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Localized high-concentration electrolytes for lithium metal batteries: progress and prospect

《化学科学与工程前沿（英文）》 doi: 10.1007/s11705-022-2286-4

摘要： With the increasing development of digital devices and electric vehicles, high energy-density rechargeable batteries are strongly required. As one of the most promising anode materials with an ultrahigh specific capacity and extremely low electrode potential, lithium metal is greatly considered an ideal candidate for next-generation battery systems. Nevertheless, limited Coulombic efficiency and potential safety risks severely hinder the practical applications of lithium metal batteries due to the inevitable growth of lithium dendrites and poor interface stability. Tremendous efforts have been explored to address these challenges, mainly focusing on the design of novel electrolytes. Here, we provide an overview of the recent developments of localized high-concentration electrolytes in lithium metal batteries. Firstly, the solvation structures and physicochemical properties of localized high-concentration electrolytes are analyzed. Then, the developments of localized high-concentration electrolytes to suppress the formation of dendritic lithium, broaden the voltage window of electrolytes, enhance safety, and render low-temperature operation for robust lithium metal batteries are discussed. Lastly, the remaining challenges and further possible research directions for localized high-concentration electrolytes are outlined, which can promisingly render the practical applications of lithium metal batteries.

关键词： high-concentration electrolyte localized high-concentration electrolyte lithium metal battery solid electrolyte interphase dendrite

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Boosting the direct conversion of NHHCO electrolyte to syngas on Ag/Zn zeolitic imidazolate framework

《化学科学与工程前沿（英文）》页码 1196-1207 doi: 10.1007/s11705-022-2289-1

摘要： The electrochemical reduction of NH₄HCO₃ to syngas can bypass the high energy consumption of high-purity CO₂ release and compression after the ammonia-based CO₂ capture process. This technology has broad prospects in industrial applications and carbon neutrality. A zeolitic imidazolate framework-8 precursor was introduced with different Ag contents via colloid chemical synthesis. This material was carbonized at 1000 °C to obtain AgZn zeolitic imidazolate framework derived nitrogen carbon catalysts, which were used for the first time for boosting the direct conversion of NH₄HCO₃ electrolyte to syngas. The AgZn zeolitic imidazolate framework derived nitrogen carbon catalyst with a Ag/Zn ratio of 0.5:1 achieved the highest CO Faradaic efficiency of 52.0% with a current density of 1.15 mA·cm^–2 at –0.5 V, a H₂/CO ratio of 1–2 (–0.5 to –0.7 V), and a stable catalytic activity of more than 6 h. Its activity is comparable to that of the CO₂-saturated NH₄HCO₃ electrolyte. The highly discrete Ag-N_x and Zn-N_x nodes may have combined catalytic effects in the catalysts synthesized by appropriate Ag doping and sufficient carbonization. These nodes could increase active sites of catalysts, which is conducive to the transport and adsorption of reactant CO₂ and the stability of *COOH intermediate, thus can improve the selectivity and catalytic activity of CO.

关键词： Ag catalyst zeolitic imidazolate framework CO₂ electroreduction ammonium bicarbonate electrolyte syngas

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A review on the development of electrolytes for lithium-based batteries for low temperature applications

《能源前沿（英文）》 2023年第17卷第1期页码 43-71 doi: 10.1007/s11708-022-0853-5

摘要： The aerospace industry relies heavily on lithium-ion batteries in instrumentation such as satellites and land rovers. This equipment is exposed to extremely low temperatures in space or on the Martian surface. The extremely low temperatures affect the discharge characteristics of the battery and decrease its available working capacity. Various solvents, cosolvents, additives, and salts have been researched to fine tune the conductivity, solvation, and solid-electrolyte interface forming properties of the electrolytes. Several different resistive phenomena have been investigated to precisely determine the most limiting steps during charge and discharge at low temperatures. Longer mission lifespans as well as self-reliance on the chemistry are now highly desirable to allow low temperature performance rather than rely on external heating components. As Martian rovers are equipped with greater instrumentation and demands for greater energy storage rise, new materials also need to be adopted involving next generation lithium-ion chemistry to increase available capacity. With these objectives in mind, tailoring of the electrolyte with higher-capacity materials such as lithium metal and silicon anodes at low temperatures is of high priority. This review paper highlights the progression of electrolyte research for low temperature performance of lithium-ion batteries over the previous several decades.

