Emerging Low-Dimensional Materials

A special issue of Crystals (ISSN 2073-4352). This special issue belongs to the section "Materials for Energy Applications".

Deadline for manuscript submissions: closed (31 August 2022) | Viewed by 23123

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Special Issue Editors

School of Chemistry and Life Sciences, Nanjing University of Posts and Telecommunications, Nanjing 210003, China
Interests: 2D materials; transition metal dichalcogenides; aberration-corrected TEM/STEM; catalysts; nanocrystals; energy storage and conversion
Special Issues, Collections and Topics in MDPI journals
School of Materials Science and Engineering, Shandong University, Jinan 250100, Shandong, China
Interests: carbon; MXenes; graphene; supercapacitor; solid-state battery; pseudocapacitance
Institute for Superconducting and Electronic Materials, University of Wollongong, Wollongong, NSW 2522, Australia
Interests: alkali metal batteries; materials engineering; energy storage engineering; electrochemistry; physical chemistry; mechanisms of reactions

Special Issue Information

Dear Colleagues,

Technologies for renewable energy and a green environment have received extensive attention in the past few decades. Recently, low-dimensional materials, such as zero-dimensional (0D), one-dimensional (1D), and two-dimensional (2D) materials, have been intensively investigated due to their unique catalytic, mechanical, electronic, and optical properties as well as their various applications. Great efforts have been devoted to studying their synthesis strategies, unique properties, chemical reaction processes, and potential applications. Nevertheless, challenges still exist. It is therefore urgent and significant to have a Special Issue that can help us to appreciate new advances and to review recent progresses in novel low-dimensional materials. The present Special Issue on “Emerging Low-Dimensional Materials” will summarize the progress achieved in the last few years. Especially in the current context of COVID-19, we hope that both researchers and the community in general can benefit from the outcomes of this Special Issue.

Prof. Dr. Bo Chen
Prof. Dr. Rutao Wang
Dr. Nana Wang
Guest Editors

Manuscript Submission Information

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Keywords

  • low-dimensional materials
  • nanocrystals
  • sustainable materials
  • emerging functional nanomaterials
  • heterostructures
  • energy storage and conversion

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Published Papers (12 papers)

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Editorial

Jump to: Research, Review

3 pages, 163 KiB  
Editorial
Emerging Low-Dimensional Materials (Volume I)
by Bo Chen, Rutao Wang and Nana Wang
Crystals 2023, 13(2), 166; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst13020166 - 18 Jan 2023
Viewed by 994
Abstract
We recently published the first volume of the Special Issue “Emerging Low-Dimensional Materials” [...] Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)

