Electrochemical science advances最新文献

Electrochemical Contributions: Svante August Arrhenius (1859–1927) 电化学的贡献斯凡特-奥古斯特-阿伦尼乌斯（1859-1927）

IF 2.9 Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2024-07-15 DOI: 10.1002/elsa.202400020

Evgeny Katz

Svante August Arrhenius (Figure 1) was a Swedish scientist, educated as a physicist, but mostly contributed to chemistry. He established a new scientific filed of physical chemistry. Although he was not the only founder of this novel area combining physics and chemistry, his work was critically important for formulation and methodology of physical chemistry (Figure 2).The most important scientific contribution made by Arrhenius was invention of the electrolytic dissociation theory. This theory explained ionic conductivity in salt/acid/base-solutions and provided background for research of electrochemical processes, including electroanalytical chemistry, electrolysis and battery chemistry. The first formulation of this theory, presently known as the Arrhenius dissociation theory, was made in his PhD thesis submitted in 1884: “Recherches sur la conductibilite galvanique des electrolytes” (Investigations on the galvanic conductivity of electrolytes). The theoretical assumption made by him was well supported with extensive experimental work made by Arrhenius, still being a student. The electrical conductivity in aqueous solutions of salts, acids and bases was explained by splitting the dissolved molecules or crystals in ions (positively charged cations and negatively charged anions). Particularly for acids and bases, he suggested their definitions based on generation of H+ and OH− ions in the case of acids and bases, respectively. This definition of the acids and bases still keeps his name: Arrhenius acids and Arrhenius bases.The Arrhenius theory had some connections to the early work made by Michael Faraday (English scientist, 1791–1867). Faraday, while studying electrolysis process, also proposed generation of cations and anions supporting conductivity in solutions. However, Faraday believed that their formation proceeds at electrode surfaces only upon pathing electric current through solutions. This explanation is incorrect according to the modern science. The Arrhenius theory proposed the cation and anion formation just upon dissolution of salts, acids, or bases, regardless the electric current applied. The dissociation of molecules into cations and anions (x2), according to the Arrhenius theory, proceeds due to weakening polaric chemical bonds in solutions based on solvents with the high dielectric constants (high polarity of the solvent molecules, water in the original Arrhenius work). This explanation appears to be correct.It is interesting to note that the theory of the electrolytic dissociation was so much novel that it was poorly accepted by the scientific community, particularly, his PhD thesis received a low score. Notably, later his theory was awarded with the Nobel Prize. Arrhenius received the Nobel Prize for Chemistry in 1903, becoming the first Nobel laureate in Sweden. Shortly after that, in 1905, Arrhenius became the director of the Nobel Institute, where he remaine

斯凡特-奥古斯特-阿伦尼乌斯（Svante August Arrhenius，图 1）是瑞典科学家，曾接受物理学家教育，但主要从事化学研究。他创立了物理化学这一新的科学领域。阿伦尼乌斯最重要的科学贡献是发明了电解解离理论。这一理论解释了盐/酸/碱溶液中的离子导电性，为电化学过程（包括电分析化学、电解和电池化学）的研究提供了背景。他在 1884 年提交的博士论文中首次提出了这一理论，即现在的阿伦尼乌斯解离理论：他在 1884 年提交的博士论文 "Recherches sur la conductibilite galvanique des electrolytes"（关于电解质电导率的研究）中首次提出了这一理论。他的理论假设得到了当时还是学生的阿伦尼乌斯大量实验工作的有力支持。盐、酸和碱水溶液的导电性是通过将溶解的分子或晶体分裂成离子（带正电的阳离子和带负电的阴离子）来解释的。特别是对于酸和碱，他分别根据酸和碱产生的 H+ 离子和 OH- 离子提出了定义。阿伦尼乌斯理论与迈克尔-法拉第（Michael Faraday，英国科学家，1791-1867 年）的早期研究有一定的联系。法拉第在研究电解过程时，也提出了在溶液中产生支持导电性的阳离子和阴离子。不过，法拉弟认为，只有当电流通过溶液时，它们才会在电极表面形成。根据现代科学，这种解释是不正确的。阿伦尼乌斯理论认为，无论电流大小，只要盐、酸或碱溶解，就会形成阳离子和阴离子。根据阿伦尼乌斯理论，分子解离成阳离子和阴离子（x2）的过程是由于在高介电常数（溶剂分子的高极性，即阿伦尼乌斯原著中的水）溶剂中极性化学键的减弱。有趣的是，由于电解解离理论过于新颖，科学界对其接受度很低，尤其是他的博士论文得分很低。值得注意的是，后来他的理论获得了诺贝尔奖。1903 年，阿伦尼乌斯获得诺贝尔化学奖，成为瑞典第一位诺贝尔奖获得者。此后不久，1905 年，阿伦尼乌斯成为诺贝尔研究所所长，并一直担任这一重要职务，直到 1927 年去世。为了表彰他的科学贡献，阿伦尼乌斯解离理论、阿伦尼乌斯方程、阿伦尼乌斯酸和阿伦尼乌斯碱都以他的名字命名。