关键词： electrolyte lithium-ion low temperature aerospace solid-electrolyte interface

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Recent advances toward high voltage, EC-free electrolytes for graphite-based Li-ion battery

Tong Zhang, Elie Paillard

《化学科学与工程前沿（英文）》 2018年第12卷第3期页码 577-591 doi: 10.1007/s11705-018-1758-z

摘要：

Lithium-ion batteries are a key technology in today’s world and improving their performances requires, in many cases, the use of cathodes operating above the anodic stability of state-of-the-art electrolytes based on ethylene carbonate (EC) mixtures. EC, however, is a crucial component of electrolytes, due to its excellent ability to allow graphite anode operation–also required for high energy density batteries–by stabilizing the electrode/electrolyte interface. In the last years, many alternative electrolytes, aiming at allowing high voltage battery operation, have been proposed. However, often, graphite electrode operation is not well demonstrated in these electrolytes. Thus, we review here the high voltage, EC-free alternative electrolytes, focusing on those allowing the steady operation of graphite anodes. This review covers electrolyte compositions, with the widespread use of additives, the change in main lithium salt, the effect of anion (or Li salt) concentration, but also reports on graphite protection strategies, by coatings or artificial solid electrolyte interphase (SEI) or by use of water-soluble binder for electrode processing as these can also enable the use of graphite in electrolytes with suboptimal intrinsic SEI formation ability.

关键词： lithium-ion electrolyte solid electrolyte interphase additives high voltage graphite

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Effect of electrolyte concentration on the tribological performance of MAO coatings on aluminum alloys

Chao Wang, Jun Chen, Jihua He, Jing Jiang, Qinyong Zhang

《化学科学与工程前沿（英文）》 2020年第14卷第6期页码 1065-1071 doi: 10.1007/s11705-019-1909-x

摘要： Micro-arc oxidation (MAO) is an efficient approach to improve the hardness, wear resistance, and other properties of aluminum alloys. In order to investigate the effect of the electrolyte concentration on the properties of MAO coatings for LY12 alloy, the voltage variation during the MAO process was recorded. The surface morphologies and phase compositions of the coatings produced with different electrolytes were investigated using scanning electron microscopy and X-ray diffraction, respectively. The roughness and thickness of the coatings were measured using a pocket roughness meter and an eddy-current thickness meter, respectively. The tribological performances of the coatings were investigated against GCr15 bearing steel on a ball-on-disc wear tester in open air. The results showed that with an increase in the Na SiO content, the working voltage of the MAO process decreased, the roughness and thickness of the coatings increased significantly, and the relative content of the -Al O phase decreased. With an increase in the KOH content, the working voltage decreased slightly, the roughness and thickness of the coatings increased slightly, and the α- and -Al O phase contents remained unchanged. The friction coefficient and wear rate of the coatings increased with an increase in the Na SiO and KOH concentrations. A decrease in the porosity and roughness and an increase in the α-Al O content of the coatings reduced their wear mass loss.

关键词： aluminum alloy micro-arc oxidation coating electrolyte concentration tribological performance

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Review of characterization and modeling of polymer electrolyte fuel cell catalyst layer: The blessing

Jun HUANG, Zhe LI, Jianbo ZHANG

《能源前沿（英文）》 2017年第11卷第3期页码 334-364 doi: 10.1007/s11708-017-0490-6

摘要： Ionomer impregnation represents a milestone in the evolution of polymer electrolyte fuel cell (PEFC) catalyst layers. Ionomer acts as the binder, facilitates proton transport, and thereby drastically improves catalyst utilization and effectiveness. However, advanced morphological and functional characterizations have revealed that up to 60% of Pt nanoparticles can be trapped in the micropores of carbon support particles. Ionomer clusters and oxygen molecules can hardly enter into micropores, leading to low Pt utilization and effectiveness. Moreover, the ionomer thin-films covering Pt nanoparticles can cause significant mass transport loss especially at high current densities. Ionomer-free ultra-thin catalyst layers (UTCLs) emerge as a promising alternative to reduce Pt loading by improving catalyst utilization and effectiveness, while theoretical issues such as the proton conduction mechanism remain puzzling and practical issues such as the rather narrow operation window remain unsettled. At present, the development of PEFC catalyst layer has come to a crossroads: staying ionomer-impregnated or going ionomer-free. It is always beneficial to look back into the past when coming to a crossroads. This paper addresses the characterization and modeling of both the conventional ionomer-impregnated catalyst layer and the emerging ionomer-free UTCLs, featuring advances in characterizing microscale distributions of Pt particles, ionomer, support particles and unraveling their interactions; advances in fundamental understandings of proton conduction and flooding behaviors in ionomer-free UTCLs; advances in modeling of conventional catalyst layers and especially UTCLs; and discussions on high-impact research topics in characterizing and modeling of catalyst layers.

