Recent Progress in MXene‐Based Materials: Potential High‐Performance Electrocatalysts

The family of transition metal carbides, nitrides, and carbonitrides (collectively called MXenes) has been a thriving field since the first invention of Ti₃C₂T_x (MXene) in 2011. MXene is a new type of nanometer 2D sheet material, which exhibits great application potentials in various fields due to its multiple advantages such as high specific surface area, good electrical conductivity, and high mechanical strength. Electrocatalysis is regarded as the core of future clean energy conversion technologies, and MXene‐based materials provide inspiration for the design and preparation of electrocatalysts with high activity, high selectivity, and long loading life time. The applications of MXene‐based materials in electrocatalysis, including hydrogen evolution reaction, nitrogen reduction reaction, oxygen evolution reaction, oxygen reduction reaction, carbon dioxide reduction reaction, and methanol oxidation reaction are summarized in this review. As a crucial session regarding experiments, the current safer and more environmentally friendly preparation methods of MXene are also discussed. Focusing on the materials design and enhancement methods, the key challenges and opportunities for MXene‐based materials as a next‐generation platform in both fundamental research and practical electrocatalysis applications are presented. This account serves to promote future efforts toward the development of MXenes and related materials in the electrocatalysis applications.     

Flexible MXene-Based Composites for Wearable Devices

In recent decades, flexible and wearable devices have been extensively investigated due to their promising applications in portable mobile electronics and human motion monitoring. MXene, a novel growing family of 2D nanomaterials, demonstrates superiorities such as outstanding electrical conductivity, abundant terminal groups, unique layered-structure, large surface area, and hydrophilicity, making it to be a potential candidate material for flexible and wearable devices. Numerous pioneering works are devoted to develop flexible MXene-based composites with various functions and designed structures. Therefore, the latest progress of the flexible MXene-based composites for wearable devices is summarized in this review, focusing on the preparation strategies, working mechanisms, performances, and applications in sensors, supercapacitors, and electromagnetic interference shielding materials. Moreover, the current challenges and future outlooks are also discussed.     

Challenges and Prospects of All-Solid-State Electrodes for Solid-State Lithium Batteries

In the development of all-solid-state lithium batteries (ASSLB), progress is made with solid-state electrolytes; however, challenges regarding compatibility and stability still exist with solid electrodes. These issues result in a low battery capacity and short cycle life, which limit the commercial application of ASSLBs. This review summarizes the recent research progress on solid-state electrodes in ASSLBs including the solid–solid interface phenomena such as the interface between electrode materials and electrolytes. The mechanical stability problems in solid electrodes, including fracture, brittleness, and deformation of electrode materials, are also discussed, and corresponding methods to measure the solid electrode stress are provided. In addition, strategies for mitigating stress-related issues are examined. Finally, the fabrication process of solid electrodes is introduced and their future developments, including the exploration of new electrode materials and the design of more intelligent electrode structures, are proposed.     

3D Porous Oxidation-Resistant MXene/Graphene Architectures Induced by In Situ Zinc Template toward High-Performance Supercapacitors

2D MXene materials have attracted intensive attention in energy storage application. However, MXene usually undergoes serious face-to-face restacking and inferior stability, significantly preventing its further commercial application. Herein, to suppress the oxidation and self-restacking of MXene, an efficient and fast self-assembly route to prepare a 3D porous oxidation-resistant MXene/graphene (PMG) composite with the assistance of an in situ sacrificial metallic zinc template is demonstrated. The self-assembled 3D porous architecture can effectively prevent the oxidation of MXene layers with no evident variation in electrical conductivity in air at room temperature after two months, guaranteeing outstanding electrical conductivity and abundant electrochemical active sites accessible to electrolyte ions. Consequently, the PMG-5 electrode possesses a striking specific capacitance of 393 F g⁻¹, superb rate performance (32.7% at 10 V s⁻¹), and outstanding cycling stability. Furthermore, the as-assembled asymmetric supercapacitor possesses a pronounced energy density of 50.8 Wh kg⁻¹ and remarkable cycling stability with a 4.3% deterioration of specific capacitance after 10 000 cycles. This work paves a new avenue to solve the two long-standing significant challenges of MXene in the future.     

