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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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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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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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Exploration of the oxygen transport behavior in non-precious metal catalyst-based cathode catalyst layer

Shiqu CHEN, Silei XIANG, Zehao TAN, Huiyuan LI, Xiaohui YAN, Jiewei YIN, Shuiyun SHEN, Junliang ZHANG

《能源前沿（英文）》 2023年 第17卷 第1期   页码 123-133 doi: 10.1007/s11708-022-0849-1

摘要： High cost has undoubtedly become the biggest obstacle to the commercialization of proton exchange membrane fuel cells (PEMFCs), in which Pt-based catalysts employed in the cathodic catalyst layer (CCL) account for the major portion of the cost. Although non-precious metal catalysts (NPMCs) show appreciable activity and stability in the oxygen reduction reaction (ORR), the performance of fuel cells based on NPMCs remains unsatisfactory compared to those using Pt-based CCL. Therefore, most studies on NPMC-based fuel cells focus on developing highly active catalysts rather than facilitating oxygen transport. In this work, the oxygen transport behavior in CCLs based on highly active Fe-N-C catalysts is comprehensively explored through the elaborate design of two types of membrane electrode structures, one containing low-Pt-based CCL and NPMC-based dummy catalyst layer (DCL) and the other containing only the NPMC-based CCL. Using Zn-N-C based DCLs of different thickness, the bulk oxygen transport resistance at the unit thickness in NPMC-based CCL was quantified via the limiting current method combined with linear fitting analysis. Then, the local and bulk resistances in NPMC-based CCLs were quantified via the limiting current method and scanning electron microscopy, respectively. Results show that the ratios of local and bulk oxygen transport resistances in NPMC-based CCL are 80% and 20%, respectively, and that an enhancement of local oxygen transport is critical to greatly improve the performance of NPMC-based PEMFCs. Furthermore, the activity of active sites per unit in NPMC-based CCLs was determined to be lower than that in the Pt-based CCL, thus explaining worse cell performance of NPMC-based membrane electrode assemblys (MEAs). It is believed that the development of NPMC-based PEMFCs should proceed not only through the design of catalysts with higher activity but also through the improvement of oxygen transport in the CCL.

关键词： proton exchange membrane fuel cells (PEMFCs)     non-precious metal catalyst (NPMC)     cathode catalyst layer (CCL)     local and bulk oxygen transport resistance    

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Comparative analysis of ceramic-carbonate nanocomposite fuel cells using composite GDC/NLC electrolytewith different perovskite structured cathode materials

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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DOW CORNING 1-2577 Conformal Coating as an efficient diffusion material for cathode in the microbial

Yanping HOU, Haiping LUO, Guangli LIU, Renduo ZHANG, Yong LUO, Bangyu QIN, Shanshan CHEN

《环境科学与工程前沿（英文）》 2013年 第7卷 第4期   页码 526-530 doi: 10.1007/s11783-013-0532-1

摘要： In this study, DOW CORNING 1-2577 Conformal Coating was proposed for the cathode diffusion layer of the microbial fuel cell (MFC). In MFCs, stainless steel mesh cathodes using DOW CORNING 1-2577 Conformal Coating/carbon as the diffusion layer and two poly (dimethylsiloxane) (PDMS)/carbon diffusion layers and carbon cloth cathode with four poly (tetrafluoroethylene) (PTFE) diffusion layers were constructed for comparison. Under the same operational condition, the MFCs with the DOW CORNING 1-2577 Conformal Coating/carbon diffusion layer produced the maximum power density of 1585±52 mW·m , compared with those using poly (tetrafluoroethylene) (PTFE) diffusion layers (1421±45 mW·m ) and poly (dimethylsiloxane) (PDMS)/carbon diffusion layers (1353±49 mW·m ). The DOW CORNING 1-2577 Conformal Coating could be an alternative for the diffusion layer construction in the MFC due to its remarkable performance and much simple construction procedure.

关键词： microbial fuel cell     diffusion layer     power density     DOW CORNING1-2577 Conformal Coating    

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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）》 2023年 第17卷 第10期   页码 1354-1371 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）》 2023年 第17卷 第9期   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-Nx and Zn-Nx 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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Mapping the trends and prospects of battery cathode materials based on patent landscape