Research

Jump to: Editorial, Review

9 pages, 1854 KiB  
Article
Ferrocene Formic Acid Surface Modified Ni(OH)2 for Highly Efficient Alkaline Oxygen Evolution
by Guo-Ping Shen, Ruo-Yao Fan, Bin Dong and Bo Chen
Crystals 2022, 12(10), 1404; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12101404 - 04 Oct 2022
Cited by 1 | Viewed by 1302
Abstract
FeNi-based hybrid materials are among the most representative catalysts for alkaline oxygen evolution reaction (OER), but the modulation of their surface atoms to achieve the optimal catalytic properties is still a big challenge. Here, we report the surface modification of Ni(OH)2/nickel [...] Read more.
FeNi-based hybrid materials are among the most representative catalysts for alkaline oxygen evolution reaction (OER), but the modulation of their surface atoms to achieve the optimal catalytic properties is still a big challenge. Here, we report the surface modification of Ni(OH)2/nickel foam (NF)-based electrocatalyst with a trace amount of ferrocene formic acid (FFA) (FFA-Ni(OH)2/NF) for highly efficient OER. Owing to the strong electron interaction and synergistic effects of Fe-Ni heteroatoms, FFA-Ni(OH)2/NF exhibits an overpotential of 311 mV at a current density of 100 mA cm−2. Impressively, the overpotential of FFA-Ni(OH)2/NF at 100 mA cm−2 is 108 mV less than that of bulk phase doped Ni/FFA(OH)2/NF, demonstrating the surprising effect of heteroatomic surface modification. In addition, by introducing a small amount of surface modifier into the electrolyte, the weak surface reconstruction process in the electrochemical process can be fully utilized to achieve obvious modification effects. Therefore, this work fully proves the feasibility of improving catalytic activities of FeNi-based catalysts by modifying surface heterogeneous atom pairs. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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8 pages, 3448 KiB  
Article
High-Temperature Electronic Transport Properties of PEDOT:PSS Top-Contact Molecular Junctions with Oligophenylene Dithiols
by Dong-Hyoup Seo, Kyungjin Im and Hyunwook Song
Crystals 2022, 12(7), 962; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12070962 - 10 Jul 2022
Cited by 2 | Viewed by 1231
Abstract
In this study, we investigated the high-temperature electronic transport behavior of spin-coated PEDOT:PSS top-contact molecular ensemble junctions based on self-assembled monolayers (SAMs) of oligophenylene dithiols. We observed irreversible temperature-dependent charge transport at the high-temperature regime over 320 K. The effective contact resistance and [...] Read more.
In this study, we investigated the high-temperature electronic transport behavior of spin-coated PEDOT:PSS top-contact molecular ensemble junctions based on self-assembled monolayers (SAMs) of oligophenylene dithiols. We observed irreversible temperature-dependent charge transport at the high-temperature regime over 320 K. The effective contact resistance and normalized resistance decreased with increasing temperature (320 to 400 K), whereas the tunneling attenuation factor was nearly constant irrespective of temperature change. These findings demonstrate that the high-temperature transport properties are not dominated by the integrity of SAMs in molecular junctions, but rather the PEDOT:PSS/SAMs contact. Transition voltage spectroscopy measurements indicated that the contact barrier height of the PEDOT:PSS/SAMs is lowered at elevated temperatures, which gives rise to a decrease in the contact resistance and normalized resistance. The high-temperature charge transport through these junctions is also related to an increase in the grain area of PEDOT cores after thermal treatment. Moreover, it was found that there was no significant change in either the current density or normalized resistance of the annealed junctions after 60 days of storage in ambient conditions. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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10 pages, 2360 KiB  
Article
Demonstration of Molecular Tunneling Junctions Based on Vertically Stacked Graphene Heterostructures
by Seock-Hyeon Hong, Dong-Hyoup Seo and Hyunwook Song
Crystals 2022, 12(6), 787; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12060787 - 29 May 2022
Cited by 4 | Viewed by 1661
Abstract
We demonstrate the fabrication and complete characterization of vertical molecular tunneling junctions based on graphene heterostructures, which incorporate a control series of arylalkane molecules acting as charge transport barriers. Raman spectroscopy and atomic force microscopy were employed to identify the formation of the [...] Read more.
