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14 pages, 5810 KiB

Open AccessArticle

Electronic Structure Regulated Nickel-Cobalt Bimetal Phosphide Nanoneedles for Efficient Overall Water Splitting

by Heyang Xu, Xilin She, Haolin Li, Chuanhui Wang, Shuai Chen, Lipeng Diao, Ping Lu, Longwei Li, Liwen Tan, Jin Sun and Yihui Zou

Molecules 2024, 29(3), 657; https://doi.org/10.3390/molecules29030657 - 31 Jan 2024

Viewed by 620

Abstract

Transition metal phosphides (TMPs) have been widely studied for water decomposition for their monocatalytic property for anodic or cathodic reactions. However, their bifunctional catalytic activity still remains a major challenge. Herein, hexagonal nickel-cobalt bimetallic phosphide nanoneedles with 1–3 μm length and 15–30 nm [...] Read more.

Transition metal phosphides (TMPs) have been widely studied for water decomposition for their monocatalytic property for anodic or cathodic reactions. However, their bifunctional catalytic activity still remains a major challenge. Herein, hexagonal nickel-cobalt bimetallic phosphide nanoneedles with 1–3 μm length and 15–30 nm diameter supported on NF (Ni_xCo_2−xP NDs/NF) with adjusted electron structure have been successfully prepared. The overall alkaline water electrolyzer composed of the optimal anode (Ni_0.67Co_1.33P NDs/NF) and cathode (Ni_1.01Co_0.99P NDs/NF) provide 100 mA cm⁻² at 1.62 V. Gibbs Free Energy for reaction paths proves that the active site in the hydrogen evolution reaction (HER) is Ni and the oxygen evolution reaction (OER) is Co in Ni_xCo_2−xP, respectively. In the HER process, Co-doping can result in an apparent accumulation of charge around Ni active sites in favor of promoting HER activity of Ni sites, and ΔG_H* of 0.19 eV is achieved. In the OER process, the abundant electron transfer around Co-active sites results in the excellent ability to adsorb and desorb *O and *OOH intermediates and an effectively reduced ∆G_RDS of 0.37 eV. This research explains the regulation of electronic structure change on the active sites of bimetallic materials and provides an effective way to design a stable and effective electrocatalytic decomposition of alkaline water. Full article

(This article belongs to the Special Issue Battery Chemistry: Recent Advances and Future Opportunities)

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14 pages, 3982 KiB

Open AccessArticle

Efficient Fe₃C-CF Cathode Catalyst Based on the Formation/Decomposition of Li_2−xO₂ for Li-O₂ Batteries

by Guanyu Yi, Gaoyang Li, Shuhuai Jiang, Guoliang Zhang, Liang Guo, Xiuqi Zhang, Zhongkui Zhao, Zhongping Zou, Hailong Ma, Xiaojiao Fu, Yan Liu and Feng Dang

Molecules 2023, 28(14), 5597; https://doi.org/10.3390/molecules28145597 - 24 Jul 2023

Cited by 1 | Viewed by 990

Abstract

Lithium-oxygen batteries have attracted considerable attention in the past several years due to their ultra-high theoretical energy density. However, there are still many serious issues that must be addressed before considering practical applications, including the sluggish oxygen redox kinetics, the limited capacity far [...] Read more.

Lithium-oxygen batteries have attracted considerable attention in the past several years due to their ultra-high theoretical energy density. However, there are still many serious issues that must be addressed before considering practical applications, including the sluggish oxygen redox kinetics, the limited capacity far from the theoretical value, and the poor cycle stability. This study proposes a surface modification strategy that can enhance the catalytic activity by loading Fe₃C particles on carbon fibers, and the microstructure of Fe₃C particle-modified carbon fibers is studied by multiple materials characterization methods. Experiments and density functional theory (DFT) calculations show that the discharge products on the Fe₃C carbon fiber (Fe₃C-CF) cathode are mainly Li_2−xO₂. Fe₃C-CF exhibits high catalytic ability based on its promotion of the formation/decomposition processes of Li_2−xO₂. Consequently, the well-designed electrode catalyst exhibits a large specific capacity of 17,653.1 mAh g⁻¹ and an excellent cyclability of 263 cycles at a current of 200 mA g⁻¹. Full article

