Multifunctional SnO2 QDs/MXene Heterostructures as Laminar Interlayers for Improved Polysulfide Conversion and Lithium Plating Behavior.

Poor cycling stability in lithium-sulfur (Li-S) batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures. Heterogeneous catalysis has emerged as a promising approach, leveraging the adsorption and catalytic performance on lithium polysulfides (LiPSs) to inhibit LiPSs shuttling and improve redox kinetics. In this study, we report an ultrathin and laminar SnO2@MXene heterostructure interlayer (SnO2@MX), where SnO2 quantum dots (QDs) are uniformly distributed across the MXene layer. The combined structure of SnO2 QDs and MXene, along with the creation of numerous active boundary sites with coordination electron environments, plays a critical role in manipulating the catalytic kinetics of sulfur species. The Li-S cell with the SnO2@MX-modified separator not only demonstrates superior electrochemical performance compared to cells with a bare separator but also induces homogeneous Li deposition during cycling. As a result, an areal capacity of 7.6 mAh cm-2 under a sulfur loading of 7.5 mg cm-2 and a high stability over 500 cycles are achieved. Our work demonstrates a feasible strategy of utilizing a laminar separator interlayer for advanced Li-S batteries awaiting commercialization and may shed light on the understanding of heterostructure catalysis with enhanced reaction kinetics.

Stable MXene Dough with Ultrahigh Solid Fraction and Excellent Redispersibility toward Efficient Solution Processing and Industrialization.

Two-dimensional (2D) transition metal carbides, and/or nitrides, so-called MXenes, have triggered intensive research interests in applications ranging from electrochemical energy storage to electronics devices. Producing these functional devices by printing necessitates to match the rheological properties of MXene dispersions to the requirements of various solution processing techniques. In particular, for additive manufacturing such as extrusion-printing, MXene inks with high solid fraction are typically required, which is commonly achieved by tediously removing excessive free water (top-down route). Here, the study reports on a bottom-up route to reach a highly concentrated binary MXene-water blend, so-called MXene dough, by controlling the water admixture to freeze-dried MXene flakes by exposure to water mist. The existence of a critical threshold of MXene solid content (≈60%), beyond which no dough is formed, or formed with compromised ductility is revealed. Such metallic MXene dough possesses high electrical conductivity, excellent oxidation stability, and can withstand a couple of months without apparent decay, providing that the MXene dough is properly stored at low-temperature with suppressed dehydration environment. Solution processing of the MXene dough into a micro-supercapacitor with gravimetric capacitance of 161.7 F g-1 is demonstrated. The impressive chemical and physical stability/redispersibility of MXene dough indicate its great promise in future commercialization.

Co-doped g-C3N4 nanotube decorated separators mediate polysulfide redox for high performance lithium sulfur batteries.

The main issue with lithium-sulfur (Li-S) batteries is the serious irreversible capacity loss caused by the polysulfide shuttle process. In this work, we propose an electro-catalytic strategy for absorbing and transferring long-chain polysulfides during the redox process, which is the key to improving the utilization of S. Reported here is a Co doped tubular g-C3N4 (CN) modified separator (Co-TCN@PP), which successfully inhibited the polysulfide shuttle by physical absorption and catalysis, thus facilitating the high utilization of S. Co-TCN with a tube-like structure ensures the uniform dispersion of Co nanoparticles, which provides abundant active sites to absorb polysulfides. Furthermore, Co-TCN exhibits fast reaction kinetics for polysulfide conversion. A Li-S battery with Co-TCN@PP achieves superior rate capacities and a long cycle life (400 times) with capacity fading as low as 0.07% per cycle at a high Li+ insertion/extraction rate of 2C. Moreover, electrodes with a high sulfur loading of 5.6 mg cm-2 can be realized by adopting the Co-TCN@PP separator.

Rational Design of Ti3C2Tx MXene Inks for Conductive, Transparent Films.

Transparent conductive electrodes (TCEs) with a high figure of merit (FOMe, defined as the ratio of transmittance to sheet resistance) are crucial for transparent electronic devices, such as touch screens, micro-supercapacitors, and transparent antennas. Two-dimensional (2D) titanium carbide (Ti3C2Tx), known as MXene, possesses metallic conductivity and a hydrophilic surface, suggesting dispersion stability of MXenes in aqueous media allowing the fabrication of MXene-based TCEs by solution processing. However, achieving high FOMe MXene TCEs has been hindered mainly due to the low intrinsic conductivity caused by percolation problems. Here, we have managed to resolve these problems by (1) using large-sized Ti3C2Tx flakes (∼12.2 µm) to reduce interflake resistance and (2) constructing compact microstructures by blade coating. Consequently, excellent optoelectronic properties have been achieved in the blade-coated Ti3C2Tx films, i.e., a DC conductivity of 19 325 S cm-1 at transmittances of 83.4% (≈6.7 nm) was obtained. We also demonstrate the applications of Ti3C2Tx TCEs in transparent Joule heaters and the field of supercapacitors, showing an outstanding Joule heating effect and high rate response, respectively, suggesting enormous potential applications in flexible, transparent electronic devices.

