Lithium‐sulfur (Li‐S) batteries are one of the most promising next‐generation energy‐storage systems. Nevertheless, the sluggish sulfur redox and shuttle effect in Li‐S batteries are the major obstacles to their commercial application. Previous investigations on adsorption for LiPSs have made great progress but cannot restrain the shuttle effect. Catalysts can enhance the reaction kinetics, and then alleviate the shuttle effect. The synergistic relationship between adsorption and catalysis has become the hotspot for research into suppressing the shuttle effect and improving battery performance. Herein, the adsorption‐catalysis synergy in Li‐S batteries is reviewed, the adsorption‐catalysis designs are divided into four categories: adsorption‐catalysis for LiPSs aggregation, polythionate or thiosulfate generation, and sulfur radical formation, as well as other adsorption‐catalysis. Then advanced strategies, future perspectives, and challenges are proposed to aim at long‐life and high‐efficiency Li‐S batteries.
Safety, nontoxicity, and durability directly determine the applicability of the essential characteristics of the lithium (Li)‐ion battery. Particularly, for the lithium–sulfur battery, due to the low ignition temperature of sulfur, metal lithium as the anode material, and the use of flammable organic electrolytes, addressing security problems is of increased difficulty. In the past few years, two basic electrolyte systems are studied extensively to solve the notorious safety issues. One system is the conventional organic liquid electrolyte, and the other is the inorganic solid‐state or quasi‐solid‐state composite electrolyte. Here, the recent development of engineered liquid electrolytes and design considerations for solid electrolytes in tackling these safety issues are reviewed to ensure the safety of electrolyte systems between sulfur cathode materials and the lithium‐metal anode. Specifically, strategies for designing and modifying liquid electrolytes including introducing gas evolution, flame, aqueous, and dendrite‐free electrolytes are proposed. Moreover, the considerations involving a high‐performance Li+ conductor, air‐stable Li+ conductors, and stable interface performance between the sulfur cathode and the lithium anode for developing all‐solid‐state electrolytes are discussed. In the end, an outlook for future directions to offer reliable electrolyte systems is presented for the development of commercially viable lithium–sulfur batteries.
despite all these promises, three intrinsic drawbacks need to be resolved before fulfilling the promise of the market potential.First, the most stable but electronically insulating S 8 (≈10 −14 S cm −2 ) with cyclic configuration is used as the starting material in Li-S cathode, significantly limiting the full utilization of the active materials to reach the theoretical capacity. Therefore, it is the first priority to design the cathode that ensures the maximum usage of the starting materials, which sets the upper limit of the capacity performance. Second, the muti-step reduction process releases highly soluble lithium polysulfides (LiPSs) intermediates (Li 2 S x , where x = 4-8) into the organic electrolyte. [6] Unlike the batteries based on ion-insertion mechanism, [7,8] Li-S battery possesses unique and complex electrochemical/chemical processes during operation. During galvanostatic discharge process, two distinct plateaus can be verified at about 2.4 and 2.1 V in the voltage profile, corresponding to the reduction of sulfur into long-chain polysulfides and subsequent reaction from short-chain polysulfides to Li 2 S, respectively. [9] Further investigations about the reaction mechanism of Li-S battery based on experimental and theoretical studies reveal that the existence of various intermediates during electrochemical processes, indicating much more complex battery chemistry compared to the simple stepwise reaction model. [10,11] As a result, the soluble intermediates can diffuse through the polymeric separator to the anode surface, causing the loss of active materials and degradation of anode. Third, the density difference between the starting material (sulfur, 2.07 g cm −3 ) and discharge product (Li 2 S, 1.66 g cm −3 ) causes significant volumetric change during continuous cycling, damaging the integrity of the cathode structure and leading to serious capacity fading. [12] Besides above problems concerning the cathode side of the Li-S battery, other issues arose on the anode side, such as the unstable solid-electrolyte interphase (SEI), surface passivation, and uncontrolled lithium dendrite growth. [13][14][15] Stemmed from the basic problems mentioned above from the very beginning of the designed Li-S battery systems, various derivative problems were gradually unraveled during persistent efforts for improving the battery performance to approach the ultimate goal for commercialization. In the past decade, fundamental studies about Li-S battery were carried in laboratories all over the world, and it gradually put the puzzle together while brought promising performance improvement. [11,[16][17][18][19][20] However, to date, most of the lab-scale progresses have been based on batteries with sulfur loading lower than 2 mg cm −2 , Lithium-sulfur (Li-S) batteries, due to the high theoretical energy density, are regarded as one of the most promising candidates for breaking the limitations of energy-storage system based on Li-ion batteries. Tremendous efforts have been made to meet the challenge of high-performan...
