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A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Energy Materials".

Deadline for manuscript submissions: closed (31 December 2019) | Viewed by 49051

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Prof. Dr. Zhaoyang Fan

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School of Electrical, Computer and Energy Engineering, Arizona State University, Tempe, AZ 85287-5706, USA
Interests: semiconductor materials; electronic devices; nanomaterials; energy storage
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Dr. Shiqi Li

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College of Electronic Information, Hangzhou Dianzi University, Hangzhou 310018, China
Interests: lithium–sulfur batteries; lithium-ion batteries; supercapacitors; microwave chemistry
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Dear Colleagues,

Electrochemical energy storage and conversion systems are becoming essential for electrified transportation, integration of intermittent renewable energy into grids, non-fossil and green fuel production, and many other energy or power applications. The electrode materials and structures, in addition to the liquid or solid electrolytes, play key roles in supporting a multitude of coupled physicochemical processes that include electronic, ionic, and diffusive transport in electrode and electrolyte phases, electrochemical reactions and material phase changes, as well as mechanical and thermal stresses, thus determining the storage energy density and power density, conversion efficiency, performance lifetime, and system cost and safety. Different material chemistries and multiscale porous structures are being investigated towards high performance and low cost. The aim of this Special Issue is to report recent advances related to materials used either in electrochemical energy storage, which encompasses supercapacitors and Li ion, Na ion, or other rechargeable batteries, or in electrochemical energy conversion, which includes electrocatalysts, green fuel production, fuel cells, etc. We are confident that publication of such a Special Issue will stimulate the imagination of researchers to develop advanced materials to further enhance the performance of electrochemical energy devices and put forward their practical application.

It is our pleasure to invite you to submit a manuscript reporting novel materials and structures, their electrochemical behaviors, fundamental mechanisms, novel device concepts, as well as other related topics for this Special Issue. Full papers, communications, and reviews are all welcome.

Prof. Zhaoyang Fan
Assoc. Prof. Shiqi Li
Guest Editors

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Keywords

rechargable betteries
supercapacitors
fuel cells
electrocatalyst
electrode materials
nanostructure
electrochemical energy
energy storage
energy conversion

Published Papers (13 papers)

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Editorial

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4 pages, 177 KiB

Open AccessEditorial

Special Issue: Advances in Electrochemical Energy Materials

by Shiqi Li and Zhaoyang Fan

Materials 2020, 13(4), 844; https://doi.org/10.3390/ma13040844 - 13 Feb 2020

Cited by 2 | Viewed by 2064

Abstract

Electrochemical energy storage is becoming essential for portable electronics, electrified transportation, integration of intermittent renewable energy into grids, and many other energy or power applications. The electrode materials and their structures, in addition to the electrolytes, play key roles in supporting a multitude of coupled physicochemical processes that include electronic, ionic, and diffusive transport in electrode and electrolyte phases, electrochemical reactions and material phase changes, as well as mechanical and thermal stresses, thus determining the storage energy density and power density, conversion efficiency, performance lifetime, and system cost and safety. Different material chemistries and multiscale porous structures are being investigated for high performance and low cost. The aim of this Special Issue is to report the recent advances of materials used in electrochemical energy storage that encompasses supercapacitors and rechargeable batteries. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

Research

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11 pages, 4104 KiB

Open AccessArticle

Submicron-Sized Nb-Doped Lithium Garnet for High Ionic Conductivity Solid Electrolyte and Performance of Quasi-Solid-State Lithium Battery

by Yan Ji, Cankai Zhou, Feng Lin, Bingjing Li, Feifan Yang, Huali Zhu, Junfei Duan and Zhaoyong Chen