Unraveling Polysulfide's Adsorption and Electrocatalytic Conversion on Metal Oxides for Li-S Batteries.

Lithium sulfur (LiS) batteries possess high theoretical capacity and energy density, holding great promise for next generation electronics and electrical vehicles. However, the LiS batteries development is hindered by the shuttle effect and sluggish conversion kinetics of lithium polysulfides (LiPSs). Designing highly polar materials such as metal oxides (MOs) with moderate adsorption and effective catalytic activity is essential to overcome the above issues. To design efficient MOs catalysts, it is critical and necessary to understand the adsorption mechanism and associated catalytic processes of LiPSs. However, most reviews still lack a comprehensive investigation of the basic mechanism and always ignore their in-depth relationship. In this review, a systematic analysis toward understanding the underlying adsorption and catalytic mechanism in LiS chemistry as well as discussion of the typical works concerning MOs electrocatalysts are provided. Moreover, to improve the sluggish "adsorption-diffusion-conversion" process caused by the low conductive nature of MOs, oxygen vacancies and heterostructure engineering are elucidated as the two most effective strategies. The challenges and prospects of MOs electrocatalysts are also provided in the last section. The authors hope this review will provide instructive guidance to design effective catalyst materials and explore practical possibilities for the commercialization of LiS batteries.

Quasi-Ionic Liquid Enabling Single-Phase Poly(vinylidene fluoride)-Based Polymer Electrolytes for Solid-State LiNi0.6 Co0.2 Mn0.2 O2 ||Li Batteries with Rigid-Flexible Coupling Interphase.

Poly(vinylidene fluoride)-based polymer electrolytes are being intensely investigated for solid-state lithium metal batteries. However, phase separation and porous structures are still pronounced issues in traditional preparing procedure. Herein, a bottom-to-up strategy is employed to design single-phase and densified polymer electrolytes via incorporating quasi-ionic liquid with poly(vinylidene fluoride-co-hexafluoropropylene). Due to strong ion/dipole-dipole interaction, the optimized polymer electrolyte delivers high room-temperature ionic conductivity of 1.55 × 10-3 S cm-1 , superior thermal and oxidation stability of 4.97 V, excellent stretchability of over 1500% and toughness of 43 MJ cm-3 as well as desirable self-extinguishing ability. Furthermore, the superb compatibility toward Li anode enables over 3000 h cycling of Li plating/stripping and ≈98% Coulombic efficiency in Li||Cu test at 0.1 mA cm-2 . In particular, lithium metal battery Li||LiNi0.6 Co0.2 Mn0.2 O2 exhibits a room-temperature discharge retention rate of 96% after 500 cycles under a rate of 0.1 C, which is associated with the rigid-flexible coupling electrodes/electrolytes interphase. This investigation demonstrates the potential application of quasi-ionic liquid/polymer electrolytes in safe lithium metal batteries.

10 µm-Thick High-Strength Solid Polymer Electrolytes with Excellent Interface Compatibility for Flexible All-Solid-State Lithium-Metal Batteries.

An ultrathin solid polymer electrolyte (SPE) consisting of modified polyethylene (PE) as the host and poly(ethylene glycol) methyl ether acrylate and lithium salts as fillers is presented. The porous poly(methyl methacrylate)-polystyrene interface layers closely attached on both sides of the PE effectively improve the interface compatibility among electrolytes and electrodes. The resultant 10 µm-thick SPEs possess an ultrahigh ionic conductance of 34.84 mS at room temperature and excellent mechanical properties of 103.0 MPa with elongation up to 142.3%. The Li//Li symmetric cell employing an optimized solid electrolyte can stably cycle more than 1500 h at 60 °C. Moreover, the LiFePO4 //Li pouch cell can stably cycle over 1000 cycles at 1 C rate and with a capacity retention of 76.4% from 148.9 to 113.7 mAh g-1 at 60 °C. The LiCoO2 //Li pouch cell can stably operate at 0.1 and 0.2 C rate for each 100 cycles. Furthermore, the LiFePO4 //Li pouch cell can work stably after curling and folding, which proves its excellent flexibility and safety simultaneously. This work offers a promising strategy to realize ultrathinness, excellent compatibility, high strength, as well as safe solid electrolytes for all-solid-state lithium-metal batteries.