关键词： polymer electrolyte fuel cell ultra-thin catalyst layer electrostatic interactions characterization and modeling structure-property-performance relation water management

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Characterization and comparison of organic functional groups effects on electrolyte performance for vanadium

《化学科学与工程前沿（英文）》页码 1221-1230 doi: 10.1007/s11705-023-2298-8

摘要： The vanadium redox flow battery with a safe and capacity-controllable large-scale energy storage system offers a new method for the sustainability. In this case, acetic acid, methane sulfonic acid, sulfonic acid, amino methane sulfonic acid, and taurine are used to overcome the low electrolyte energy density and stability limitations, as well as to investigate the effects of various organic functional groups on the vanadium redox flow battery. When compared to the pristine electrolyte (0.22 Ah, 5.0 Wh·L^–1, 85.0%), the results show that taurine has the advantage of maintaining vanadium ion concentrations, discharge capacity (1.43 Ah), energy density (33.9 Wh·L^–1), and energy efficiency (90.5%) even after several cycles. The acetic acid electrolyte is more conducive to the low-temperature stability of the V(II) electrolyte (177 h at −25 °C) than pristine (82 h at −2 °C). The –SO₃H group, specifically the coaction of the –NH₂ and –SO₃H groups, improves electrolyte stability. The –NH₂ and –COOH additive groups improved conductivity and electrochemical activity.

关键词： vanadium redox flow battery functional groups organic additives energy density stability

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低温固体氧化物燃料电池的复合电解质材料

谢富丞,王诚,毛宗强

《中国工程科学》 2013年第15卷第2期页码 72-76

摘要：

固体氧化物燃料电池（SOFC）是一种高效、环保的发电装置。低温化是SOFC的主要发展方向。探索适合在低温（400~600 ℃）条件下操作的高性能电解质材料是SOFC低温化发展的关键。近年来，研究人员发展了新型的复合电解质材料，取得了较好的成果。本文综述了近年来低温SOFC复合电解质材料的研究进展，简要介绍了复合电解质材料的特点、类型和传导机理。

关键词：低温SOFC 复合电解质传导机理

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Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganese

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

《能源前沿（英文）》 2017年第11卷第3期页码 365-373 doi: 10.1007/s11708-017-0500-8

摘要： Lithium manganese oxide (LiMn O ) is a principal cathode material for high power and high energy density electrochemical storage on account of its low cost, non-toxicity, and ease of preparation relative to other cathode materials. However, there are well-documented problems with capacity fade of lithium ion batteries containing LiMn O . Experimental observations indicate that the manganese content of the electrolyte increases as an electrochemical cell containing LiMn O ages, suggesting that active material loss by dissolution of divalent manganese from the LiMn O surface is the primary reason for reduced cell life in LiMn O batteries. To improve the retention of manganese in the active material, it is key to understand the reactions that occur at the cathode surface. Although a thin layer of electrolyte decomposition products is known to form at the cathode surface, the speciation and reaction mechanisms of Mn in this interface layer are not yet well understood. To bridge this knowledge gap, reactive force field (ReaxFF) based molecular dynamics was applied to investigate the reactions occurring at the LiMn O cathode surface and the mechanisms that lead to manganese dissolution. The ReaxFFMD simulations reveal that the cathode-electrolyte interface layer is composed of oxidation products of electrolyte solvent molecules including aldehydes, esters, alcohols, polycarbonates, and organic radicals. The oxidation reaction pathways for the electrolyte solvent molecules involve the formation of surface hydroxyl species that react with exposed manganese atoms on the cathode surface. The presence of hydrogen fluoride (HF) induces formation of inorganic metal fluorides and surface hydroxyl species. Reaction products predicted by ReaxFF-based MD are in agreement with experimentally identified cathode-electrolyte interface compounds. An overall cathode-electrolyte interface reaction scheme is proposed based on the molecular simulation results.

关键词： lithium manganese oxide batteries reactive force field (ReaxFF) cathode-electrolyte interface layer molecular dynamics

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固体氧化物燃料电池的电解质及电极材料的电导率研究方法

贺贝贝,潘鑫,夏长荣

《中国工程科学》 2013年第15卷第2期页码 57-65

摘要：

论述了晶体材料，重点是固体氧化物燃料电池组件的导电机理，介绍了影响电导率的几个因素。针对不同的电解质和电极材料，讨论了几种常用的测量电解质和电极总电导率、电子电导率以及离子电导率的方法，并指出在测量中需要注意的问题。