We demonstrate the fabrication and complete characterization of vertical molecular tunneling junctions based on graphene heterostructures, which incorporate a control series of arylalkane molecules acting as charge transport barriers. Raman spectroscopy and atomic force microscopy were employed to identify the formation of the molecular monolayer via an electrophilic diazonium reaction on a pre-patterned bottom graphene electrode. The top graphene electrode was transferred to the deposited molecular layer to form a stable electrical connection without filamentary damage. Then, we showed proof of intrinsic charge carrier transport through the arylalkane molecule in the vertical tunneling junctions by carrying out multiprobe approaches combining complementary transport characterization methods, which included length- and temperature-dependent charge transport measurements and transition voltage spectroscopy. Interpretation of all the electrical characterizations was conducted on the basis of intact statistical analysis using a total of 294 fabricated devices. Our results and analysis can provide an objective criterion to validate molecular electronic devices fabricated with graphene electrodes and establish statistically representative junction properties. Since many of the experimental test beds used to examine molecular junctions have generated large variation in the measured data, such a statistical approach is advantageous to identify the meaningful parameters with the data population and describe how the results can be used to characterize the graphene-based molecular junctions. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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9 pages, 2144 KiB  
Article
Bias-Voltage Dependence of Tunneling Decay Coefficient and Barrier Height in Arylalkane Molecular Junctions with Graphene Contacts as a Protecting Interlayer
by Kyungjin Im, Dong-Hyoup Seo and Hyunwook Song
Crystals 2022, 12(6), 767; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12060767 - 26 May 2022
Cited by 2 | Viewed by 1660
Abstract
We studied a molecular junction with arylalkane self-assembled monolayers sandwiched between two graphene contacts. The arrangement of graphene-based molecular junctions provides a stable device structure with a high yield and allows for extensive transport measurements at 78 K. We observed a temperature-independent current [...] Read more.
We studied a molecular junction with arylalkane self-assembled monolayers sandwiched between two graphene contacts. The arrangement of graphene-based molecular junctions provides a stable device structure with a high yield and allows for extensive transport measurements at 78 K. We observed a temperature-independent current density–voltage (JV) characteristic and the exponential dependency of the current density on the molecular length, proving that the charge transport occurs by non-resonant tunneling through the molecular barrier. Based on the Simmons model, the bias-voltage dependence of the decay coefficient and barrier height was extracted from variable-length transport characterizations. The JV data measured were simulated by the Simmons model, which was modified with the barrier lowering induced by the bias voltage. Indeed, there isno need for adjustable fitting parameters. The resulting simulation was in remarkable consistency with experimental measurements over a full bias range up to |V| ≤ 1.5 V for the case of graphene/arylalkane/graphene heterojunctions. Our findings clearly showed the demonstration of stable and reliable molecular junctions with graphene contacts and their intrinsic charge transport characteristics, as well as justifying the application of the voltage-induced barrier lowering approximation to the graphene-based molecular junction. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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9 pages, 2623 KiB  
Article
In Situ Electrochemical Derivation of Sodium-Tin Alloy as Sodium-Ion Energy Storage Devices Anode with Overall Electrochemical Characteristics
by Liangfeng Niu, Shoujie Guo, Wei Liang, Limin Song, Burong Song, Qianlong Zhang and Lijun Wu
Crystals 2022, 12(5), 575; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12050575 - 20 Apr 2022
Cited by 2 | Viewed by 1670
Abstract
Inspired by the fermentation of multiple small bread embryos to form large bread embryos, in this study, the expansion of tin foil inlaid with sodium rings in the process of repeated sodium inlaid and removal was utilized to maximum extent to realize the [...] Read more.
Inspired by the fermentation of multiple small bread embryos to form large bread embryos, in this study, the expansion of tin foil inlaid with sodium rings in the process of repeated sodium inlaid and removal was utilized to maximum extent to realize the formation of sodium-tin alloy anode and the improvement of sodium storage characteristics. The special design of Sn foil inlaid with Na ring realized the in-situ electrochemical formation of fluffy porous sodium-tin alloy, effectively alleviated the volume expansion and shrinkage of non-electrochemical active Sn metal, and inhibited the generation of sodium dendrites. The abundance of sodium ions provided by the Na metal ring compensated for the active sodium components consumed during the repeated formation of SEI. When sodium-tin alloy in situ derived by Sn foil inlaid with Na ring was used as negative electrodes matched with SCDC and Na0.91MnO2 hexagonal tablets (NMO HTs) positive electrodes, the as-assembled sodium-ion energy storage devices present high specific capacity and excellent cycle stability. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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11 pages, 2691 KiB  
