical elements for RFBs. Traditional RFBs employ inorganic materials as redox-active species, however, high cost, toxicity, resource limitation, dendrite formation and low electrochemical activity of inorganic redox-active species have hindered RFBs toward a large-scale application. Owing to advantages of low-cost, "green", abundance, molecular-energy-level (MEL) tunability and rapid redox kinetics,organic active species have drawn much attention in academic and industrial communities. In recent few years, performances of organic redox flow batteries (ORFBs) have been improved rapidly, and a series of novel organic active species have been explored and developed. This article reviews recent progresses in ORFBs. Firstly, an application field and working principle of RFBs are briefly introduced, and then technical features of vanadium redox flow battery (VRFB), zinc based flow battery (ZBFB), and hydrogen-based flow battery (HBFB) are presented with reasons for developing organic active species. Subsequently, based on a variety of support electrolyte, aqueous organic redox flow batteries (AORFBs) can be divided into acid, alkaline and neutral forms with merits and limitations of these systems are discussed. Non-aqueous organic redox flow batteries (NAORFBs) are also discussed in terms of energy density, current density, stability and bipolar molecule. Finally, the critical challenges and potential research opportunities for developing practically relevant ORFBs are prospected.
    Research Progresses in Improvement for Low Temperature Performance of Lithium-Ion Batteries
    GU Yue-ru, ZHAO Wei-min, SU Chang-hu, LUO Chuan-jun, ZHANG Zhong-ru, XUE Xu-jin,YANG Yong
    2018, 24(5):  488-496.  doi:10.13208/j.electrochem.180145
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    Lithium-ion batteries (LIBs) have become a new research hotspot due to their high energy density and long service life. However, the temperature characteristics, especially the poor performance at low temperatures, have seriously limited their wider applications. In this report, the research progresses in the low temperature performance of LIBs are reviewed. The main existing limitations of LIBs at low temperatures were systematically analyzed, and followed by discussion on the recent improvements in low temperature performances by developing novel cathode, electrolyte, and anode materials. The developments for improving the low temperature performance of LIBs are prospected. The three most important factors that influence the low temperature electrochemical performance of LIBs are as follows: 1) a reduced ion conductivity of the electrolyte and solid electrolyte interface (SEI) film formed on the electrode/electrolyte interface; 2) increased charge-transfer resistances at both the cathode and anode electrolyte- electrode interfaces; 3) slow lithium diffusion in the electrodes. The above three points lead to high polarization and lithium deposition, which may cause problems in terms of performance, reliability and safety of the cell. The key point is to provide expedite paths for the transport of lithium ions and electrons at low temperatures. All the influential aspects, such as cathode, electrolyte,and anode, should be considered to improve the low temperature performance of LIBs. The low temperature electrolyte can be obtained by adjusting the relative compositions, and species of the solvent, salt, and additive. The conductivity of electrolyte can be improved by adding low melting point cosolvents and salts. In addition, use of electrolyte additives forming low impedance interface film is one of the most economic and effective methods to improve the low temperature performance. And the structure of electrode materials can be optimized by doping, coating and decreasing the particle size, which can ensure sufficient conductivity and shorten diffusion path length for lithium ions and electrons. Managing the electrolyte and developing electrodes are efficient methods to improve the low temperature performance. Future studies should be focused on achieving high performance lithium-ion battery materials.
    Preparation of Nanoprobes and Their Possible Applications in Nanoscale Scanning Electrochemical Microscopy for Studying Electrocatalytic Oxygen and Hydrogen Reactions
    CHEN Xing-xing
    2018, 24(5):  497-510.  doi:10.13208/j.electrochem.180141
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    Scanning electrochemical microscopy (SECM) is a type of scanning probe microscopy, which can not only provide the topographical information, but also offer the electrochemical properties of different samples. The interrelationship of physical and electrochemical properties of a sample can be searched at a high-resolution scale due to the introduction of ultramicroelectrode (UME). With the continuous development of modern nanotechnology, the SECM probe has been improved with drastically decreasing its size down to nanometer. Meanwhile, to evaluate and understand the electrochemical performance of various electrocatalysts for both oxygen and hydrogen reactions with high-efficiency is highly demanded in the research area of green new energy conversion and storage systems, such as regenerative fuel cells and rechargeable metal-air batteries. Therefore, this review will provide a snapshot in the preparations and developments for different types of nanoprobes of SECM. The recent advances in applications of nanoscale SECM in studies of electrocatalysts for both oxygen and hydrogen reactions are also summarized. Finally, some prospects for the future development of nanoscale SECM are discussed.