关键词：导电机理电解质电极电导率固体氧化物燃料电池

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synthesis of double-shell truncated octahedral Pt-Ni alloys for oxygen reduction reaction of polymer electrolyte

Xiashuang LUO, Yangge GUO, Hongru ZHOU, Huan REN, Shuiyun SHEN, Guanghua WEI, Junliang ZHANG

《能源前沿（英文）》 2020年第14卷第4期页码 767-777 doi: 10.1007/s11708-020-0667-2

摘要： Shape-controlled Pt-Ni alloys usually offer an exceptional electrocatalytic activity toward the oxygen reduction reaction (ORR) of polymer electrolyte membrane fuel cells (PEMFCs), whose tricks lie in well-designed structures and surface morphologies. In this paper, a novel synthesis of truncated octahedral PtNi alloy catalysts that consist of homogeneous Pt-Ni alloy cores enclosed by NiO-Pt double shells through thermally annealing defective heterogeneous PtNi alloys is reported. By tracking the evolution of both compositions and morphologies, the outward segregation of both PtO and NiO are first observed in Pt-Ni alloys. It is speculated that the diffusion of low-coordination atoms results in the formation of an energetically favorable truncated octahedron while the outward segregation of oxides leads to the formation of NiO-Pt double shells. It is very attractive that after gently removing the NiO outer shell, the dealloyed truncated octahedral core-shell structure demonstrates a greatly enhanced ORR activity. The as-obtained truncated octahedral Pt Ni core-shell alloy presents a 3.4-folds mass-specific activity of that for unannealed sample, and its activity preserves 45.4% after 30000 potential cycles of accelerated degradation test (ADT). The peak power density of the dealloyed truncated octahedral Pt Ni core-shell alloy catalyst based membrane electrolyte assembly (MEA) reaches 679.8 mW/cm , increased by 138.4 mW/cm relative to that based on commercial Pt/C.

关键词： dealloyed Pt-Ni alloys truncated octahedron double-shell thermal annealing oxygen reduction reaction (ORR)

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低温固体氧化物燃料电池电解质材料

韩达,吴天植,辛显双,王绍荣,占忠亮

《中国工程科学》 2013年第15卷第2期页码 66-71

摘要：

低温化是固体氧化物燃料电池（SOFC）发电技术的重要发展趋势。SOFC工作温度的降低不仅可极大地降低材料及制备成本，更重要的是可极大地提高其长期运行的稳定性。电解质是SOFC的核心部件，可以采用电解质薄膜化或新型电解质材料来降低SOFC的工作温度。本文概述了目前被广泛研究的低温SOFC的电解质材料，并从其结构及性能出发，重点阐述了它们各自的优点和局限性。

关键词：低温SOFC 新型电解质离子电导率

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Comparative analysis of ceramic-carbonate nanocomposite fuel cells using composite GDC/NLC electrolyte

Muhammad I. Asghar, Sakari Lepikko, Janne Patakangas, Janne Halme, Peter D. Lund

《化学科学与工程前沿（英文）》 2018年第12卷第1期页码 162-173 doi: 10.1007/s11705-017-1642-2

摘要： A comparative analysis of perovskite structured cathode materials, La Sr MnO (LSM), La Sr CoO (LSC), La Sr FeO (LSF) and La Sr Co Fe O (LSCF), was performed for a ceramic-carbonate nanocomposite fuel cell using composite electrolyte consisting of Gd Ce O (GDC) and a eutectic mixture of Na CO and Li CO . The compatibility of these nanocomposite electrode powder materials was investigated under air, CO and air/CO atmospheres at 550 °C. Microscopy measurements together with energy dispersive X-ray spectroscopy (EDS) elementary analysis revealed few spots with higher counts of manganese relative to lanthanum and strontium under pure CO atmosphere. Furthermore, electrochemical impedance (EIS) analysis showed that LSC had the lowest resistance to oxygen reduction reaction (ORR) (14.12 Ω·cm ) followed by LSF (15.23 Ω·cm ), LSCF (19.38 Ω·cm ) and LSM (>300 Ω·cm ). In addition, low frequency EIS measurements (down to 50 µHz) revealed two additional semi-circles at frequencies around 1 Hz. These semicircles can yield additional information about electrochemical reactions in the device. Finally, a fuel cell was fabricated using GDC/NLC nanocomposite electrolyte and its composite with NiO and LSCF as anode and cathode, respectively. The cell produced an excellent power density of 1.06 W/cm at 550 °C under fuel cell conditions.