Graphene and MXene Nanomaterials: Toward High‐Performance Electromagnetic Wave Absorption in Gigahertz Band Range

Searching for advanced microwave absorption (MA) nanomaterials is one of the most feasible ways to address the increasing electromagnetic pollution in both military and civil fields. To this end, graphene and MXene have won the widespread attention as the main representatives due to their remarkable structures and properties. The common features such as the large aspect ratio, active chemical surface, and varieties of synthesis processes endow graphene and MXene with unique superiorities for developing high‐efficiency MA structures, in particular lightweight assemblies and various hybrids. Meanwhile, the structural and performance differences (such as different conductivities) between them result in distinctive techniques in the design, fabrication, and application of their MA materials. Herein, the research progress in graphene‐ and MXene‐based MA materials is reviewed, with a special focus on advances in general strategies. Moreover, through the comparison between graphene‐ and MXene‐based MA materials, their respective advantages in achieving high‐performance MA are presented. Furthermore, the future challenge, research orientation, and prospect for these MA materials are also highlighted and discussed.     

Rational Design of Transition Metal Phosphide-Based Electrocatalysts for Hydrogen Evolution

Developing efficient and inexpensive electrocatalysts for the hydrogen evolution reaction (HER) is critical to the commercial viability of electrochemical clean energy technologies. Transition metal phosphides (TMPs), with the merits of abundant reserves, unique structure, tunable composition, and high electronic conductivity, are recognized as attractive HER catalytic materials. Nevertheless, the HER electrocatalytic activity of TMPs is still limited by various thorough issues and inherent performance bottlenecks. In this review, these issues are carefully sorted, and the corresponding reasonable explanations and solutions are elucidated on the basis of the HER catalytic activity origins of TMPs. Subsequently, highly targeted multiscale strategies to improve the HER performance of TMPs are comprehensively presented. Additionally, critical scientific issues for constructing high-efficiency TMP-based electrocatalysts are proposed. Finally, the HER reaction process, catalytic mechanism research, TMP-based catalyst construction, and their application expansion are mentioned as challenges and future directions for this research field. Expectedly, this review offers professional and targeted guidelines for the rational design and practical application of TMP-based HER catalysts.     

Recently advances in flexible zinc ion batteries

Flexible batteries are key component of wearable electronic devices.Based on the requirements of medical and primary safety of wearable energy storage devices,rechargeable aqueous zinc ion batteries (ZIBs) are promising portable candid-ates in virtue of its intrinsic safety,abundant storage and low cost.However,many inherent challenges have greatly hindered the development in flexible Zn-based energy storage devices,such as rigid current collector and/or metal anode,easily de-tached cathode materials and a relatively narrow voltage window of flexible electrolyte.Thus,overcoming these challenges and further developing flexible ZIBs are inevitable and imperative.This review summarizes the most advanced progress in designs and discusses of flexible electrode,electrolyte and the practical application of flexible ZIBs in different environments.We also exhibit the heart of the matter that current flexible ZIBs faces.Finally,some prospective approaches are proposed to ad-dress these key issues and point out the direction for the future development of flexible ZIBs.     

Engineering 3D Ion Transport Channels for Flexible MXene Films with Superior Capacitive Performance

2D MXene materials are of considerable interest for future energy storage. A MXene film could be used as an effective flexible supercapacitor electrode due to its flexibility and, more importantly, its high specific capacitance. However, although it has excellent electronic conductivity, sluggish ionic kinetics within the MXene film becomes a fundamental limitation to the electrochemical performance. To compensate for the relative deficiency, MXene films are frequently reduced to several micrometer dimensions with low mass loading (<1 mg cm^?2), to the point of detriment of areal performance and commercial value. Herein, for the first time, the design of a 3D porous MXene/bacterial cellulose (BC) self‐supporting film is reported for ultrahigh capacitance performance (416 F g^?1, 2084 mF cm^?2) with outstanding mechanical properties and high flexibility, even when the MXene loading reaches 5 mg cm^?2. The highly interconnected MXene/BC network enables both excellent electron and ion transport channel. Additionally, a maximum energy density of 252 µWh cm^?2 is achieved in an asymmetric supercapacitor, higher than that of all ever‐reported MXene‐based supercapacitors. This work exploits a simple route for assembling 2D MXene materials into 3D porous films as state‐of‐the‐art electrodes for high performance energy storage devices.     

