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Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage

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A special issue of Coatings (ISSN 2079-6412). This special issue belongs to the section "Surface Engineering for Energy Harvesting, Conversion, and Storage".

Deadline for manuscript submissions: 10 August 2025 | Viewed by 10522

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Dr. Yong Liu

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Guest Editor

School of Materials Science and Engineering, Henan University of Science and Technology, Luoyang, China
Interests: metal-based nanomaterials; metal-based nanocomposites; metal batteries; electrocatalysis; advanced characterization techniques
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Special Issue Information

Dear Colleagues,

Widespread application of fossil fuels for energy generation and transportation purposes during the past few decades has dramatically increased the concentration of greenhouse gases in the atmosphere, causing an unprecedented rise in the Earth’s temperature and acidification of the oceans. Therefore, there is an urgent need to reduce the devastating consequences of global warming, as highlighted in the Global Summit on Climate Change (Paris Agreement), as well as the European Commission. Replacing conventional fossil fuels with renewable sources of energy has been recognized as one of the crucial actions required. In this regard, a switch from internal combustion engines (ICE) to electric vehicles (EVs) has recently attracted great attention as the major portion of fossil fuels is consumed for transportation purposes. Meanwhile, transition metal compounds are also rich in physical and chemical properties and widely used in the electrochemical energy storage. They are key materials for chemical power supply, such as lithium/sodium–ion batteries, lithium–sulfur batteries, metal air batteries, supercapacitors, etc. Transition metal compounds are usually of variable valence, composition and structure, involved in complex chemical reactions and structure–activity relationships. Developing their controllable preparatory methods, revealing the laws of physical properties, building battery devices, and achieving high-density energy storage have been the hot spots and focuses of cross-disciplinary research in chemistry, materials, energy and other disciplines. Different surface modification methods, such as atomic layer deposition, chemical vapor deposition, ion beam sputtering, wet chemistry method, solvent casting method, etc., have been used to fabricate high-performance transition metal-based electrodes for electrochemical energy storage.

We are pleased to invite you to contribute original research articles and reviews that will stimulate further research activities in this area and improve our understanding of the key scientific and technological problems in surface modification of advanced transition metal-based materials for electrochemical energy storage. We are particularly interested in articles describing advanced materials with effective surface modifications for energy-storage devices (Li/Na/K/Zn/Mg ion batteries, metal–sulfur batteries, metal-air batteries, supercapacitors) and other transition metal-based electrodes for electrochemical energy storage.

In this Special Issue, original research articles and reviews are welcome. Research areas may include (but are not limited to) the following:

Advanced electrode materials with surface modifications for Li/Na/K/Zn/Mg-ion batteries and supercapacitors;
Surface-defect-rich nanostructured electrode materials for lithium–sulfur and metal-air batteries;
Novel design and advanced surface modification techniques of electrodes;
Materials analytics, structure characterization and functional evaluation;
Theoretical and experimental understanding of the relationships between structure and performance;
The structure evolution during the electrochemical reactions of the related materials.

We look forward to receiving your contributions.

Dr. Yong Liu
Guest Editor

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Coatings is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2600 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

surface modification
energy storage technology
transition metal-based materials
advanced characterization methods
properties of transition metals
transition metal oxide
transition metal sulfide
transition metal phosphide
metal organic frameworks

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Published Papers (9 papers)

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Research

Jump to: Review

11 pages, 11165 KiB

Open AccessArticle

Effect of Trace Bismuth on Deformation Behavior of Ultrahigh-Purity Copper during Hot Compression

by Haitao Liu, Yunxiao Hua, Weiqiang Li, Zhenguo Hou, Jincan Dong and Yong Liu

Coatings 2024, 14(10), 1261; https://doi.org/10.3390/coatings14101261 - 1 Oct 2024

Viewed by 560

Abstract

The effect of trace Bi impurities on the flow stress, microstructure evolution, and dynamic recrystallization (DRX) of the ultrahigh-purity copper was systematically investigated by a hot compression test at 600 °C. The results show that the peak stress of the ultrahigh-purity copper gradually decreases with increasing Bi content. Trace Bi impurities can refine the microstructure of ultrahigh-purity copper. However, the refinement effect of 50 wt ppm Bi is much more significant than that of 140 wt ppm Bi during the hot deformation. This effect is ascribed to the higher concentration of Bi at GBs, which induces severe GB cracks that reduces the driving force for the nucleation of DRX grains. In addition, the introduction of Bi inhibits the DRX of the ultrahigh-purity copper and transforms its DRX process from the discontinuous dynamic recrystallization (DDRX) to the coexistence of DDRX and continuous dynamic recrystallization (CDRX) mechanisms. Full article