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引用次数: 0

Electrochemical contributions: Tatyana Aleksandrovna Kryukova (1906–1987) 对电化学的贡献塔季扬娜-亚历山大罗夫娜-克留科娃（1906-1987）

Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2024-01-12 DOI: 10.1002/elsa.202400001

Evgeny Katz

Tatyana Alexandrovna Kryukova (Figure 1), a Russian scientist and electrochemist, made important contributions to electroanalytical chemistry (Figure 2), particularly working in close collaboration with Professor Aleksandr Naumovich Frumkin, who was the greatest Russian scientist in the area of electrochemistry. Kryukova is particularly remembered for developing the theory of polarographic maxima, which were observed as a sharp increase in the current produced upon polarographic measurements under some conditions (Figure 3). These current peaks originated from tangential movements (rotation) of a mercury droplet electrode, then stimulating diffusion in the depletion layer and current increase. Kryukova experimentally observed and theoretically explained the formation and then inhibition of these peaks upon adsorption of organic substances (mostly surfactants) on a mercury droplet electrode. It should be noted that for the first time, the effect of surfactants on polarographic measurements was reported in the 1920s in the laboratory of Professor Jaroslav Heyrovský (polarography inventor and Nobel Prize laureate in 1959), and the study of this effect was published in 1931. However, the study of the surfactant effect performed by Heyrovský was only fragmental. Then, the credit for a detailed explanation of the reasons for the polarographic maxima origin and a systematic study of this effect belongs to Kryukova.In 1949, Kryukova discovered another very unusual phenomenon, later named as “Kryukova effect” (Figure 4). This effect was observed as a sudden decrease in the current at very negative potentials upon polarographic reduction of anionic species, for example, persulfate or dichromate anions, particularly when a very diluted supporting electrolyte was present in the analyte solution. This current minimum disappeared when the electrolyte concentration was increased. Later, in 1952, Frumkin and G. M. Florianovich (a graduate student at that time) theoretically explained the effect observed by Kryukova as the repulsion of redox anions from the negatively charged electrode surface, as predicted by the Frumkin theory of 1933. This is exactly why the effect was only observed for anionic redox species particularly with very negative potentials, providing a negative charge at the working electrode. As expected, the high concentration of the supporting electrolyte was screening the electrostatic interaction between the negative Hg droplet electrode and the negative redox-anions, then eliminating the current decrease.It should be noted that the electrochemical study of persulfate ions when the “Kryukova effect” was observed, had not only gained theoretical interest demonstrating a fundamental electrostatic effect at polarized electrodes, but it was also practically important as a part of the Russian uranium project because they were used as a reagent in the separation of uranium isotopes.Kryukova published many important research pa