    An Investigation on the Structure of Au(111)/Imidazolium-Based Ionic Liquid Interface: Effect of Alkyl Side Chain Length
    CHEN Li, LIU Shuai, LI Mian-gang, Su Jian-jia, YAN Jia-wei, MAO Bing-wei
    2018, 24(5):  511-516.  doi:10.13208/j.electrochem.180148
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    In this work, we comparatively investigated the interfacial structures at Au(111) electrode surfaces in two ionic liquids (ILs) with different alkyl chain lengths by combining AFM force curve technique and electrochemical methods. The number and stability of the layering structures, and their potential-dependency were analyzed. The experimental results indicated that the tendencies of force-potential curves in the two ILs behave the same way. At potentials close to PZC, the ions arrange loosely, which lowers the stability of the layering structure. As the potential shifting away from PZC, more ions attach to electrode surface, which increases the stability of layering structure, while further increase of the ions will weaken the stability because of the lattice saturation of ions. However, the location of the alkyl chain at potentials negative to the PZC differs from that at potentials positive to the PZC, leading to an adverse effect on the stability at negatively charged surface and a synergistic effect on the stability at positively charged surface, respectively.
    Recent Advances in Continuous Models of Electrochemical Supercapacitors
    LU Hao-tian, ZHOU Jing-hong, YE Guang-hua, ZHOU Xing-gui
    2018, 24(5):  517-528.  doi:10.13208/j.electrochem.180409
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    Electrochemical capacitors (supercapacitors) have been developed as a new type of energy storage device with high energy and power densities, which have the advantages of both fast charging-discharging as traditional capacitors and high energy density as batteries. Notable improvements in their electrochemical performance have been achieved in recent years owing to the recent advances in understanding of charge storage mechanisms and the development of advanced nanostructured materials. Recently, modeling and simulation of these supercapacitors has been applied as a useful approach to better understand the working mechanisms of the supercapacitors by describing the concentrations and electric fields inside the capacitors. Particularly, the continuous models for supercapacitors, which can provide insights into the mass transport and interfacial phenomena in supercapacitors under different operating conditions, have been drawing more and more attention. And there is no review article addresses this topic so far. This paper will try to summarize the basic theories of supercapacitors and the latest progresses in the continuous models for supercapacitors. The focus is the recent advances in the application of continuous models to optimize device parameters under different conditions. Meanwhile, the prospects and challenges associated with the continuous models in the future are also discussed. We believe that modelling of supercapacitors could help design the next-generation supercapacitors for versatile electronic devices.
    Effects of Sulfur-Containing Additive on Low Temperature Performance of Graphite Anode
    WU Ze-li, ZHENG Ye-zhen, ZHANG Zhong-ru, YANG Yong
    2018, 24(5):  529-537.  doi:10.13208/j.electrochem.180322
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    The low temperature performance of lithium ion battery mainly depends on the graphite anode, and one of the research focuses is to improve the low temperature performance of the anode by additives. In this paper, the effects of different sulfur-containing functional groups such as DTD (ethylene sulfate), 1,3-PS (1,3-propane sultone) and ES (ethylene sulfite) on low temperature performances of artificial graphite materials were systematically studied. The results in density functional theory (DFT) calculations, cyclic voltammetry (CV), scanning electron microscopy (SEM) and charge-discharge measurement clearly demonstrated that all three sulfur-containing additives could participate in formation of films on the surface of electrode, which had a greater impact on the low temperature properties. The apparent enhancement was achieved with DTD because of the film formed with a smaller resistance. In contrast, the reduced performance was observed with 1,3-PS due to its non-conductive film formed at low temperatures, while no obvious effect with ES. The data in electrochemical impedance spectroscopy (EIS) and X-ray photoelectron spectroscopy (XPS) indicated that these three kinds of additives influenced differently the low temperature performances of lithium ion battery due mainly to their significantly different impedances resulted from the films formed at the interfaces of electrodes.