过渡金属碳氮化合物(MXenes)在能量储存装置的研究进展

层状过渡金属碳化物和/或氮化物(MXenes)凭借其特有的结构和性能成为了新型储能装置电极催化剂的重要候选材料。MXenes的表达式一般为Mn+1 Xn Tx,其中“M”代表早期的过渡金属元素,“x”表示C、N或CN,而“Tx”为“-OH”、“-F”等基团,n的值一般为1,2或3。MXenes具有比表面积高、离子电导率大、亲水性好等优良特性,有利于其在离子电池、超级电容器等储能装置中应用推广。本文综述了近几年MXenes在能源储存装置中的应用及研究现状,归纳总结了MXenes的结构及能量储存机制,指出了目前研究过程中存在的短板,并对其发展方向进行展望。     

Recent advances in MXene for terahertz applications

Since first synthesized in 2011, MXenes have attracted extensive attention in many scientific fields as a new two-dimensional(2D) material because of the unique physical and chemical properties. Over the past decade, in particular, MXenes have obtained numerous exciting achievements in the field of terahertz applications. In this review, we first briefly introduce the MXene materials, such as the basic structure and main fabrication processes of MXenes. Then, we summarize the recent applications...     

Engineered Polymeric Carbon Nitride Additive for Energy Storage Materials: A Review

The ever-increasing demands for high energy density electronics have motivated research on exploring new types of electrode materials featuring mechanical flexibility and electrical storage capability. Of these, polymeric carbon nitride (PCN) has been increasingly studied in regard to electrical energy storage (EES) because of its abundant pyridinic N content, which is beneficial for enhancing electrochemical performance. However, state-of-the-art PCN-based electrode materials for EES are still far from industrial requirements. Herein, the current status of PCN-based materials in batteries and supercapacitors (SCs) is primarily discussed. A particular emphasis is placed on the PCN processing into composite electrode materials, including the defect engineering of pristine PCN and its coupling with other conductive materials to develop heterojunction nanostructures, which is essential for developing highly efficient electrode materials. Moreover, the direct pyrolysis of PCN into N-doped graphene with a tunable N content is introduced and achieves remarkable energy storage performance with superior electronic conductivity. Furthermore, the energy storage mechanisms for batteries and SCs are also highlighted to reveal structure–performance relationship. Finally, this comprehensive review outlines the remaining challenges and strategies for future improvements in PCN-based materials in this emerging field. This review will provide inspiration on developing future PCN-based materials for EES.     

A Review of Emerging Dual-Ion Batteries: Fundamentals and Recent Advances

Dual-ion batteries (DIBs), based on the working mechanism involving the storage of cations and anions separately in the anode and cathode during the charging/discharging process, are of great interest beyond lithium-ion batteries (LIBs) in high-efficiency energy storage due to the merits of high working voltage, material availability, as well as low cost and excellent safety. Despite the progress achieved, the practical applications of DIBs are still hindered by negative issues, such as limited capacity and cyclic stability, which triggers the development of suitable electrode materials with highly reversible capacities, and corresponding electrolytes with high oxidative stability as well as sufficient reaction kinetics of active ions. Herein, in this article, a systematic and comprehensive review of fundamentals and recent advances in current DIBs with subcategories of cathode materials, anode materials, and electrolytes are presented. In particular, their energy storage mechanisms, as well as their respective features, are dissected. Furthermore, some strategies and perspectives are proposed for facilitating the further development of DIBs in the future.     

Controlled Assembly of MXene Nanosheets as an Electrode and Active Layer for High-Performance Electronic Skin

MXenes are an emerging class of 2D transition metal carbides and nitrides. They have been widely used in flexible electronics owing to their excellent conductivity, mechanical flexibility, and water dispersibility. In this study, the electrode and active layer applications of MXene materials in electronic skins are realized. By utilizing vacuum filtration technology, few-layer MXene electrodes are integrated onto the top and bottom surfaces of the 3D polyacrylonitrile (PAN) network to form a stable electronic skin. The fabricated flexible device with Ti₃C₂T_x MXene electrodes outperforms those with other electrodes and exhibits excellent device performance, with a high sensitivity of 104.0 kPa⁻¹, fast response/recovery time of 30/20 ms, and a low detection limit of 1.5 Pa. Furthermore, the electrode and the constructed MXene/PAN-based flexible pressure sensor exhibit robust mechanical stability and can survive 240 bending cycles. Such a robust, flexible device can be enlarged or folded like a jigsaw puzzle or origami and transformed from 2D to 3D structures; moreover, it can detect tiny movements of human muscles, such as movements corresponding to sound production and intense movements during bending of fingers.     