俄罗斯科学家和电化学家塔季扬娜-亚历山德罗芙娜-克留科娃（Tatyana Alexandrovna Kryukova）（图 1）对电分析化学做出了重要贡献（图 2），尤其是与亚历山大-瑙莫维奇-弗鲁姆金（Aleksandr Naumovich Frumkin）教授密切合作，后者是俄罗斯电化学领域最伟大的科学家。Kryukova 因提出了极谱最大值理论而被世人所铭记，极谱最大值是指在某些条件下进行极谱测量时产生的电流急剧增加（图 3）。这些电流峰值源于汞滴电极的切向运动（旋转），然后刺激耗尽层的扩散和电流增加。Kryukova 通过实验观察并从理论上解释了有机物质（主要是表面活性剂）在汞液滴电极上吸附时这些峰值的形成和抑制。需要指出的是，20 世纪 20 年代，Jaroslav Heyrovský 教授（极谱学发明人，1959 年诺贝尔奖获得者）的实验室首次报道了表面活性剂对极谱测量的影响，并于 1931 年发表了对这一影响的研究报告。然而，海罗夫斯基对表面活性剂效应的研究只是片面的。1949 年，克留科娃发现了另一种非常不寻常的现象，后来被命名为 "克留科娃效应"（图 4）。这种效应表现为阴离子物质（如过硫酸盐或重铬酸根阴离子）在极化还原时，电流在极负电位突然减小，尤其是当分析溶液中存在非常稀释的支持电解质时。当电解质浓度增加时，这种电流最小值就会消失。后来，弗鲁姆金和 G. M. Florianovich（当时的研究生）于 1952 年从理论上解释了 Kryukova 观察到的效应，正如 1933 年弗鲁姆金理论所预测的那样，氧化还原阴离子与带负电荷的电极表面相排斥。这正是为什么只有在阴离子氧化还原物种中才能观察到这种效应，特别是在电位非常负的情况下，工作电极上会产生负电荷。值得注意的是，在观察到 "克留科娃效应 "时对过硫酸根离子进行的电化学研究不仅在理论上证明了极化电极上的基本静电效应，而且作为俄罗斯铀项目的一部分也具有重要的实际意义，因为它们被用作分离铀同位素的试剂。克留科娃发表了许多重要的研究论文，她与其他几位科学家合作撰写的长达 800 页的教科书《极谱分析》于 1959 年以俄文出版，多年来一直是苏联最重要的教材和极谱学参考指南之一。

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引用次数: 0

Electrochemical contributions: Ludwig Mond (1839−1909) 电化学的贡献路德维希-蒙德（1839-1909）

Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2024-01-12 DOI: 10.1002/elsa.202400002

Evgeny Katz

The general concept of fuel cells starts from the experiments of British physicist William Grove who published the first results on fuel cells in 1839. He used hydrogen and oxygen as a fuel and oxidizer, respectively, reacting on platinum catalytic electrodes and generating electric power. However, his research was considered only as scientific proof of the process reversed to the water electrolysis with no practical importance. Indeed, the cell invented by Grove produced a very small current and voltage over a short time. Obviously, after the concept demonstration, some engineering had to be done for improving the cell efficiency to make it feasible for practical use.

During the late 1880s, two British chemists, Ludwig Mond and his assistant Carl Langer (Figure 1), developed a fuel cell with a longer service life with improved geometry of the catalytic electrodes and flow channels (Figure 2). They used the known scientific concept from Grove's cell, but with the improved engineering. Their fuel cell generated 6 amps per square foot current density and 730 mV voltage. The cell operated with coal-derived gas as a fuel and air (actually oxygen in the air) as an oxidizer. The cell was filled with diluted sulfuric acid and included thin perforated platinum electrodes separated with a porous nonconducting membrane. The first engineered fuel cell was demonstrated and patented in 1889. Note that Ludwig Mond and Carl Langer were the first to introduce the term “fuel cell” which is commonly used now.

The author declares that he has no conflict of interest.

燃料电池的一般概念源于英国物理学家威廉-格罗夫的实验，他于 1839 年发表了燃料电池的首批研究成果。他将氢气和氧气分别作为燃料和氧化剂，在铂催化电极上发生反应并产生电能。然而，他的研究仅被认为是对水电解反向过程的科学证明，并无实际意义。事实上，格罗夫发明的电池在短时间内产生的电流和电压非常小。19 世纪 80 年代末，两位英国化学家路德维希-蒙德和他的助手卡尔-朗格（图 1）通过改进催化电极和流道的几何形状，开发出一种使用寿命更长的燃料电池（图 2）。他们采用了格鲁夫电池的已知科学概念，但改进了工程设计。他们的燃料电池可产生每平方英尺 6 安培的电流密度和 730 毫伏的电压。该电池使用煤制气作为燃料，空气（实际上是空气中的氧）作为氧化剂。电池中充满了稀硫酸，包括用多孔非导电膜隔开的薄穿孔铂电极。第一个工程燃料电池于 1889 年展示并获得专利。请注意，路德维希-蒙德（Ludwig Mond）和卡尔-朗格（Carl Langer）是第一个提出 "燃料电池 "一词的人，该词现在已被普遍使用。