    Electrochemical Deposition of Cr from Cr(III)-Based [BMIM]HSO4 and NaOAc Electrolyte
    LIU De-ying,LUO Wei,ZHANG Wen-juan,HU Shuo-zhen,XU Heng,ZHANG Xin-sheng
    2018, 24(5):  538-545.  doi:10.13208/j.electrochem.180326
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    Using trivalent chromium ions (Cr(III)) as the chromium source for chromium electrodeposition has attracted much attention since it can reduce the toxicity of the whole process. Even though the chromium deposition in Cr(III)-based ionic liquid bath can avoid the most hydrogen evolution problem, CrCl3·6H2O is widely used as the Cr(III) precursor, which still contains water and has the stable octahedral structure. As a result, it is difficult to deposit Cr and there is still hydrogen evolution reaction (HER). Moreover, the hydroxyl ions (OH-) produced during HER react with Cr3+ to form Cr(OH)3, which will affect the performance and property of the Cr layer. To avoid the formation of Cr(OH)3, 1-butyl-3-methylimidazolium hydro sulfate ([BMIM]HSO4) aqueous solution was used as the electrolyte in this work. To enhance the depositing ability and to lower the reduction onset potential of Cr(III), NaOAc was used as the additive. Electrochemical measurements such as cyclic voltammetry (CV) and linear sweep voltammetry (LSV) were made to test the electrochemical performance in different electrolytes. Chromium layers were electrodeposited on copper plates at a constant potential of -3.0 V (vs. Pt). The Cr thickness and current efficiency were calculated based on the gravimetric method. Scanning electron microscopy (SEM), X-ray diffraction (XRD) and energy dispersive X-ray spectroscopy (EDX) techniques were used to study the surface morphology, crystalline structure and elemental composition of the deposited Cr layer, respectively. The cyclic voltammetric results showed that the reduction of Cr(III) to Cr(0) is a two-step process. First, Cr(III) reduced to Cr(II) at -1.50 V (vs. Pt). Then, Cr(II) further reduced to Cr(0) at -2.10 V (vs. Pt). Both of the peak current and peak potential followed the Rendle-Sevcik equation, by which the diffusion coefficient of Cr3+ at 40 ℃ was calculated to be 1.6 ×10-8 cm2·s-1. The XRD and SEM characterizations indicated that the Cr coating layers were composed of Cr nanoparticles with an average particle size of 0.87μm. The NaOAc effect on the electrodeposition of Cr was also studied. After adding NaOAc, the reduction peak potential of Cr(III)shifted to positive direction, indicating less energy required to reduce Cr3+. Additionally, the molar ratio of Cr:O in the coating layer increased from 4.48 to 6.28, indicating that OAc- was helpful for the electrodeposition of Cr metal. This was because the addition of OAc- could break the stable octahedral structure of CrCl3·6H2O. Overall, the best coating thickness (63 μm) and highest current efficiency (33.5%) were obtained when the molar ratio of NaOAc-[BMIM]HSO4-CrCl3-H2O electrolyte was 0.075:1:0.5:6. Based on this study, it can be concluded that [BMIM]HSO4-NaOAc aqueous electrolyte might be benefited to electrodeposit pure Cr, instead of Cr(OH)3, with relatively high current efficiency and low reduction onset potential.
    Electrodeposition of Cobalt from Eutectic-Based Ionic Liquid
    M. Rostom Ali, S Sankar Saha, Md Ziaur Rahman
    2018, 24(5):  546-554.  doi:10.13208/j.electrochem.161123
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    The electrodeposition of cobalt from a solution containing cobalt chloride in either a urea-choline chloride based or an ethylene glycol (EG)-choline chloride based ionic liquid has been carried out onto copper and steel cathodes by constant current and constant potential methods at different temperatures. The influences of various experimental conditions on electrodeposition and morphology of the deposited layers have been investigated by scanning electron microscopy (SEM) and X-ray diffraction (XRD)technique. It has been shown that the smooth, shiny with good adherence and bright metallic coloured cobalt coatings were obtained from both urea and EG based ionic liquids at the applied deposition potentials up to -0.8 V and applied deposition current densities up to -6.0 A·m-2 by the addition of 0.05 mol·L-1 P2O5 at temperatures ranging from 30 to 90 ℃. The cathodic current efficiency for the deposition of cobalt reached 98%.
    Synthesis of Keggin Polyoxometalates Modified Carbon Paste Electrode as A Sensor for Dopamine Detection
    DONG Peng-fei, LI Na, ZHAO Hai-yan, CUI Min, ZHANG Cong, REN Ju-jie,JI Xue-ping
    2018, 24(5):  555-562.  doi:10.13208/j.electrochem.180405
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    Polyoxometalates, a class of anionic clusters with structure diversity and size variability, make them very attractive in many fields such as electrochemistry, catalysis and medicine. The Co(C15N6H12)2[PW12O38]·5H2O(Co[PW12O38]) modified carbon paste electrode was prepared in this work, and its electrochemical performances as the sensor for dopamine detection were characterized with electrochemical impedance spectroscopy, cyclic voltammetry and differential pulse voltammetry. The preparation conditions and test conditions were optimized respectively. Under the optimized conditions, the POMs modified carbon paste electrode exhibited good selectivity and sensitivity in dopamine detection. The linear response range was from 8.0 × 10-6 mol·L-1 to 3 × 10-5 mol·L-1, and the sensitivity was 0.039 μA·(μmol·L-1)-1 with the detection limit of 5.4 × 10-6 mol·L-1 (S/N=3). The POMs modified carbon paste electrode used for the dopamine sensing showed good stability, repeatability and anti-interference under the coexistence of ascorbic acid, uric acid and so on. The preparation process was simple, convenient, and low cost, and the electrode obtained had good sensing performance, thus, the present POMs modified electrode demonstrated a promising application for the detection of dopamine.
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    2018, 24(5):  563-564. 
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    2018, 24(5):  565-567. 
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    2018, 24(5):  568-569. 
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    2018, 24(5):  570-570. 
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