(This article belongs to the Special Issue Battery Chemistry: Recent Advances and Future Opportunities)

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14 pages, 4702 KiB

Open AccessArticle

Enhanced Capacity Retention of Li₃V₂(PO₄)₃-Cathode-Based Lithium Metal Battery Using SiO₂-Scaffold-Confined Ionic Liquid as Hybrid Solid-State Electrolyte

by Shihao Peng, Jiakun Luo, Wenwen Liu, Xiaolong He and Fang Xie

Molecules 2023, 28(13), 4896; https://doi.org/10.3390/molecules28134896 - 21 Jun 2023

Viewed by 1009

Abstract

Li₃V₂(PO₄)₃ (LVP) is one of the candidates for high-energy-density cathode materials matching lithium metal batteries due to its high operating voltage and theoretical capacity. However, the inevitable side reactions of LVP with a traditional liquid-state electrolyte [...] Read more.

Li₃V₂(PO₄)₃ (LVP) is one of the candidates for high-energy-density cathode materials matching lithium metal batteries due to its high operating voltage and theoretical capacity. However, the inevitable side reactions of LVP with a traditional liquid-state electrolyte under high voltage, as well as the uncontrollable growth of lithium dendrites, worsen the cycling performance. Herein, a hybrid solid-state electrolyte is prepared by the confinement of a lithium-containing ionic liquid with a mesoporous SiO₂ scaffold, and used for a LVP-cathode-based lithium metal battery. The solid-state electrolyte not only exhibits a high ionic conductivity of 3.14 × 10⁻⁴ S cm⁻¹ at 30 °C and a wide electrochemical window of about 5 V, but also has good compatibility with the LVP cathode material. Moreover, the cell paired with a solid-state electrolyte exhibits good reversibility and can realize a stable operation at a voltage of up to 4.8 V, and the discharge capacity is well-maintained after 100 cycles, which demonstrates excellent capacity retention. As a contrast, the cell paired with a conventional liquid-state electrolyte shows only an 87.6% discharge capacity retention after 100 cycles. In addition, the effectiveness of a hybrid solid-state electrolyte in suppressing dendritic lithium is demonstrated. The work presents a possible choice for the use of a hybrid solid-state electrolyte compatible with high-performance cathode materials in lithium metal batteries. Full article

(This article belongs to the Special Issue Battery Chemistry: Recent Advances and Future Opportunities)

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16 pages, 7092 KiB

Open AccessArticle

Effect of Indole-2-carboxylic Acid on the Self-Corrosion and Discharge Activity of Aluminum Alloy Anode in Alkaline Al–Air Battery

by Lei Guo, Yue Huang, Alessandra Gilda Ritacca, Kai Wang, Ida Ritacco, Yan Tan, Yujie Qiang, Nabil Al-Zaqri, Wei Shi and Xingwen Zheng

Molecules 2023, 28(10), 4193; https://doi.org/10.3390/molecules28104193 - 19 May 2023

Cited by 2 | Viewed by 1488

Abstract

Al–air battery has been regarded as a promising new energy source. However, the self-corrosion of aluminum anode leads to a loss of battery capacity and a decrease in battery longevity, limiting its commercial applications. Herein, indole-2-carboxylic acid (ICA) has been added to 4 [...] Read more.