(This article belongs to the Special Issue Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage)

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21 pages, 10824 KiB

Open AccessArticle

ULPING-Based Titanium Oxide as a New Cathode Material for Zn-Ion Batteries

by Suben Sri Shiam, Jyotisman Rath, Eduardo Gutiérrez Vera and Amirkianoosh Kiani

Coatings 2024, 14(9), 1163; https://doi.org/10.3390/coatings14091163 - 9 Sep 2024

Cited by 1 | Viewed by 899

Abstract

The need for alternative energy storage options beyond lithium-ion batteries is critical due to their high costs, resource scarcity, and environmental concerns. Zinc-ion batteries offer a promising solution, given zinc’s abundance, cost effectiveness, and safety, particularly its compatibility with non-flammable aqueous electrolytes. In this study, the potential of laser-ablation-based titanium oxide as a novel cathode material for zinc-ion batteries was investigated. The ultra-short laser pulses for in situ nanostructure generation (ULPING) technique was employed to generate nanostructured titanium oxide. This laser ablation process produced highly porous nanostructures, enhancing the electrochemical performance of the electrodes. Zinc and titanium oxide samples were evaluated using two-electrode and three-electrode setups, with cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and galvanostatic charge–discharge (GCD) techniques. Optimal cathode materials were identified in the Ti-5W (laser ablated twice) and Ti-10W (laser ablated ten times) samples, which demonstrated excellent charge capacity and energy density. The Ti-10W sample exhibited superior long-term performance due to its highly porous nanostructures, improving ion diffusion and electron transport. The potential of laser-ablated titanium oxide as a high-performance cathode material for zinc-ion batteries was highlighted, emphasizing the importance of further research to optimize laser parameters and enhance the stability and scalability of these electrodes. Full article

(This article belongs to the Special Issue Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage)

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17 pages, 13049 KiB

Open AccessArticle

Effect of Trace Elements on the Thermal Stability and Electrical Conductivity of Pure Copper

by Haitao Liu, Jincan Dong, Shijun Liang, Weiqiang Li and Yong Liu

Coatings 2024, 14(8), 1017; https://doi.org/10.3390/coatings14081017 - 10 Aug 2024

Viewed by 945

Abstract

The impact of introducing trace transition elements on the thermal stability and conductivity of pure copper was examined through metallographic microscopy (OM), transmission electron microscopy (TEM), and electrical conductivity measurements; the interaction between trace transition element and trace impurity element S in the matrix was analyzed. The results show that the addition of trace Ti and trace Cr, Ni, and Ag elements significantly enhances the thermal stability of the pure copper grain size. After high-temperature treatment at 900 °C/30 min, the grain sizes of Cu, Cu-Ti-S, and Cu-Cr-Ni-Ag-S were measured and found to be 200.24 μm, 83.83 μm, and 31.08 μm, respectively, thus establishing a thermal stability ranking of Cu-Cr-Ni-Ag-S > Cu-Ti-S > Cu. Furthermore, the conductivities of pure copper remain high even after the addition of trace transition elements, with recorded values for Cu, Cu-Ti-S, and Cu-Cr-Ni-Ag-S of 100.7% IACS, 100.2% IACS, and 98.5% IACS, respectively. The enhancement of thermal stability is primarily attributed to the pinning effect of the TiS and CrS phases, as well as the solid solution dragging of Ni and Ag elements. Trace Ti and Cr elements can react with S impurities to form a hexagonal-structure TiS phase and monoclinic-structure CrS phase, which are non-coherent with the matrix. Notably, the CrS phase is smaller than the TiS phase. In addition, the precipitation of these compounds also reduces the scattering of free electrons by solute atoms, thereby minimizing their impact on the alloy’s conductivity. Full article

(This article belongs to the Special Issue Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage)

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15 pages, 12864 KiB

Open AccessArticle

The Influence of Aging Temperatures on the Microstructure and Stress Relaxation Resistance of Cu-Cr-Ag-Si Alloy

by Haitao Liu, Longlong Lu, Guojie Wang and Yong Liu

Coatings 2024, 14(7), 909; https://doi.org/10.3390/coatings14070909 - 20 Jul 2024