《能源前沿（英文）》   页码 822-832 doi: 10.1007/s11708-023-0900-x

摘要： Advancing portable electronics and electric vehicles is heavily dependent on the cutting-edge lithium-ion (Li-ion) battery technology, which is closely linked to the properties of cathode materials. Identifying trends and prospects of cathode materials based on patent analysis is considered a kernel to optimize and refine battery related markets. In this paper, a patent analysis is performed on 6 popular cathode materials by comprehensively considering performance comparison, development trend, annual installed capacity, technology life cycle, and distribution among regions and patent assignees. In the technology life cycle, the cathode materials majorly used in electric vehicle have entered maturity stage, while the lithium cobalt oxide (LCO) cathode that is widely used in portable electronics is still in the growth stage. In global patent distributions, China holds more than 50% of total patents. In the top 10 patent assignees of 6 cathode materials, 2 institutes are from China with the rest being Japan (6) and Republic of Korea (2), indicating that the technology of cathode materials in China is relatively scattered while cathode research is highly concentrated in Japan and Republic of Korea. Moreover, the patent distribution has to consider practical issues as well as the impacts of core patents. For example, the high cost discourages the intention of applying international patents. This paper is expected to stimulate battery research, understand technical layout of various countries, and probably forecast innovative technology breakthroughs.

关键词： patent analysis     cathode     batteries     technology life cycle    

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Fabrication of layered structure VS anchor in 3D graphene aerogels as a new cathode material for lithium

《能源前沿（英文）》 2019年 第13卷 第3期   页码 597-602 doi: doi:10.1007/s11708-018-0576-9

摘要： VS4 has gained more and more attention for its high theoretical capacity (449 mAh/g with 3e− transfer) in lithium ion batteries (LIBs). Herein, a layered structure VS4 anchored in graphene aerogels is prepared and first reported as cathode material for LIBs. VS4@GAs composite exhibits an exceptional high initial reversible capacity (511 mAh/g), an excellent high-rate capability (191 mAh/g at the 5 C), and an excellent cyclic stability (239 mAh/g after 15 cycles).

关键词： VS4     graphene aerogels     cathode     lithium storage    

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Recent advances in cathode electrocatalysts for PEM fuel cells

Junliang ZHANG

《能源前沿（英文）》 2011年 第5卷 第2期   页码 137-148 doi: 10.1007/s11708-011-0153-y

摘要： Great progress has been made in the past two decades in the development of the electrocatalysts for proton exchange membrane fuel cells (PEMFCs). This review article is focused on recent advances made in the kinetic-activity improvement on platinum- (Pt-) based cathode electrocatalysts for the oxygen reduction reaction (ORR). The origin of the limited ORR activity of Pt catalysts is discussed, followed by a review on the development of Pt alloy catalysts, Pt monolayer catalysts, and shape- and facet-controlled Pt-alloy nanocrystal catalysts. Mechanistic understanding is reviewed as well on the factors contributing to the enhanced ORR activity of these catalysts. Finally, future directions for PEMFC catalyst research are proposed.

关键词： proton exchange membrane fuel cells (PEMFCs)     cathode electrocatalysts     platinum     oxygen reduction reaction (ORR)    

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Current challenge and perspective of PGM-free cathode catalysts for PEM fuel cells

Gang WU

《能源前沿（英文）》 2017年 第11卷 第3期   页码 286-298 doi: 10.1007/s11708-017-0477-3

摘要： To significantly reduce the cost of proton exchange membrane fuel cells, platinum-group metal (PGM)-free cathode catalysts are highly desirable. Current M-N-C (M: Fe, Co or Mn) catalysts are considered the most promising due to their encouraging performance. The challenge thus has been their stability under acidic conditions, which has hindered their use for any practical applications. In this review, based on the author’s research experience in the field for more than 10 years, current challenges and possible solutions to overcome these problems were discussed. The current Edisonian approach (i.e., trial and error) to developing PGM-free catalysts has been ineffective in achieving revolutionary breakthroughs. Novel synthesis techniques based on a more methodological approach will enable atomic control and allow us to achieve optimal electronic and geometric structures for active sites uniformly dispersed within the 3D architectures. Structural and chemical controlled precursors such as metal-organic frameworks are highly desirable for making catalysts with an increased density of active sites and strengthening local bonding structures among N, C and metals. Advanced electrochemical and physical characterization, such as electron microscopy and X-ray absorption spectroscopy should be combined with first principle density functional theory (DFT) calculations to fully elucidate the active site structures.