关键词： electrode fuel cell low-temperature nanocomposite perovskite

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Fabrication and performance of PEN SOFCs with proton-conducting electrolyte

ZHONG Li, LUO Jingli, Karl Chuang

《化学科学与工程前沿（英文）》 2007年第1卷第1期页码 40-44 doi: 10.1007/s11705-007-0008-6

摘要： A positive-electrolyte-negative (PEN) assembly solid oxide fuel cell (SOFC) with a thin electrolyte film for intermediate temperature operation was fabricated. Instead of the traditional screen-printing method, both anode and cathode catalysts were pressed simultaneously and formed with the fabrication of nano-composite electrolyte by press method. This design offered some advantageous configurations that diminished ohmic resistance between electrolyte and electrodes. It also increased the proton-conducting rate and improved the performance of SOFC due to the reduction of membrane thickness and good contact between electrolyte and electrodes. The fabricated PEN cell generated electricity between 600?C and 680?C using HS as fuel feed and air as oxidant. Maximum power densities 40 mW " cm and 130 mW " cm for the PEN configuration with a Mo-Ni-S-based composite anode, nano-composite electrolyte (LiSO+AlO) film and a NiO-based composite cathode were achieved at 600?C and 680?C, respectively.

关键词： proton-conducting positive-electrolyte-negative temperature operation Mo-Ni-S-based composite advantageous

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Modeling the methyldiethanolamine-piperazine scrubbing system for CO

Stefania Moioli,Laura A. Pellegrini

《化学科学与工程前沿（英文）》 2016年第10卷第1期页码 162-175 doi: 10.1007/s11705-016-1555-5

摘要： Aqueous solutions of methyldiethanolamine (MDEA) and piperazine (PZ) are commonly used solvent nowadays. In this work a thermodynamic analysis with the Electrolyte-NRTL model has been performed for systems composed of acidic gases and MDEA+PZ aqueous solution. ASPEN Plus has been used for thermodynamic modeling. Values of binary interaction parameters for liquid phase activity coefficients have been estimated from regressions of experimental data. Moreover, the influence of the interactions between ion pairs and MDEA or PZ molecular species has been analyzed. The final aim is to obtain a reliable tool for design and simulation of absorption and stripping columns, fundamentals also in order to carry out energy saving studies.

关键词： vapor-liquid equilibrium methyldietanolamine piperazine regression Electrolyte-NRTL

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标题作者时间类型操作

Localized high-concentration electrolytes for lithium metal batteries: progress and prospect

期刊论文

Boosting the direct conversion of NHHCO electrolyte to syngas on Ag/Zn zeolitic imidazolate framework

期刊论文

A review on the development of electrolytes for lithium-based batteries for low temperature applications

期刊论文

Recent advances toward high voltage, EC-free electrolytes for graphite-based Li-ion battery

Tong Zhang, Elie Paillard

期刊论文

Effect of electrolyte concentration on the tribological performance of MAO coatings on aluminum alloys

Chao Wang, Jun Chen, Jihua He, Jing Jiang, Qinyong Zhang

期刊论文

Review of characterization and modeling of polymer electrolyte fuel cell catalyst layer: The blessing

Jun HUANG, Zhe LI, Jianbo ZHANG

期刊论文

Characterization and comparison of organic functional groups effects on electrolyte performance for vanadium

期刊论文

低温固体氧化物燃料电池的复合电解质材料

谢富丞,王诚,毛宗强

期刊论文

Chemical composition and formation mechanisms in the cathode-electrolyte interface layer of lithium manganese

Sahithya REDDIVARI, Christian LASTOSKIE, Ruofei WU, Junliang ZHANG

期刊论文

固体氧化物燃料电池的电解质及电极材料的电导率研究方法

贺贝贝,潘鑫,夏长荣

期刊论文

synthesis of double-shell truncated octahedral Pt-Ni alloys for oxygen reduction reaction of polymer electrolyte

Xiashuang LUO, Yangge GUO, Hongru ZHOU, Huan REN, Shuiyun SHEN, Guanghua WEI, Junliang ZHANG

期刊论文

低温固体氧化物燃料电池电解质材料

韩达,吴天植,辛显双,王绍荣,占忠亮

期刊论文

Comparative analysis of ceramic-carbonate nanocomposite fuel cells using composite GDC/NLC electrolyte

Muhammad I. Asghar, Sakari Lepikko, Janne Patakangas, Janne Halme, Peter D. Lund

期刊论文

Fabrication and performance of PEN SOFCs with proton-conducting electrolyte

ZHONG Li, LUO Jingli, Karl Chuang

期刊论文

Modeling the methyldiethanolamine-piperazine scrubbing system for CO

Stefania Moioli,Laura A. Pellegrini

期刊论文

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