Article
Zeolitic Imidazolate Framework 67-Derived Ce-Doped CoP@N-Doped Carbon Hollow Polyhedron as High-Performance Anodes for Lithium-Ion Batteries
by Yanjun Zhai, Shuli Zhou, Linlin Guo, Xiaole Xin, Suyuan Zeng, Konggang Qu, Nana Wang and Xianxi Zhang
Crystals 2022, 12(4), 533; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12040533 - 11 Apr 2022
Cited by 7 | Viewed by 2871
Abstract
Zeolitic Imidazolate Framework 67 (ZIF-67) and its derivates have attracted extensive interest for lithium-ion batteries (LIBs). Here, Cerium-doped cobalt phosphide@nitrogen-doped carbon (Ce-doped CoP@NC) with hollow polyhedron structure materials were successfully synthesized via ionic-exchange with Co and Ce ions using the ZIF-67 as a [...] Read more.
Zeolitic Imidazolate Framework 67 (ZIF-67) and its derivates have attracted extensive interest for lithium-ion batteries (LIBs). Here, Cerium-doped cobalt phosphide@nitrogen-doped carbon (Ce-doped CoP@NC) with hollow polyhedron structure materials were successfully synthesized via ionic-exchange with Co and Ce ions using the ZIF-67 as a template followed with a facile low-temperature phosphorization treatment. Benefitting from the well-designed hollow polyhedron, steady carbon network, and Ce-doping structural merits, the as-synthesized Ce-doped CoP@NC electrode demonstrated superior performance as the anode in LIBs: a superior cyclability (400 mA h g−1 after 500 cycles) and outstanding rate-capability (590 mA h g−1, reverted to 100 mA g−1). These features not only produced more lithium-active sites for LIBs anode and a shorter Li-ion diffusion pathway to expedite the charge transfer, but also the better tolerance against volume variation of CoP during the repeated lithiation/delithiation process and greater electronic conductivity properties. These results provide a methodology for the design of well-organized ZIFs and rare earth element-doped transition metal phosphate with a hollow polyhedron structure. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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16 pages, 4436 KiB  
Article
The Preparation and Electrochemical Pseudocapacitive Performance of Mutual Nickel Phosphide Heterostructures
by Shao-Bo Guo, Wei-Bin Zhang, Ze-Qin Yang, Xu Bao, Lun Zhang, Yao-Wen Guo, Xiong-Wei Han and Jianping Long
Crystals 2022, 12(4), 469; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12040469 - 28 Mar 2022
Cited by 4 | Viewed by 1750
Abstract
Transition metal phosphide composite materials have become an excellent choice for use in supercapacitor electrodes due to their excellent conductivity and good catalytic activity. In our study, a series of nickel phosphide heterostructure composites was prepared using a temperature-programmed phosphating method, and their [...] Read more.
Transition metal phosphide composite materials have become an excellent choice for use in supercapacitor electrodes due to their excellent conductivity and good catalytic activity. In our study, a series of nickel phosphide heterostructure composites was prepared using a temperature-programmed phosphating method, and their electrochemical performance was tested in 2 mol L−1 KOH electrolyte. Because the interface effect can increase the catalytic active sites and improve the ion transmission, the prepared Ni2P/Ni3P/Ni (Ni/P = 7:3) had a specific capacity of 321 mAh g−1 under 1 A g−1 and the prepared Ni2P/Ni5P4 (Ni/P = 5:4) had a specific capacity of 218 mAh g−1 under 1 A g−1. After the current density was increased from 0.5 A g−1 to 5 A g−1, 76% of the specific capacity was maintained. After 7000 cycles, the capacity retention rate was above 82%. Due to the phase recombination effect, the electrochemical performance of Ni2P/Ni3P/Ni and Ni2P/Ni5P4 was much better than that of single-phase N2P. After assembling the prepared composite and activated carbon into a supercapacitor, the Ni2P/Ni3P/Ni//AC had an energy density of 22 W h kg−1 and a power density of 800 W kg−1 and the Ni2P/Ni5P4//AC had an energy density of 27 W h kg−1 and a power density of 800 W kg−1. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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11 pages, 3802 KiB  
Article
Layer-by-Layer Assembly of Polyelectrolytes on Urchin-like MnO2 for Extraction of Zn2+, Cu2+ and Pb2+ from Alkaline Solutions
by Dong Chen and Zhongren Nan
Crystals 2022, 12(3), 358; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12030358 - 08 Mar 2022
Cited by 3 | Viewed by 1788
Abstract
Three-dimensional (3D) urchin-like MnO2@poly (sodium 4-styrene sulfonate) (PSS)/poly (diallyl dimethylammonium chloride) (PDDA)/PSS particles were prepared via the layer-by-layer (LBL) assembly of polyelectrolytes for the extraction of Zn2+ from alkaline media. The adsorption performance of Zn2+ on MnO2, [...] Read more.