Engineering Aggregation-Resistant MXene Nanosheets As Highly Conductive and Stable Inks for All-Printed Electronics

MXenes are interesting 2D materials that have been considered as attractive frontier materials for potential applications in the fields of energy and electronic devices due to their excellent optoelectronic properties including metallic conductivity and high optical transparency. However, it is still challenging to achieve compatibility for the as-synthesized MXene nanosheets with simple solution-deposition and patterning processes because of their limited solubility in many solvents. Here, a promising strategy is developed for obtaining alcohol-dispersible MXene nanosheets suitable for all-printed electronics while enhancing their electrical conductivity. This strategy includes a trifluoroacetic acid treatment—applied in order to contribute to the modification of intercalants between the MXene nanosheets—and achieves long-term dispersion of the MXene in alcoholic media and balanced jetting conditions during the electrohydrodynamic printing process. Furthermore, the high conductivity levels of the treated MXenes allow their printed patterns to be applied as gate and source/drain electrodes in all-printed logic circuits, displaying good and robust operation in transistors, inverters, and NAND, and NOR logic gates. This study provides a promising approach for modifying MXene nanosheets with the purpose of achieving desirable properties suitable for large-area printing processes, suggesting the feasibility of using MXene in practical applications involving all-printed electronics.     

Alternating‐Current MXene Polymer Light‐Emitting Diodes

MXenes (Ti₃C₂) are 2D transition‐metal carbides and carbonitrides with high conductivity and optical transparency. However, transparent MXene electrodes suitable for polymer light‐emitting diodes (PLEDs) have rarely been demonstrated. With the discovery of the excellent electrical stability of MXene under an alternating current (AC), herein, PLEDs that employ MXene electrodes and exhibit high performance under AC operation (AC MXene PLEDs) are presented. The PLED exhibits a turn‐on voltage, current efficiency, and brightness of 2.1 V, 7 cd A^?1, and 12 547 cd m^?2, respectively, when operated under AC with a frequency of 1 kHz. The results indicate that the undesirable electric breakdown associated with heat arising from the poor interface of the MXene with a hole transport layer in the direct‐current mode is efficiently suppressed by the transient injection of carriers accompanied by the alternating change of the electric polarity under the AC, giving rise to reliable light emission with a high efficiency. The solution‐processable MXene electrode can be readily fabricated on a flexible polymer substrate, allowing for the development of a mechanically flexible AC MXene PLED with a higher performance than flexible PLEDs employing solution‐processed nanomaterial‐based electrodes such as carbon nanotubes, reduced graphene oxide, and Ag nanowires.     

Nanoarchitectured Design of Vertical-Standing Arrays for Supercapacitors: Progress,Challenges, and Perspectives

Vertical-standing arrays have aroused great enthusiasm as electrode materials for supercapacitors in recent years owing to their structural and compositional characteristics. Although significant efforts have been made in the construction of vertical-standing arrays with tailored compositions and architectures, an in-depth understanding of the relevant structure–activity relationships has not yet been reviewed in detail. Herein, recent important progress in controllably synthesizing vertical-standing arrays as well as their application as supercapacitors is reviewed. Afterward, promising strategies to improve the electrochemical performance of vertical-standing arrays are discussed. Finally, the challenges and possible directions for developing vertical-standing arrays with outstanding performance are outlined. This review provides important guidelines for designing and regulating vertical-standing arrays and constructing desirable electrode materials for future electrochemical energy storage.     

Complex Hydrides for Electrochemical Energy Storage

Complex hydrides have energy storage‐related functions such as i) solid‐state hydrogen storage, ii) electrochemical Li storage, and iii) fast Li‐ and Na‐ionic conductions. Here, recent progress on the development of fast Li‐ionic conductors based on the complex hydrides is reported. The validity of using them as electrolytes in all‐solid‐state lithium rechargeable batteries is also examined. Not only coated oxides but also bare sulfides are found to be applicable as positive electrode active materials. Results related to fast Na‐ionic conductivity in the complex hydrides are presented. In the last section, the future prospects for battery assemblies with high‐energy densities, and Mg ion batteries with the liquid and the solid‐state electrolytes are discussed.     