Al–air battery has been regarded as a promising new energy source. However, the self-corrosion of aluminum anode leads to a loss of battery capacity and a decrease in battery longevity, limiting its commercial applications. Herein, indole-2-carboxylic acid (ICA) has been added to 4 M NaOH as a corrosion inhibitor. Its impact on the self-corrosion of aluminum alloy and the enhancement of the functionality of Al–air batteries at various concentrations have been investigated. X-ray photoelectron spectroscopy (XPS), attenuated total reflection Fourier transform infrared (ATR-FTIR) spectroscopy, atomic force microscopy (AFM), and scanning electron microscopy (SEM) techniques have been used to examine the compositional and morphological alterations of aluminum alloy surfaces. Electrochemical and hydrogen evolution tests showed that indole-2-carboxylic acid is an efficient corrosion inhibitor in alkaline solutions, and its impact grows with concentration. Our findings demonstrated that when the inhibitor concentration is 0.07 M, the inhibition efficiency is 54.0%, the anode utilization rises from 40.2% to 79.9%, the capacity density increases from 1197.6 to 2380.9 mAh g⁻¹, and the energy density increases from 1469.9 to 2951.8 Wh kg⁻¹. In addition, theoretical calculations have been performed to support the experimental results. Full article

(This article belongs to the Special Issue Battery Chemistry: Recent Advances and Future Opportunities)

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Review

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29 pages, 8261 KiB

Open AccessReview

From Molecular Simulations to Experiments: The Recent Development of Room Temperature Ionic Liquid-Based Electrolytes in Electric Double-Layer Capacitors

by Kun Zhang, Chunlei Wei, Menglian Zheng, Jingyun Huang and Guohui Zhou

Molecules 2024, 29(6), 1246; https://doi.org/10.3390/molecules29061246 - 11 Mar 2024

Viewed by 682

Abstract

Due to the unique properties of room temperature ionic liquids (RTILs), most researchers’ interest in RTIL-based electrolytes in electric double-layer capacitors (EDLCs) stems from molecular simulations, which are different from experimental scientific research fields. The knowledge of RTIL-based electrolytes in EDLCs began with [...] Read more.

Due to the unique properties of room temperature ionic liquids (RTILs), most researchers’ interest in RTIL-based electrolytes in electric double-layer capacitors (EDLCs) stems from molecular simulations, which are different from experimental scientific research fields. The knowledge of RTIL-based electrolytes in EDLCs began with a supposition obtained from the results of molecular simulations of molten salts. Furthermore, experiments and simulations were promoted and developed rapidly on this topic. In some instances, the achievements of molecular simulations are ahead of even those obtained from experiments in quantity and quality. Molecular simulations offer more information on the impacts of overscreening, quasicrowding, crowding, and underscreening for RTIL-based electrolytes than experimental studies, which can be helpful in understanding the mechanisms of EDLCs. With the advancement of experimental technology, these effects have been verified by experiments. The simulation prediction of the capacitance curve was in good agreement with the experiment for pure RTILs. For complex systems, such as RTIL–solvent mixtures and RTIL mixture systems, both molecular simulations and experiments have reported that the change in capacitance curves is not monotonous with RTIL concentrations. In addition, there are some phenomena that are difficult to explain in experiments and can be well explained through molecular simulations. Finally, experiments and molecular simulations have maintained synchronous developments in recent years, and this paper discusses their relationship and reflects on their application. Full article

(This article belongs to the Special Issue Battery Chemistry: Recent Advances and Future Opportunities)

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22 pages, 7110 KiB

Open AccessFeature PaperReview

Modification Strategies of High-Energy Li-Rich Mn-Based Cathodes for Li-Ion Batteries: A Review

by Zhenjie Xi, Qing Sun, Jing Li, Ying Qiao, Guanghui Min and Lijie Ci

Molecules 2024, 29(5), 1064; https://doi.org/10.3390/molecules29051064 - 29 Feb 2024

Viewed by 1043

Abstract

Li-rich manganese-based oxide (LRMO) cathode materials are considered to be one of the most promising candidates for next-generation lithium-ion batteries (LIBs) because of their high specific capacity (250 mAh g⁻¹) and low cost. However, the inevitable irreversible structural transformation during cycling [...] Read more.