Materials 2020, 13(3), 560; https://doi.org/10.3390/ma13030560 - 24 Jan 2020

Cited by 46 | Viewed by 4746

Abstract

The garnet Li₇La₃Zr₂O₁₂ (LLZO) has been widely investigated because of its high conductivity, wide electrochemical window, and chemical stability with regards to lithium metal. However, the usual preparation process of LLZO requires high-temperature sintering for a long time and a lot of mother powder to compensate for lithium evaporation. In this study submicron Li_6.6La₃Zr_1.6Nb_0.4O₁₂ (LLZNO) powder―which has a stable cubic phase and high sintering activity―was prepared using the conventional solid-state reaction and the attrition milling process, and Li stoichiometric LLZNO ceramics were obtained by sintering this powder―which is difficult to control under high sintering temperatures and when sintered for a long time―at a relatively low temperature or for a short amount of time. The particle-size distribution, phase structure, microstructure, distribution of elements, total ionic conductivity, relative density, and activation energy of the submicron LLZNO powder and the LLZNO ceramics were tested and analyzed using laser diffraction particle-size analyzer (LD), X-Ray Diffraction (XRD), Scanning Electron Microscope (SEM), Electrochemical Impedance Spectroscopy (EIS), and the Archimedean method. The total ionic conductivity of samples sintered at 1200 °C for 30 min was 5.09 × 10⁻⁴ S·cm⁻¹, the activation energy was 0.311 eV, and the relative density was 87.3%. When the samples were sintered at 1150 °C for 60 min the total ionic conductivity was 3.49 × 10⁻⁴ S·cm⁻¹, the activation energy was 0.316 eV, and the relative density was 90.4%. At the same time, quasi-solid-state batteries were assembled with LiMn₂O₄ as the positive electrode and submicron LLZNO powder as the solid-state electrolyte. After 50 cycles, the discharge specific capacity was 105.5 mAh/g and the columbic efficiency was above 95%. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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12 pages, 7452 KiB

Open AccessArticle

High-Performance Lithium-Rich Layered Oxide Material: Effects of Preparation Methods on Microstructure and Electrochemical Properties

by Qiming Liu, Huali Zhu, Jun Liu, Xiongwei Liao, Zhuolin Tang, Cankai Zhou, Mengming Yuan, Junfei Duan, Lingjun Li and Zhaoyong Chen

Materials 2020, 13(2), 334; https://doi.org/10.3390/ma13020334 - 11 Jan 2020

Cited by 25 | Viewed by 3473

Abstract

Lithium-rich layered oxide is one of the most promising candidates for the next-generation cathode materials of high-energy-density lithium ion batteries because of its high discharge capacity. However, it has the disadvantages of uneven composition, voltage decay, and poor rate capacity, which are closely related to the preparation method. Here, 0.5Li₂MnO₃·0.5LiMn_0.8Ni_0.1Co_0.1O₂ was successfully prepared by sol–gel and oxalate co-precipitation methods. A systematic analysis of the materials shows that the 0.5Li₂MnO₃·0.5LiMn_0.8Ni_0.1Co_0.1O₂ prepared by the oxalic acid co-precipitation method had the most stable layered structure and the best electrochemical performance. The initial discharge specific capacity was 261.6 mAh·g⁻¹ at 0.05 C, and the discharge specific capacity was 138 mAh·g⁻¹ at 5 C. The voltage decay was only 210 mV, and the capacity retention was 94.2% after 100 cycles at 1 C. The suppression of voltage decay can be attributed to the high nickel content and uniform element distribution. In addition, tightly packed porous spheres help to reduce lithium ion diffusion energy and improve the stability of the layered structure, thereby improving cycle stability and rate capacity. This conclusion provides a reference for designing high-energy-density lithium-ion batteries. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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12 pages, 6992 KiB

Open AccessArticle

Effect of Different Composition on Voltage Attenuation of Li-Rich Cathode Material for Lithium-Ion Batteries

by Jun Liu, Qiming Liu, Huali Zhu, Feng Lin, Yan Ji, Bingjing Li, Junfei Duan, Lingjun Li and Zhaoyong Chen

Materials 2020, 13(1), 40; https://doi.org/10.3390/ma13010040 - 20 Dec 2019

Cited by 23 | Viewed by 3790

Abstract

Li-rich layered oxide cathode materials have become one of the most promising cathode materials for high specific energy lithium-ion batteries owning to its high theoretical specific capacity, low cost, high operating voltage and environmental friendliness. Yet they suffer from severe capacity and voltage attenuation during prolong cycling, which blocks their commercial application. To clarify these causes, we synthesize Li_1.5Mn_0.55Ni_0.4Co_0.05O_2.5 (Li_1.2Mn_0.44Ni_0.32Co_0.04O₂) with high-nickel-content cathode material by a solid-sate complexation method, and it manifests a lot slower capacity and voltage attenuation during prolong cycling compared to Li_1.5Mn_0.66Ni_0.17Co_0.17O_2.5 (Li_1.2Mn_0.54Ni_0.13Co_0.13O₂) and Li_1.5Mn_0.65Ni_0.25Co_0.1O_2.5 (Li_1.2Mn_0.52Ni_0.2Co_0.08O₂) cathode materials. The capacity retention at 1 C after 100 cycles reaches to 87.5% and the voltage attenuation after 100 cycles is only 0.460 V. Combining X-ray diffraction (XRD), scanning electron microscope (SEM), and transmission electron microscopy (TEM), it indicates that increasing the nickel content not only stabilizes the structure but also alleviates the attenuation of capacity and voltage. Therefore, it provides a new idea for designing of Li-rich layered oxide cathode materials that suppress voltage and capacity attenuation. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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11 pages, 6944 KiB