Rational Design of Electrode Materials for Advanced Supercapacitors: From Lab Research to Commercialization

Supercapacitors can harvest electrical energy from intermittent sources and transfer it quickly, but their specific energy must be raised if they are applied to efficiently power wearable and flexible electronics, as well as larger equipment. However, the remaining big gap between the lab research and practical applications seriously hinders the further progress of advanced supercapacitors, especially for electrode materials. Consequently, from a commercial/usable perspective, a clear guideline from lab research to commercialization is highly desired for bringing advanced supercapacitors from basic research into reality. This review focuses on the key factors of advanced supercapacitors from lab research to commercialization and summarizes recent progress in the field of supercapacitors as well as outlines key perspectives for future research. First, the several energy storage mechanisms are illustrated for building better supercapacitors. Then, the up-to-date key achievements and progresses of smart methods toward high-energy supercapacitors and effective strategies for commercial-level mass-loading as well as high packing density electrodes are summarized and commented upon. Also, integrated systems of supercapacitors and application fields of commercial supercapacitors are also highlighted. Subsequently, future research directions are presented here to guide research toward the commercialization of advanced supercapacitors.     

Inkjet Printing of Self‐Assembled 2D Titanium Carbide and Protein Electrodes for Stimuli‐Responsive Electromagnetic Shielding

2D titanium carbides (MXene) possess significant characteristics including high conductivity and electromagnetic interference shielding efficiency (EMI SE) that are important for applications in printed and flexible electronics. However, MXene‐based ink formulations are yet to be demonstrated for proper inkjet printing of MXene patterns. Here, tandem repeat synthetic proteins based on squid ring teeth (SRT) are employed as templates of molecular self‐assembly to engineer MXene inks that can be printed as stimuli‐responsive electrodes on various substrates including cellulose paper, glass, and flexible polyethylene terephthalate (PET). MXene electrodes printed on PET substrates are able to display electrical conductivity values as high as 1080 ± 175 S cm^?1, which significantly exceeds electrical conductivity values of state‐of‐the‐art inkjet‐printed electrodes composed of other 2D materials including graphene (250 S cm^?1) and reduced graphene oxide (340 S cm^?1). Furthermore, this high electrical conductivity is sustained under excessive bending deformation. These flexible electrodes also exhibit effective EMI SE values reaching 50 dB at films with thicknesses of 1.35 µm, which mainly originate from their high electrical conductivity and layered structure.     

A Novel Approach for Achieving High‐Efficiency Photoelectrochemical Water Oxidation in InGaN Nanorods Grown on Si System: MXene Nanosheets as Multifunctional Interfacial Modifier

MXene nanosheets with attractive electrical conductivity and tunable work function have been adopted as multifunctional interfacial modifier between InGaN nanorods and Si for photoelectrochemical water oxidation for the first time. Compared to bare InGaN/Si systems, MXene interfacial layers give rise to an ultralow onset potential of 75 mV versus reversible hydrogen electrode (RHE), which is the highest ever reported for InGaN‐ or Si‐based photoanodes by interfacial modification. Furthermore, the modified photoanode exhibits a significantly enhanced photocurrent density (7.27 mA cm^?2) at 1.23 V versus RHE, which is about 10 times higher than that achieved with the InGaN/Si photoanode. The detailed mechanism demonstrates that the formed type‐II band alignment in InGaN/MXene heterojunction and an Ohmic junction at the MXene/Si interface make MXene an ideal electron‐migration channel to enhance charge separation and transfer process. This synergetic effect of MXene can significantly decrease the charge resistance at semiconductor/Si and semiconductor/electrolyte hetero‐interfaces, eventually resulting in the fast hole injection efficiency of 82% and superior stability against photocorrosion. This work not only provides valuable guidance for designing high‐efficiency photoelectrodes through the integration of multiscale and multifunctional materials, but also presents a novel strategy for achieving high‐performance artificial photosynthesis by introducing interfacial modifier.