Li-rich manganese-based oxide (LRMO) cathode materials are considered to be one of the most promising candidates for next-generation lithium-ion batteries (LIBs) because of their high specific capacity (250 mAh g⁻¹) and low cost. However, the inevitable irreversible structural transformation during cycling leads to large irreversible capacity loss, poor rate performance, energy decay, voltage decay, etc. Based on the recent research into LRMO for LIBs, this review highlights the research progress of LRMO in terms of crystal structure, charging/discharging mechanism investigations, and the prospects of the solution of current key problems. Meanwhile, this review summarizes the specific modification strategies and their merits and demerits, i.e., surface coating, elemental doping, micro/nano structural design, introduction of high entropy, etc. Further, the future development trend and business prospect of LRMO are presented and discussed, which may inspire researchers to create more opportunities and new ideas for the future development of LRMO for LIBs with high energy density and an extended lifespan. Full article

(This article belongs to the Special Issue Battery Chemistry: Recent Advances and Future Opportunities)

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22 pages, 9169 KiB

Open AccessReview

Stannate-Based Materials as Anodes in Lithium-Ion and Sodium-Ion Batteries: A Review

by You-Kang Duan, Zhi-Wei Li, Shi-Chun Zhang, Tong Su, Zhi-Hong Zhang, Ai-Jun Jiao and Zhen-Hai Fu

Molecules 2023, 28(13), 5037; https://doi.org/10.3390/molecules28135037 - 27 Jun 2023

Cited by 4 | Viewed by 1506

Abstract

Binary metal oxide stannate (M₂SnO₄; M = Zn, Mn, Co, etc.) structures, with their high theoretical capacity, superior lithium storage mechanism and suitable operating voltage, as well as their dual suitability for lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs), [...] Read more.

Binary metal oxide stannate (M₂SnO₄; M = Zn, Mn, Co, etc.) structures, with their high theoretical capacity, superior lithium storage mechanism and suitable operating voltage, as well as their dual suitability for lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs), are strong candidates for next-generation anode materials. However, the capacity deterioration caused by the severe volume expansion problem during the insertion/extraction of lithium or sodium ions during cycling of M₂SnO₄-based anode materials is difficult to avoid, which greatly affects their practical applications. Strategies often employed by researchers to address this problem include nanosizing the material size, designing suitable structures, doping with carbon materials and heteroatoms, metal–organic framework (MOF) derivation and constructing heterostructures. In this paper, the advantages and issues of M₂SnO₄-based materials are analyzed, and the strategies to solve the issues are discussed in order to promote the theoretical work and practical application of M₂SnO₄-based anode materials. Full article

(This article belongs to the Special Issue Battery Chemistry: Recent Advances and Future Opportunities)

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17 pages, 3882 KiB

Open AccessReview

Layered-Oxide Cathode Materials for Fast-Charging Lithium-Ion Batteries: A Review

by Xin Meng, Jiale Wang and Le Li

Molecules 2023, 28(10), 4007; https://doi.org/10.3390/molecules28104007 - 10 May 2023

Cited by 5 | Viewed by 3214

Abstract

Layered oxides are considered prospective state-of-the-art cathode materials for fast-charging lithium-ion batteries (LIBs) owning to their economic effectiveness, high energy density, and environmentally friendly nature. Nonetheless, layered oxides experience thermal runaway, capacity decay, and voltage decay during fast charging. This article summarizes various [...] Read more.

Layered oxides are considered prospective state-of-the-art cathode materials for fast-charging lithium-ion batteries (LIBs) owning to their economic effectiveness, high energy density, and environmentally friendly nature. Nonetheless, layered oxides experience thermal runaway, capacity decay, and voltage decay during fast charging. This article summarizes various modifications recently implemented in the fast charging of LIB cathode materials, including component improvement, morphology control, ion doping, surface coating, and composite structure. The development direction of layered-oxide cathodes is summarized based on research progress. Further, possible strategies and future development directions of layered-oxide cathodes to improve fast-charging performance are proposed. Full article

(This article belongs to the Special Issue Battery Chemistry: Recent Advances and Future Opportunities)

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