Open AccessArticle

Development of ZIF-Derived Nanoporous Carbon and Cobalt Sulfide-Based Electrode Material for Supercapacitor

by Rabia Ahmad, Naseem Iqbal and Tayyaba Noor

Materials 2019, 12(18), 2940; https://doi.org/10.3390/ma12182940 - 11 Sep 2019

Cited by 25 | Viewed by 3744

Abstract

Zeolitic Imidazolate Framework (ZIF-67) was prepared in two different solvents—water and methanol. Nanoporous carbon was derived from ZIF-67 via pyrolysis in an inert atmosphere. Anion exchange step of sulfidation on the synthesized material has a great influence on the structure and properties. Structural morphology and thermal stability were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM)/energy dispersive x-ray spectroscopy (EDS), Brunauer-Emmett-Teller (BET), and thermogravimetric (TG) analysis. The electrochemical analysis was evaluated by cyclic voltammetry, chronopotentiometry, and impedance analysis. The as-prepared nanoporous carbon and cobalt sulfide (NPC/CS) electrode material (water) in 2M KOH electrolyte solution exhibit high specific capacitance of 677 F/g. The excellent electrochemical performance of the NPC/CS was attributed to its hierarchical structure. This functionalized ZIF driven strategy paves the way to the preparation of various metal oxide and metal sulfide-based nanoheterostructures by varying the type of metal. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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11 pages, 3562 KiB

Open AccessArticle

Enhanced Electrochemical Performances of Cobalt-Doped Li₂MoO₃ Cathode Materials

by Zhiyong Yu, Jishen Hao, Wenji Li and Hanxing Liu

Materials 2019, 12(6), 843; https://doi.org/10.3390/ma12060843 - 13 Mar 2019

Cited by 15 | Viewed by 2708

Abstract

Co-doped Li₂MoO₃ was successfully synthesized via a solid phase method. The impacts of Co-doping on Li₂MoO₃ have been analyzed by X-ray photoelectron spectroscopy (XPS), X-ray powder diffraction (XRD), scanning electron microscope (SEM), and Fourier transform infrared spectroscopy (FTIR) measurements. The results show that an appropriate amount of Co ions can be introduced into the Li₂MoO₃ lattices, and they can reduce the particle sizes of the cathode materials. Electrochemical tests reveal that Co-doping can significantly improve the electrochemical performances of the Li₂MoO₃ materials. Li₂Mo_0.90Co_0.10O₃ presents a first-discharge capacity of 220 mAh·g⁻¹, with a capacity retention of 63.6% after 50 cycles at 5 mA·g⁻¹, which is much better than the pristine samples (181 mAh·g⁻¹, 47.5%). The enhanced electrochemical performances could be due to the enhancement of the structural stability, and the reduction in impedance, due to the Co-doping. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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14 pages, 1701 KiB

Open AccessArticle

Simulation-driven Selection of Electrode Materials Based on Mechanical Performance for Lithium-Ion Battery

by Abhishek Sarkar, Pranav Shrotriya and Abhijit Chandra

Materials 2019, 12(5), 831; https://doi.org/10.3390/ma12050831 - 12 Mar 2019

Cited by 11 | Viewed by 3583

Abstract

Experimental and numerical studies have shown that mechanical loading associated with lithiation/delithiation may limit the useful life of battery electrode materials. The paper presents an approach to parameterize and compare electrode material performance based on mechanical stability. A mathematical model was developed to determine particle deformation and stress fields based upon an elastic-perfectly plastic constitutive response. Mechanical deformation was computed by combining the stress equilibrium equations with the electrochemical diffusion of lithium ions into the electrode particle. The result provided a time developing stress field which shifts from purely elastic to partially plastic deformation as the lithium-ion diffuses into the particle. The model was used to derive five merit indices that parameterize mechanical stability of electrode materials. The merit indices were used to analyze the mechanical stability for the six candidate electrode materials—three for anode materials and three for the cathode material. Finally, the paper suggests ways to improve the mechanical performance of electrode materials and identifies mechanical properties that need to be considered for selection and optimal design of electrode materials. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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13 pages, 3604 KiB