Viewed by 646

Abstract

Copper alloys used in connectors rely significantly on stress relaxation resistance as a key property. In this study, a heavily deformed Cu-Cr-Ag-Si alloy underwent aging at varying temperatures, with a subsequent analysis of its mechanical properties and microstructure, with a particular emphasis on understanding the mechanism of improving stress relaxation resistance. As the aging temperature rose, the Cr precipitated into a Cr-Si composite element precipitated phase. Both work hardening and precipitation strengthening played vital roles in enhancing the stress relaxation resistance of the Cu-Cr-Ag-Si alloy, with the latter exerting a more pronounced impact. The notable performance enhancement observed after aging at 450 °C can be attributed to the synergistic effects of work hardening and precipitation strengthening. Following aging at 450 °C, the alloy demonstrated optimal performance, boasting a tensile strength of 495.25 MPa, an electrical conductivity of 84.2% IACS, and a level of 91.12%. These exceptional properties position the alloy as a highly suitable material for connector contacts. Full article

(This article belongs to the Special Issue Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage)

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11 pages, 4251 KiB

Open AccessArticle

Preparation and Capacitive Properties of Ni-Doped Zinc Cobaltate/Carbon Fiber Composite Porous Mesh Materials

by Donghua Chen, Yang Liu, Jun Wang, Tenghao Ma, Hui Zhi, Wei Xiao, Yabin Wang and Jing Wang

Coatings 2024, 14(5), 584; https://doi.org/10.3390/coatings14050584 - 8 May 2024

Viewed by 1069

Abstract

Nickel-element-doped zinc cobaltate/carbon fiber composites (Ni-ZnCo₂O₄/CF) were prepared on carbon cloth (made of a combination of carbon fibers) conductive substrates using a simple ambient stirring method combined with heat treatment. Characterization tests of the materials revealed that the prepared products were porous Ni-ZnCo₂O₄/CF mesh structures. This porous network structure increases the surface area of the material and helps shorten the diffusion path of ions and electrons. The samples were analyzed using X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) methods to investigate the effect of Ni elemental doping on the stability of the materials. The results show that there are no other impurity peaks and no other impurity elements in the Ni-ZnCo₂O₄/CF electrode material, which indicates that the sample purity is high. Meanwhile, the electrochemical properties of Ni-ZnCo₂O₄/CF electrode materials were studied. Under the condition of 15 A·g⁻¹, the specific capacitance of Ni-ZnCo₂O₄/CF electrode material is 1470 F·g⁻¹, and after 100 cycles, its specific capacity reaches 1456 F·g⁻¹, which is 99.0% of the specific capacity of 1470 F·g⁻¹, indicating that the electrode material has good stability. In addition, we assembled asymmetric supercapacitors (Ni-ZnCo₂O₄/CF//CNTs) with Ni-ZnCo₂O₄/CF as the positive material and carbon nanotubes (CNTs) as the negative material. In the cyclic stability experiment of Ni-ZnCo₂O₄/CF/CNTs devices, when the current density was 1 A·g⁻¹, the specific capacitance was 182 F·g⁻¹. After 10,000 cyclic charge–discharge tests, the specific capacity became 167 F·g⁻¹, which was basically unchanged compared with the initial specific capacity, reaching 91.8%. It shows that it has higher charge–discharge performance and higher cycle stability. Full article

(This article belongs to the Special Issue Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage)

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11 pages, 4901 KiB

Open AccessArticle

CoMoO₄ Nanoflowers Doped with La Element for Advanced Electrode Materials

by Donghua Chen, Yang Liu, Danting Li, Tenghao Ma and Jing Wang

Coatings 2024, 14(4), 388; https://doi.org/10.3390/coatings14040388 - 27 Mar 2024

Viewed by 1096

Abstract

La-CoMoO₄ was prepared as the electrode material for supercapacitors using the freeze-drying method. The physical and structural properties of the prepared electrode La-CoMoO₄ were characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). We further investigated the electrochemical performance of La-CoMoO₄ electrode materials through cyclic voltammetry, constant current charge–discharge, and electrochemical impedance spectroscopy. The research results indicate that compared with CoMoO₄ material (1400 F/g), La-CoMoO₄ material has a high specific capacitance of 2248 F/g at a current density of 1 A/g. In addition, La-CoMoO₄ has a high stability, with a capacitance retention rate of up to 99.2% after 5500 cycles. Finally, supercapacitor devices using La-CoMoO₄ material as the positive electrode have a high energy density of 55 Wh/Kg (power density of 1000 W/Kg), making them a promising electrode material. Full article

(This article belongs to the Special Issue Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage)

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12 pages, 4848 KiB

Open AccessArticle

Preparation of ZrO₂/TiO₂/Al₂O₃ Nanofiltration Lab-Scale Membrane for Filtering Heavy Metal Ions

by Jie Yang, Jinquan Sun, Huanzhong Bao, Song Li, Lianbao Zhang, Xinyue Bao, Fujie Li, Qingkun He, Na Wei, Kun Xie and Wensheng Li

Coatings 2022, 12(11), 1681; https://doi.org/10.3390/coatings12111681 - 4 Nov 2022