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引用次数: 0

Electrochemical contributions: John Alfred Valentine Butler (1899–1977) 电化学贡献约翰-阿尔弗雷德-瓦伦丁-巴特勒（1899-1977）

Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2024-01-12 DOI: 10.1002/elsa.202400003

Evgeny Katz

John Alfred Valentine Butler was the first to connect the kinetic electrochemistry built up in the second half of the twentieth century with the thermodynamic electrochemistry that dominated the first half. John Alfred Valentine Butler had, to his credit, not only the first exponential relation between current and potential (1924) but also (along with R.W. Gurney) the introduction of energy-level thinking into electrochemistry (1951).

However, Butler was not alone in this study and therefore it is necessary to give credit also to Max Volmer, a great German surface chemist, and his student (at that time) Erdey-Gruz. Butler's very early contribution in 1924 and the Erdey-Gruz and Volmer contribution in 1930 form the basis of phenomenological kinetic electrochemistry. The resulting famous Butler-Volmer equation is very important in electrochemistry.

The author declares no conflict of interest.

约翰-阿尔弗雷德-瓦伦丁-巴特勒是第一个将二十世纪下半叶建立起来的动力学电化学与在上半叶占主导地位的热力学电化学联系起来的人。约翰-阿尔弗雷德-瓦伦丁-巴特勒不仅首次提出了电流与电势之间的指数关系（1924 年），而且（与 R.W. 格尼一起）将能级思想引入了电化学（1951 年），这都是他的功劳。然而，巴特勒并不是唯一从事这项研究的人，因此有必要将功劳归于德国伟大的表面化学家马克斯-沃尔默和他的学生（当时）埃尔德-格鲁兹。巴特勒在 1924 年的早期贡献以及埃代-格鲁兹和沃尔默在 1930 年的贡献构成了现象动力学电化学的基础。由此产生的著名的巴特勒-沃尔默方程在电化学中非常重要。

引用次数: 0

Sustainable supercapacitor with a natural rubber‐based electrolyte and natural graphite‐based electrodes 采用天然橡胶电解质和天然石墨电极的可持续超级电容器

Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2023-12-26 DOI: 10.1002/elsa.202300025

K. Perera, K. Vidanapathirana, Lewis J. Adams, N. Balakrishnan

Supercapacitors are at the forefront of energy storage devices due to their ability to fulfill quick power requirements. However, safety and cost are important parameters for their real‐world applications. Green materials‐based electrodes and electrolytes can make them safer and cost‐effective. Herein, a supercapacitor based on a methyl‐grafted natural rubber/salt‐based electrolyte and natural graphite (NG)‐based electrodes are fabricated and characterized. Zinc trifluoromethanesulfonate [Zn(CF3SO3)2] is used as the salt for the electrolyte. A mixture of NG, activated charcoal, and polyvinylidenefluoride is used for electrodes. Our supercapacitor shows a single electrode specific capacitance, Csc of 4.2 Fg−1 from impedance measurement. Moreover, the capacitive and resistive features are dominant at low and high frequencies, respectively. The cyclic voltammetry test shows the dependence of Csc on the scan rate with a high value at slow scan rates. Performance of the supercapacitor during 5000 charge and discharge cycles at a constant current of 90 μA shows a rapid decrease of single electrode specific discharge capacitance at the beginning, but it starts to stabilize after about 2500 cycles. These findings are relevant to further developments of green materials‐based supercapacitors, offering opportunities to expand the functionalities of supercapacitors in green technologies.

超级电容器能够满足快速的电力需求，因此处于储能设备的最前沿。然而，安全和成本是其实际应用的重要参数。基于绿色材料的电极和电解质可以使超级电容器更安全、更经济。本文制备了一种基于甲基接枝天然橡胶/盐基电解质和天然石墨（NG）电极的超级电容器，并对其进行了表征。电解质采用三氟甲磺酸锌[Zn(CF3SO3)2]。电极使用了 NG、活性炭和聚偏氟乙烯的混合物。阻抗测量显示，我们的超级电容器的单电极比电容 Csc 为 4.2 Fg-1。此外，电容和电阻特性分别在低频和高频时占主导地位。循环伏安测试表明，Csc 与扫描速率有关，扫描速率较低时，Csc 值较高。在 90 μA 的恒定电流下，超级电容器在 5000 次充放电循环期间的性能表明，单电极比放电电容在开始时迅速下降，但在大约 2500 次循环后开始趋于稳定。这些发现与基于绿色材料的超级电容器的进一步开发有关，为扩大超级电容器在绿色技术中的功能提供了机会。