Open AccessArticle

Super-Capacitive Performance of Manganese Dioxide/Graphene Nano-Walls Electrodes Deposited on Stainless Steel Current Collectors

by Roger Amade, Arevik Muyshegyan-Avetisyan, Joan Martí González, Angel Pérez del Pino, Eniko György, Esther Pascual, José Luís Andújar and Enric Bertran Serra

Materials 2019, 12(3), 483; https://doi.org/10.3390/ma12030483 - 04 Feb 2019

Cited by 21 | Viewed by 4014

Abstract

Graphene nano-walls (GNWs) are promising materials that can be used as an electrode in electrochemical devices. We have grown GNWs by inductively-coupled plasma-enhanced chemical vapor deposition on stainless steel (AISI304) substrate. In order to enhance the super-capacitive properties of the electrodes, we have deposited a thin layer of MnO₂ by electrodeposition method. We studied the effect of annealing temperature on the electrochemical properties of the samples between 70 °C and 600 °C. Best performance for supercapacitor applications was obtained after annealing at 70 °C with a specific capacitance of 104 F·g⁻¹ at 150 mV·s⁻¹ and a cycling stability of more than 14k cycles with excellent coulombic efficiency and 73% capacitance retention. Electrochemical impedance spectroscopy, cyclic voltammetry, and galvanostatic charge/discharge measurements reveal fast proton diffusion (1.3 × 10⁻¹³ cm²·s⁻¹) and surface redox reaction after annealing at 70 °C. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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13 pages, 10396 KiB

Open AccessArticle

Enhanced Electrochemical Performance of Li_1.27Cr_0.2Mn_0.53O₂ Layered Cathode Materials via a Nanomilling-Assisted Solid-state Process

by Chengkang Chang, Jian Dong, Li Guan and Dongyun Zhang

Materials 2019, 12(3), 468; https://doi.org/10.3390/ma12030468 - 03 Feb 2019

Cited by 6 | Viewed by 2624

Abstract

Li_1.27Cr_0.2Mn_0.53O₂ layered cathodic materials were prepared by a nanomilling-assisted solid-state process. Whole-pattern refinement of X-ray diffraction (XRD) data revealed that the samples are solid solutions with layered α-NaFeO₂ structure. SEM observation of the prepared powder displayed a mesoporous nature composed of tiny primary particles in nanoscale. X-ray photoelectron spectroscopy (XPS) studies on the cycled electrodes confirmed that triple-electron-process of the Cr³⁺/Cr⁶⁺ redox pair, not the two-electron-process of Mn redox pair, dominants the electrochemical process within the cathode material. Capacity test for the sample revealed an initial discharge capacity of 195.2 mAh·g⁻¹ at 0.1 C, with capacity retention of 95.1% after 100 cycles. EIS investigation suggested that the high Li ion diffusion coefficient (3.89 × 10⁻¹⁰·cm²·s⁻¹), caused by the mesoporous nature of the cathode powder, could be regarded as the important factor for the excellent performance of the Li_1.27Cr_0.2Mn_0.53O₂ layered material. The results demonstrated that the cathode material prepared by our approach is a good candidate for lithium-ion batteries. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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13 pages, 3055 KiB

Open AccessArticle

Preparation of LiFePO₄/C Cathode Materials via a Green Synthesis Route for Lithium-Ion Battery Applications

by Rongyue Liu, Jianjun Chen, Zhiwen Li, Qing Ding, Xiaoshuai An, Yi Pan, Zhu Zheng, Minwei Yang and Dongju Fu

Materials 2018, 11(11), 2251; https://doi.org/10.3390/ma11112251 - 12 Nov 2018

Cited by 29 | Viewed by 7314

Abstract

In this work, LiFePO₄/C composite were synthesized via a green route by using Iron (III) oxide (Fe₂O₃) nanoparticles, Lithium carbonate (Li₂CO₃), glucose powder and phosphoric acid (H₃PO₄) solution as raw materials. The reaction principles for the synthesis of LiFePO₄/C composite were analyzed, suggesting that almost no wastewater and air polluted gases are discharged into the environment. The morphological, structural and compositional properties of the LiFePO₄/C composite were characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), transmission electron microscopy (TEM), Raman and X-ray photoelectron spectroscopy (XPS) spectra coupled with thermogravimetry/Differential scanning calorimetry (TG/DSC) thermal analysis in detail. Lithium-ion batteries using such LiFePO₄/C composite as cathode materials, where the loading level is 2.2 mg/cm², exhibited excellent electrochemical performances, with a discharge capability of 161 mA h/g at 0.1 C, 119 mA h/g at 10 C and 93 mA h/g at 20 C, and a cycling stability with 98.0% capacity retention at 1 C after 100 cycles and 95.1% at 5 C after 200 cycles. These results provide a valuable approach to reduce the manufacturing costs of LiFePO₄/C cathode materials due to the reduced process for the polluted exhaust purification and wastewater treatment. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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7 pages, 1615 KiB