Three-dimensional (3D) urchin-like MnO2@poly (sodium 4-styrene sulfonate) (PSS)/poly (diallyl dimethylammonium chloride) (PDDA)/PSS particles were prepared via the layer-by-layer (LBL) assembly of polyelectrolytes for the extraction of Zn2+ from alkaline media. The adsorption performance of Zn2+ on MnO2, MnO2@PSS/PDDA/PSS, and MnO2@(PSS/PDDA)3/PSS was investigated in batch experiments. The adsorption of Zn2+ on MnO2@PSS/PDDA/PSS has been studied under various conditions, such as initial Zn2+ concentration, adsorbent dosage, the solution’s pH, and reaction time. The Zn2+ adsorption process is well represented by the pseudo-second-order kinetic model, and the equilibrium data fit the Freundlich isotherm well. MnO2@PSS/PDDA/PSS also showed high efficiency for Pb2+ and Cu2+ removal from slightly alkaline water. Thus, our research provides a deep insight into the preparation of 3D manganese oxides with polyelectrolyte films for the extraction of heavy metal ions, such as Pb2+, Cu2+, and Zn2+, from slightly alkaline wastewater. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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9 pages, 2858 KiB  
Article
Boosting pH-Universal Hydrogen Evolution of FeP/CC by Anchoring Trace Platinum
by Chuancang Zhou, Feipeng Zhang and Hongyu Wu
Crystals 2022, 12(1), 37; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12010037 - 27 Dec 2021
Cited by 4 | Viewed by 1940
Abstract
To improve the electrocatalytic properties for hydrogen evolution reactions, strategies need to be adopted, such as increasing specific surface area and active site, as well as decreasing interface energy. Herein, we report the preparation of FeP on carbon cloth using a two-step process [...] Read more.
To improve the electrocatalytic properties for hydrogen evolution reactions, strategies need to be adopted, such as increasing specific surface area and active site, as well as decreasing interface energy. Herein, we report the preparation of FeP on carbon cloth using a two-step process of hydrothermal and phosphating. Otherwise, to utilize the excellent catalytic performance of Pt and decrease consumption of Pt, the hyperdispersed Pt nanoparticles for the sake of modifying transition-metal phosphides film were designed and fabricated. Finally, 3D FeP-Pt/CC was successfully prepared by means of electro-deposition using three electrodes. The crystalline structure, surface morphology and elemental composition of the synthesized samples have been investigated by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) and energy dispersive X-ray analysis (EDS). The XRD results show that the as-prepared products are of orthorhombic FeP structure, and EDS results indicate that there exist Pt elements in 3D FeP-Pt/CC. The electrocatalytic performances were evaluated by, such as linear scan voltammetry, tafel plots and electrochemical impedance spectroscopy on electrochemical workstations. These results show that the FeP-Pt/CC exhibit a current density of 10 mA·cm−2 at an over-potential of 58 mV for HER in 0.5 M H2SO4, which is very close to the values of 20%Pt/C which was previously reported. FeP-Pt/CC has excellent durability. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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14 pages, 3780 KiB  
Article
Electrochemical In Situ Fabrication of Titanium Dioxide Nanotubes on a Titanium Wire as a Fiber Coating for Solid-Phase Microextraction of Polycyclic Aromatic Hydrocarbons
by Mingguang Ma, Yunxia Wei, Jie Chen and Qiong Shang
Crystals 2021, 11(11), 1384; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst11111384 - 12 Nov 2021
Cited by 3 | Viewed by 1460
Abstract
A novel titanium dioxide nanotube (TiO2NTS) coated fiber for solid-phase microextraction (SPME) was prepared by in situ anodization of titanium wire in electrolyte containing ethylene glycol and ammonium fluoride (NH4F). The effects of different electrolyte solutions (NH4F [...] Read more.
A novel titanium dioxide nanotube (TiO2NTS) coated fiber for solid-phase microextraction (SPME) was prepared by in situ anodization of titanium wire in electrolyte containing ethylene glycol and ammonium fluoride (NH4F). The effects of different electrolyte solutions (NH4F and ethylene glycol) and oxidation voltages on the formation and size of TiO2NTs was studied. It was obtained from the experiment that TiO2NTs arrays were arranged with a wall thickness of 25 nm and the diameter of 100 nm pores in ethylene glycol and water (v/v, 1:1) containing NH4F of 0.5% (w/v) with a voltage of 20 V at 25 °C for 30 min. The TiO2NTs were used as solid-phase microextraction fiber coatings coupled with high-performance liquid chromatography (HPLC) in sensitive determination of polycyclic aromatic hydrocarbons (PAHs) in spiked real samples water. Under the optimized SPME conditions, the calibration curve has good linearity in the range of 0.20–500 μg·L−1, and the correlation coefficient (R2) is between 0.9980 and 0.9991. Relative standard deviations (RSDs) of 3.5–4.7% (n = 5) for single fiber repeatability and of 5.2% to 7.9% for fiber-to-fiber reproducibility (n = 3) was obtained. The limits of detection (LOD) (S/N = 3) and limits of quantification (LOQ) (S/N = 10) of PAHs were 0.03–0.05 µg·L−1 and 0.12–0.18 µg·L−1. The developed method was applied to the preconcentration and determination of trace PAHs in spiked real samples of water with good recoveries from 78.6% to 119% and RSDs from 4.3 to 8.9%, respectively. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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Review