关键词： oxygen reduction     fuel cells     cathode     nonprecious metal catalysts     carbon nanocomposites    

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Effects of bicarbonate and cathode potential on hydrogen production in a biocathode electrolysis cell

Dawei LIANG,Yanyan LIU,Sikan PENG,Fei LAN,Shanfu LU,Yan XIANG

《环境科学与工程前沿（英文）》 2014年 第8卷 第4期   页码 624-630 doi: 10.1007/s11783-013-0584-2

摘要： A biocathode with microbial catalyst in place of a noble metal was successfully developed for hydrogen evolution in a microbial electrolysis cell (MEC). The strategy for fast biocathode cultivation was demonstrated. An exoelectrogenic reaction was initially extended with an H -full atmosphere to enrich H -utilizing bacteria in a MEC bioanode. This bioanode was then inversely polarized with an applied voltage in a half-cell to enrich the hydrogen-evolving biocathode. The electrocatalytic hydrogen evolution reaction (HER) kinetics of the biocathode MEC could be enhanced by increasing the bicarbonate buffer concentration from 0.05 mol·L to 0.5 mol·L and/or by decreasing the cathode potential from -0.9 V to -1.3 V vs. a saturated calomel electrode (SCE). Within the tested potential region in this study, the HER rate of the biocathode MEC was primarily influenced by the microbial catalytic capability. In addition, increasing bicarbonate concentration enhances the electric migration rate of proton carriers. As a consequence, more mass H can be released to accelerate the biocathode-catalyzed HER rate. A hydrogen production rate of 8.44 m ·m ·d with a current density of 951.6 A·m was obtained using the biocathode MEC under a cathode potential of -1.3 V vs. SCE and 0.4 mol·L bicarbonate. This study provided information on the optimization of hydrogen production in biocathode MEC and expanded the practical applications thereof.

关键词： microbial electrolysis cell (MEC)     biocathode     hydrogen production     bicarbonate     cathode potential    

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Effect of current density on groundwater arsenite removal performance using air cathode electrocoagulation

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1399-1

摘要：

• With the same charge, current density had little effect on As(III) removal in ACEC.

关键词： Electrocoagulation     Air cathode     Arsenic     Current density     Energy consumption    

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Effect of interface adhesion factor on the bearing capacity of strip footing placed on cohesive soil

《结构与土木工程前沿（英文）》 2021年 第15卷 第6期   页码 1494-1503 doi: 10.1007/s11709-021-0768-y

摘要： The problem related to bearing capacity of footing either on pure soil or on pure rock mass has been investigated over the years. Currently, no study deals with the bearing capacity of strip footing on a cohesive soil layer overlying rock mass. Therefore, by implementing the lower bound finite element limit analysis in conjunction with the second-order cone programming and the power cone programming, the ultimate bearing capacity of a strip footing located on a cohesive soil overlying rock mass is determined in this study. By considering the different values of interface adhesion factor (αcr) between the cohesive soil and rock mass, the ultimate bearing capacity of strip footing is expressed in terms of influence factor (If) for different values of cohesive soil layer cover ratio (Tcs/B). The failure of cohesive soil is modeled by using Mohr−Coulomb yield criterion, whereas Generalized Hoek−Brown yield criterion is utilized to model the rock mass at failure. The variations ofIf with different magnitudes of αcr are studied by considering the influence of the rock mass strength parameters of beneath rock mass layer. To examine stress distribution at different depths, failure patterns are also plotted.

关键词： bearing capacity     soil-rock interface     Hoek−Brown yield criterion     plasticity     limit analysis    

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标题 作者 时间 类型 操作

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

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

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

Exploration of the oxygen transport behavior in non-precious metal catalyst-based cathode catalyst layer

Shiqu CHEN, Silei XIANG, Zehao TAN, Huiyuan LI, Xiaohui YAN, Jiewei YIN, Shuiyun SHEN, Junliang ZHANG

期刊论文

Comparative analysis of ceramic-carbonate nanocomposite fuel cells using composite GDC/NLC electrolytewith different perovskite structured cathode materials

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

期刊论文

DOW CORNING 1-2577 Conformal Coating as an efficient diffusion material for cathode in the microbial

Yanping HOU, Haiping LUO, Guangli LIU, Renduo ZHANG, Yong LUO, Bangyu QIN, Shanshan CHEN

期刊论文

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

Mapping the trends and prospects of battery cathode materials based on patent landscape

期刊论文

Fabrication of layered structure VS anchor in 3D graphene aerogels as a new cathode material for lithium

期刊论文

Recent advances in cathode electrocatalysts for PEM fuel cells

Junliang ZHANG

期刊论文

Current challenge and perspective of PGM-free cathode catalysts for PEM fuel cells

Gang WU

期刊论文

Effects of bicarbonate and cathode potential on hydrogen production in a biocathode electrolysis cell

Dawei LIANG,Yanyan LIU,Sikan PENG,Fei LAN,Shanfu LU,Yan XIANG

期刊论文

Effect of current density on groundwater arsenite removal performance using air cathode electrocoagulation

期刊论文

Effect of interface adhesion factor on the bearing capacity of strip footing placed on cohesive soil

期刊论文