With the continuous exploration of 2D transition metal dichalcogenides (TMDs), novel high‐performance devices based on the remarkable electronic and optoelectronic natures of 2D TMDs are increasingly emerging. As fresh blood of 2D TMD family, anisotropic MTe2 and ReX2 (M = Mo, W, and X = S, Se) have drawn increasing attention owing to their low‐symmetry structures and charming properties of mechanics, electronics, and optoelectronics, which are suitable for the applications of field‐effect transistors (FETs), photodetectors, thermoelectric and piezoelectric applications, especially catering to anisotropic devices. Herein, a comprehensive review is introduced, concentrating on their recent progresses and various applications in recent years. First, the crystalline structure and the origin of the strong anisotropy characterized by various techniques are discussed. Specifically, the preparation of these 2D materials is presented and various growth methods are summarized. Then, high‐performance applications of these anisotropic TMDs, including FETs, photodetectors, and thermoelectric and piezoelectric applications are discussed. Finally, the conclusion and outlook of these applications are proposed.
Two‐dimensional (2D) materials, benefitting from their unique planar structure and various appealing electronic properties, have attracted much attention for novel electronic and optoelectronic applications. As a basis for practical devices, the study of micro/nano‐2D material arrays based on coupling effects and synergistic effects is critical to the functionalization and integration of 2D materials. Moreover, micro/nano‐2D material arrays are compatible with traditional complementary metal oxide semiconductor (CMOS) electronics, catering well to high‐integration, high‐sensitivity, and low‐cost sensing and imaging systems. This review presents some recent studies on 2D material arrays in sequence from their novel preparations to high‐integration applications as well as explorations on dimension tuning. A first focus is on various typical fabrication methods for 2D material arrays, including photolithography, 2D printing, seeded growth, van der Waals epitaxial growth, and self‐assembly. Then, the applications of 2D material arrays, such as field effect transistors, photodetectors, pressure sensors, as well as flexible electronic devices of photodetectors and strain sensors, are elaborately introduced. Furthermore, the recent burgeoning exploration of mixed‐dimensional heterostructure arrays including 0D/2D, 1D/2D, and 3D/2D is discussed. Ultimately, conclusions and an outlook based on the current developments in this promising field are presented.
It is a rapidly developed subject in expanding the fundamental properties and application of two‐dimensional (2D) materials. The weak van der Waals interaction in 2D materials inspired researchers to explore 2D heterostructures (2DHs) based broadband photodetectors in the far‐infrared (IR) and middle‐IR regions with high response and high detectivity. This review focuses on the strategy and motivation of designing 2DHs based high‐performance IR photodetectors, which provides a wide view of this field and new expectation for advanced photodetectors. First, the photocarriers' generation mechanism and frequently employed device structures are presented. Then, the 2DHs are divided into semimetal/semiconductor 2DHs, semiconductor/semiconductor 2DHs, and multidimensional semi‐2DHs; the advantages, motivation, mechanism, recent progress, and outlook are discussed. Finally, the challenges for next‐generation photodetectors are described for this rapidly developing field.
Ternary two‐dimensional (2D) semiconductors with controllable wide bandgap, high ultraviolet (UV) absorption coefficient, and critical tuning freedom degree of stoichiometry variation have a great application prospect for UV detection. However, as‐reported ternary 2D semiconductors often possess a bandgap below 3.0 eV, which must be further enlarged to achieve comprehensively improved UV, especially deep‐UV (DUV), detection capacity. Herein, sub‐one‐unit‐cell 2D monolayer BiOBr nanoflakes (≈0.57 nm) with a large size of 70 µm are synthesized for high‐performance DUV detection due to the large bandgap of 3.69 eV. Phototransistors based on the 2D ultrathin BiOBr nanoflakes deliver remarkable DUV detection performance including ultrahigh photoresponsivity (Rλ, 12739.13 A W−1), ultrahigh external quantum efficiency (EQE, 6.46 × 106%), and excellent detectivity (D*, 8.37 × 1012 Jones) at 245 nm with a gate voltage (Vg) of 35 V attributed to the photogating effects. The ultrafast response (τrise = 102 µs) can be achieved by utilizing photoconduction effects at Vg of −40 V. The combination of photocurrent generation mechanisms for BiOBr‐based phototransistors controlled by Vg can pave a way for designing novel 2D optoelectronic materials to achieve optimal device performance.
The electrochemical nitrogen reduction reaction (NRR), as an environmentally friendly method to convert nitrogen to ammonia at ambient temperature and pressure, has attracted the attention of numerous researchers. However, when compared with industrial production, electrochemical NRR often suffers from unsatisfactory yields and poor Faraday efficiency (FE). Recently, various structure engineering strategies have aimed to introduce extra active sites or enhance intrinsic activity to optimize the activation and hydrogenation of N2. In this review, recent progress in atomic structure modification is summarized and discussed to design high‐efficiency NRR catalysts, with a focus on defect engineering (heteroatom doping and atom vacancy), surface orientation and amorphization, as well as heterostructure engineering. In addition, existing challenges and future development directions are proposed to obtain more credible NRR catalysts with high catalytic performance and selectivity.
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