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引用次数: 0

Electrical energy input efficiency limitations in CO₂‐to‐CO electrolysis and attempts for improvement CO2 - to - CO电解中电能输入效率的限制及改进尝试

Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2023-11-13 DOI: 10.1002/elsa.202300024

Thomas Reichbauer, Bernhard Schmid, Kim‐Marie Vetter, David Reinisch, Nemanja Martić, Christian Reller, Alexander Grasruck, Romano Dorta, Günter Schmid

Abstract Electrochemical CO 2 reduction is a potentially up‐coming technology to convert anthropogenic emitted CO 2 into chemical feedstock. Due to alkaline operating conditions of CO 2 ‐electrolyis in gas diffusion electrodes, exothermal hydroxide ion neutralization with the excess of supplied CO 2 leads to unavoidable electricity‐to‐heat conversion at the cathode, therefore limiting electrical energy input efficiency. The decomposition reaction of carbonates by protons from water oxidation completes the inherent CO 2 transport at the anode. In this work, different production routes to CO are thermodynamically examined and experimentally validated. Using formic acid as an intermediate towards CO the electrical energy input efficiency can rise to 71% on a thermodynamical basis. Additionally, the possibility of altering the mechanism of CO 2 reduction under acidic conditions is investigated, which would lead to even larger electrical energy input efficiencies. The concept was investigated by pH series measurements (pH = 0–6) at 50 mA/cm 2 where Pb derived from Pb 3 O 4 was used as a CO 2 reduction catalyst. The reduction to formic acid under acidic bulk electrolyte pH is stable at FE HCOOH = 70% down to pH ≈ 1, while HER is becoming dominant below. Even under such acidic bulk electrolyte conditions no change in reduction mechanism could be forced, which is reflected in invariant cell voltages in the model experiment.

电化学CO 2还原是一种将人为排放的CO 2转化为化学原料的潜在技术。由于气体扩散电极中CO 2 -电解质的碱性操作条件，放热氢氧化物离子中和与过量供应的CO 2导致阴极不可避免的电-热转换，因此限制了电能输入效率。由水氧化产生的质子对碳酸盐的分解反应完成了在阳极固有的CO 2运输。在这项工作中，对不同的CO生产路线进行了热力学检查和实验验证。在热力学基础上，使用甲酸作为CO的中间体，电能输入效率可提高到71%。此外，还研究了在酸性条件下改变CO 2还原机制的可能性，这将导致更大的电能输入效率。该概念通过pH系列测量(pH = 0-6)在50 mA/ cm2下进行了研究，其中Pb来源于pb3o4作为CO 2还原催化剂。酸性电解液pH值在FE HCOOH = 70%至pH≈1范围内还原为甲酸较为稳定，在FE HCOOH = 70%至pH≈1范围内，HER的还原作用逐渐占主导地位。即使在这种酸性的散装电解质条件下，也不能强迫还原机制发生变化，这在模型实验中反映在不变的电池电压上。

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引用次数: 0

Through the interface: New insights of the hydrogen evolution and oxidation reactions in aqueous solutions 穿越界面：水溶液中氢进化和氧化反应的新见解

Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2023-10-30 DOI: 10.1002/elsa.202300016

Ershuai Liu, Li Jiao, Qingying Jia, Sanjeev Mukerjee

Hydrogen evolution and oxidation reactions (HER/HOR) are the most fundamental reactions in electrocatalysis. Despite the practical significance, the mechanisms of HER/HOR in aqueous solutions are still elusive. Various theories have been proposed to rationalize the pH effect, cation effect, and structure effect of HER/HOR but none of them can explain all observations. In this review, we discuss four schools of thought for the HER/HOR, focusing on the strengths and shortcomings of each hypothesis and highlighting the magnitude of electrochemical interface structure in hydrogen electrocatalysis.