Jump to: Editorial, Research

38 pages, 16683 KiB  
Review
Research Progress on MXene-Based Flexible Supercapacitors: A Review
by Baoshou Shen, Rong Hao, Yuting Huang, Zhongming Guo and Xiaoli Zhu
Crystals 2022, 12(8), 1099; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12081099 - 05 Aug 2022
Cited by 6 | Viewed by 3566
Abstract
The increasing demands for portable, intelligent, and wearable electronics have significantly promoted the development of flexible supercapacitors (SCs) with features such as a long lifespan, a high degree of flexibility, and safety. MXenes, a class of unique two-dimensional materials with excellent physical and [...] Read more.
The increasing demands for portable, intelligent, and wearable electronics have significantly promoted the development of flexible supercapacitors (SCs) with features such as a long lifespan, a high degree of flexibility, and safety. MXenes, a class of unique two-dimensional materials with excellent physical and chemical properties, have been extensively studied as electrode materials for SCs. However, there is little literature that systematically summarizes MXene-based flexible SCs according to different flexible electrode construction methods. Recent progress in flexible electrode fabrication and its application to SCs is reviewed according to different flexible electrode construction methods based on MXenes and their composite electrodes, with or without substrate support. The fabrication methods of flexible electrodes, electrochemical performance, and the related influencing factors of MXene-based flexible SCs are summarized and discussed in detail. In addition, the future possibilities of flexible SCs based on MXene are explored and presented. Full article
(This article belongs to the Special Issue Emerging Low-Dimensional Materials)
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