Cited by 4 | Viewed by 1657

Abstract

ZrO₂ is an excellent ceramic preparation material that can maintain chemical stability in medium–strong acid and alkali environments. The sintering impregnation method was used to prepare the ZrO₂/TiO₂/Al₂O₃ composite nanofiltration membrane (ZTA membrane). Nano-ZrO₂, submicron TiO₂, and microporous Al₂O₃ were used as the surface layer, the transition layer, and the support layer, respectively. The structure and phase of the membrane were measured by scanning electron microscopy (SEM) and X-ray diffractometer (XRD). The composite membrane’s retention, hydrophilic and hydrophobic properties were characterized and evaluated using a UV–Vis spectrophotometer, a water contact angle tester (WCA), and a dead-end filtration device. With the increase in separation layer deposition time, the retention rate of methyl blue increased, and the water flux decreased. At a deposition time of 75 min, the retention rate of methyl blue was more than 80%, and the water flux reached 337.5 L·m⁻² h⁻¹ bar⁻¹ at −1 bar transmembrane pressure. The membranes are hydrophilic and have different interception abilities for metal ions, and the order of retention effect is Ag⁺ > Cu²⁺ > Mg²⁺ > Na⁺, and Ag⁺ and Cu²⁺ reached 65.3% and 50.5%, respectively. The prepared ZTA composite nanofiltration membrane has potential application value in heavy metal ion filtration. Full article

(This article belongs to the Special Issue Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage)

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Review

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23 pages, 4633 KiB

Open AccessReview

Modification of Cu-Based Current Collectors and Their Application in High-Performance Zn Metal Anode: A Review

by Xiujie Gao, Fei Wang, Yibo Xing, Chunyang Kong, Yumeng Gao, Zhihui Jia, Guangbin Wang, Yifei Pei and Yong Liu

Coatings 2024, 14(10), 1300; https://doi.org/10.3390/coatings14101300 - 11 Oct 2024

Viewed by 664

Abstract

Zinc-based batteries (ZBBs) have proven to be tremendously plausible for large-scale electrochemical energy storage applications due to their merits of desirable safety, low-cost, and low environmental impact. Nevertheless, the zinc metal anodes in ZBBs still suffer from many issues, including dendrite growth, hydrogen evolution reactions (HERs), corrosion, passivation, and other types of undesirable side reactions, which severely hinder practical application. The modification of Cu-based current collectors (CCs) has proven to be an efficient method to regulate zinc deposition and prevent dendritic growth, thereby improving the Coulombic efficiency (CE) and lifespan of batteries (e.g., up to 99.977% of CE over 6900 cycles after modification), which is an emerging research topic in recent years. In this review, we provide a systematic overview of the modification of copper-based CCs and their application in zinc metal anodes. The relationships between their modification strategies, nano-micro-structures, and electrochemical performance are systematically reviewed. Ultimately, their promising prospects for future development are also proposed. We hope that this review could contribute to the design of copper-based CCs for zinc-based batteries and facilitate their practical application. Full article

(This article belongs to the Special Issue Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage)

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20 pages, 6487 KiB

Open AccessReview

Recent Advances in Metal–Organic Frameworks for the Surface Modification of the Zinc Metal Anode: A Review

by Yibo Xing, Kaijia Feng, Chunyang Kong, Guangbin Wang, Yifei Pei, Qixiang Huang and Yong Liu

Coatings 2023, 13(8), 1457; https://doi.org/10.3390/coatings13081457 - 18 Aug 2023

Cited by 5 | Viewed by 2041

Abstract

Aqueous zinc ion batteries (AZIBs) are considered as one of the most promising energy storage technologies due to their advantages of being low in cost, high in safety, and their environmental friendliness. However, dendrite growth and parasitic side reactions on the zinc metal anode during cycling lead to a low coulombic efficiency and an unsatisfactory lifespan, which seriously hinders the further development of AZIBs. In this regard, metal–organic frameworks (MOFs) are deemed as suitable surface modification materials for the Zn anode to deal with the abovementioned problems because of their characteristics of a large specific surface area, high porosity, and excellent tunability. Considering the rapidly growing research enthusiasm for this topic in recent years, herein, we summarize the recent advances in the design, fabrication, and application of MOFs and their derivatives in the surface modification of the zinc metal anode. The relationships between nano/microstructures, synthetic methods of MOF-based materials, and the enhanced electrochemical performance of the zinc metal anode via MOF surface modification are systematically summarized and discussed. Finally, the existing problems and future development of this area are proposed. Full article

(This article belongs to the Special Issue Surface Modification of Advanced Transition Metal-Based Materials for Electrochemical Energy Storage)

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