Open AccessArticle

Structure and Electrochemical Properties of Mn₃O₄ Nanocrystal-Coated Porous Carbon Microfiber Derived from Cotton

by Dongya Sun, Liwen He, Yongle Lai, Jiqiong Lian, Jingjing Sun, An Xie and Bizhou Lin

Materials 2018, 11(10), 1987; https://doi.org/10.3390/ma11101987 - 15 Oct 2018

Cited by 9 | Viewed by 2648

Abstract

Biomorphic Mn₃O₄ nanocrystal/porous carbon microfiber composites were hydrothermally fabricated and subsequently calcined using cotton as a biotemplate. The as-prepared material exhibited a specific capacitance of 140.8 F·g⁻¹ at 0.25 A·g⁻¹ and an excellent cycle stability with a capacitance retention of 90.34% after 5000 cycles at 1 A·g⁻¹. These characteristics were attributed to the introduction of carbon fiber, the high specific surface area, and the optimized microstructure inherited from the biomaterial. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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9 pages, 5868 KiB

Open AccessArticle

High Electrochemical Performance of Nanotube Structured ZnS as Anode Material for Lithium–Ion Batteries

by Wen Zhang, Junfan Zhang, Yan Zhao, Taizhe Tan and Tai Yang

Materials 2018, 11(9), 1537; https://doi.org/10.3390/ma11091537 - 26 Aug 2018

Cited by 14 | Viewed by 2980

Abstract

By using ZnO nanorods as an ideal sacrificial template, one-dimensional (1-D) ZnS nanotubes with a mean diameter of 10 nm were successfully synthesized by hydrothermal method. The phase composition and microstructure of the ZnS nanotubes were characterized by using XRD (X-ray diffraction), SEM (scanning electron micrograph), and TEM (transmission electronic microscopy) analysis. X-ray photoelectron spectroscopy (XPS) and nitrogen sorption isotherms measurements were also used to study the information on the surface chemical compositions and specific surface area of the sample. The prepared ZnS nanotubes were used as anode materials in lithium-ion batteries. Results show that the ZnS nanotubes deliver an impressive prime discharge capacity as high as 950 mAh/g. The ZnS nanotubes also exhibit an enhanced cyclic performance. Even after 100 charge/discharge cycles, the discharge capacity could still remain at 450 mAh/g. Moreover, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) measurements were also carried out to evaluate the ZnS electrodes. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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Review

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15 pages, 2979 KiB

Open AccessFeature PaperReview

AC-Filtering Supercapacitors Based on Edge Oriented Vertical Graphene and Cross-Linked Carbon Nanofiber

by Wenyue Li, Nazifah Islam, Guofeng Ren, Shiqi Li and Zhaoyang Fan

Materials 2019, 12(4), 604; https://doi.org/10.3390/ma12040604 - 18 Feb 2019

Cited by 11 | Viewed by 4276

Abstract

There is strong interest in developing high-frequency (HF) supercapacitors or electrochemical capacitors (ECs), which can work at the hundreds to kilo hertz range for line-frequency alternating current (AC) filtering in the substitution of bulky aluminum electrolytic capacitors, with broad applications in the power and electronic fields. Although great progress has been achieved in the studies of electrode materials for ECs, most of them are not suitable to work in this high frequency range because of the slow electrochemical processes involved. Edge-oriented vertical graphene (VG) networks on 3D scaffolds have a unique structure that offers straightforward pore configuration, reasonable surface area, and high electronic conductivity, thus allowing the fabrication of HF-ECs. Comparatively, highly conductive freestanding cross-linked carbon nanofibers (CCNFs), derived from bacterial cellulose in a rapid plasma pyrolysis process, can also provide a large surface area but free of rate-limiting micropores, and are another good candidate for HF-ECs. In this mini review, advances in these fields are summarized, with emphasis on our recent contributions in the study of these materials and their electrochemical properties including preliminary demonstrations of HF-ECs for AC line filtering and pulse power storage applications. Full article

(This article belongs to the Special Issue Advances in Electrochemical Energy Materials)

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