氢气进化和氧化反应（HER/HOR）是电催化中最基本的反应。尽管氢进化和氧化反应具有重要的实际意义，但其在水溶液中的机理仍然难以捉摸。人们提出了各种理论来解释 HER/HOR 的 pH 值效应、阳离子效应和结构效应，但没有一种理论能解释所有的观察结果。在这篇综述中，我们将讨论 HER/HOR 的四种学说，重点讨论每种假说的优势和不足，并强调电化学界面结构在氢气电催化中的重要性。

引用次数: 0

Investigation of physicochemical drivers directing ionic liquid assembly on polymeric nanoparticles 高分子纳米粒子上离子液体组装的物理化学驱动因素研究

Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2023-10-04 DOI: 10.1002/elsa.202300013

Sara X. Edgecomb, Christine M. Hamadani, Angela Roberts, George Taylor, Anya Merrell, Ember Suh, Mahesh Loku Yaddehige, Indika Chandrasiri, Davita L. Watkins, Eden E. L. Tanner

Abstract Ionic liquids (ILs) have emerged as promising biomaterials for enhancing drug delivery by functionalizing polymeric nanoparticles (NPs). Despite the biocompatibility and biofunctionalization they confer upon the NPs, little is understood regarding the degree in which non‐covalent interactions, particularly hydrogen bonding and electrostatic interactions, govern IL‐NP supramolecular assembly. Herein, we use salt (0‐1 M sodium sulfate) and acid (0.25 M hydrochloric acid at pH 4.8) titrations to disrupt IL‐functionalized nanoassembly for four different polymeric platforms during synthesis. Through quantitative 1 H‐nuclear magnetic resonance spectroscopy and dynamic light scattering, we demonstrate that the driving force of choline trans‐2‐hexenoate (CA2HA 1:1) IL assembly varies with either hydrogen bonding or electrostatics dominating, depending on the structure of the polymeric platform. In particular, the covalently bound or branched 50:50 block co‐polymer systems (diblock PEG‐PLGA [DPP] and polycaprolactone [PCl]‐poly[amidoamine] amine‐based linear‐dendritic block co‐polymer) are predominantly affected by hydrogen bonding disruption. In contrast, a purely linear block co‐polymer system (carboxylic acid terminated poly[lactic‐co‐glycolic acid]) necessitates both electrostatics and hydrogen bonding to assemble with IL and a two‐component electrostatically bound system (electrostatic PEG‐PLGA [EPP]) favors hydrogen‐bonding with electrostatics serving as a secondary role.

离子液体(ILs)是一种很有前途的生物材料，可以通过功能化聚合物纳米颗粒(NPs)来增强药物的传递。尽管它们赋予NPs生物相容性和生物功能，但对于非共价相互作用，特别是氢键和静电相互作用，在多大程度上控制IL - NP超分子组装，人们知之甚少。本文中，我们在合成过程中使用盐(0.1 M硫酸钠)和酸(0.25 M盐酸，pH值为4.8)滴定来破坏四种不同聚合物平台的IL功能化纳米组装。通过定量核磁共振波谱和动态光散射，我们证明了胆碱反式- 2 -己烯酸酯(CA2HA 1:1) IL组装的驱动力随氢键或静电主导而变化，这取决于聚合物平台的结构。特别是，共价结合或支链的50:50嵌段共聚物体系(二嵌段PEG - PLGA [DPP]和聚己内酯[PCl] -聚[氨基胺]胺基线性树枝状嵌段共聚物)主要受到氢键破坏的影响。相比之下，纯线性嵌段共聚物体系(羧酸端接的聚[乳酸- co -乙醇酸])需要静电和氢键才能与IL组装，而双组分静电结合体系(静电PEG - PLGA [EPP])有利于氢键，静电作为次要作用。

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引用次数: 0

Correlation of the electronic structure and Li‐ion mobility with modulus and hardness in LiNi_0.6Co_0.2Mn_0.2O₂ cathodes by combined near edge X‐ray absorption finestructure spectroscopy, atomic force microscopy, and nanoindentation 结合近边X射线吸收精细结构光谱、原子力显微镜和纳米压痕研究LiNi0.6Co0.2Mn0.2O2阴极的电子结构和Li离子迁移率与模量和硬度的关系

Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2023-09-20 DOI: 10.1002/elsa.202300017

Florian Hausen, Niklas Scheer, Bixian Ying, Karin Kleiner

Abstract The electrochemical performance of cathode materials in Li‐ion batteries is reflected in macroscopic observables such as the capacity, the voltage, and the state of charge (SOC). However, the physical origin of performance parameters are atomistic processes that scale up to a macroscopic picture. Thus, revealing the function and failure of electrochemical devices requires a multiscale (and ‐time) approach using spectroscopic and microscopic techniques. In this work, we combine near‐edge X‐ray absorption fine structure spectroscopy (NEXAFS) to determine the chemical binding state of transition metals in LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622), electrochemical strain microscopy to understand the Li‐ion mobility in such materials, and nanoindentation to relate the mechanical properties exhibited by the material to the chemical state and ion mobility. Strikingly, a clear correlation between the chemical binding, the mechanical properties, and the Li‐ion mobility is found. Thereby, the significant relation of chemo‐mechanical properties of NCM622 on a local and global scale is clearly demonstrated.

摘要:锂离子电池正极材料的电化学性能主要反映在容量、电压和荷电状态等宏观观察指标上。然而，性能参数的物理起源是原子过程，可以放大到宏观图像。因此，揭示电化学装置的功能和故障需要使用光谱和微观技术的多尺度(和时间)方法。在这项工作中，我们结合了近边X射线吸收精细结构光谱(NEXAFS)来确定LiNi 0.6 Co 0.2 Mn 0.2 o2 (NCM622)中过渡金属的化学结合状态，电化学应变显微镜来了解这种材料中的锂离子迁移率，以及纳米压痕来将材料所表现出的机械性能与化学状态和离子迁移率联系起来。引人注目的是，发现了化学结合、机械性能和锂离子迁移率之间的明显相关性。因此，NCM622在局部和全局尺度上的化学力学性能的显著关系得到了清楚的证明。

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引用次数: 1

Probing passivity of corroding metals using scanning electrochemical probe microscopy 用扫描电化学探针显微镜探测腐蚀金属的钝化性

IF 2.9 Q2 ELECTROCHEMISTRY

Electrochemical science advances

Pub Date : 2023-08-03 DOI: 10.1002/elsa.202300014

Sebastian Amland Skaanvik, Samantha Michelle Gateman

Passive films are essential for the longevity of metals and alloys in corrosive environments. A great deal of research has been devoted to understanding and characterizing passive films, including their chemical composition, uniformity, thickness, porosity, and conductivity. Many characterization techniques are conducted under vacuum, which do not portray the true in-service environments passive films will endure. Scanning electrochemical probe microscopy (SEPM) techniques have emerged as necessary tools to complement research on characterizing passive films to enable the in situ extraction of passive film parameters and monitoring of local breakdown events of compromised films. Herein, we review the current research efforts using scanning electrochemical microscopy, scanning electrochemical cell microscopy (or droplet cell measurements), and local electrochemical impedance spectroscopy techniques to advance the knowledge of local properties of passivated metals. The future use of SEPM for quantitative extraction of local film characteristics within in-service environments (i.e., with varying pH, solution composition, and applied potential) is promising, which can be correlated to nanostructural and microstructural features of the passive film and underlying metal using complementary microscopy and spectroscopy methods. The outlook on this topic is highlighted, including exciting avenues and challenges of these methods in characterizing advanced alloy systems and protective surface films.

钝化膜对于金属和合金在腐蚀性环境中的寿命至关重要。大量的研究致力于了解和表征钝化膜，包括它们的化学成分、厚度、均匀性、厚度、孔隙率和电导率。许多表征技术都是在真空条件下进行的，这并不能描述被动式薄膜在实际使用环境中所能承受的真实情况。扫描电化学探针显微镜(SEPM)技术已经成为补充钝化膜表征研究的必要工具，能够原位提取钝化膜参数并监测受损膜的局部击穿事件。在此，我们回顾了目前使用扫描电化学显微镜、扫描电化学电池显微镜(或液滴电池测量)和局部电化学阻抗谱技术来推进钝化金属局部性质的研究工作。在使用环境中(即在不同的pH值、溶液组成和应用潜力下)，SEPM用于定量提取局部膜特性的未来是有希望的，这可以通过互补显微镜和光谱学方法与钝化膜和底层金属的纳米结构和微观结构特征相关联。展望了这一主题，包括令人兴奋的途径和挑战，这些方法表征先进的合金系统和保护表面膜。

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引用次数: 0