All-solid-state lithium ion batteries (ASSLBs) are considered next-generation devices for energy storage due to their advantages in safety and potentially high energy density. As the key component in ASSLBs, solid-state electrolytes (SSEs) with non-flammability and good adaptability to lithium metal anodes have attracted extensive attention in recent years. Among the current SSEs, composite solid-state electrolytes (CSSEs) with multiple phases have greater flexibility to customize and combine the advantages of single-phase electrolytes, which have been widely investigated recently and regarded as promising candidates for commercial ASSLBs. Based on existing investigations, herein, we present a comprehensive overview of the recent developments in CSSEs. Initially, we introduce the historical development from solid-state ionic conductors to CSSEs, and then summarize the fundamentals including mechanisms of lithium ion transport, key evaluation parameters, design principles, and key materials. Four main types of advanced structures for CSSEs are classified and highlighted according to the recent progress. Moreover, advanced characterization and computational simulation techniques including machine learning are reviewed for the first time, and the main challenges and perspectives of CSSEs are also provided for their future development.

A review of composite solid-state electrolytes for lithium batteries: fundamentals, key materials and advanced structures.

The design and development of crystalline porous materials (CPMs), including metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs), have been subjects of extensive study due to their regular crystalline lattices and well-defined pore structures. In recent times, an enormous amount of research effort has gone into using CPMs as sacrificial templates to fabricate electrochemically functional materials. The inherently electrochemically active sites inside CPMs are notably abundant and being explored with respect to electrochemical reactions. In this review, electrochemically active sites and the space around them (metal ions, ligands, crystal structures, pores, and morphologies) inside CPMs are the focus and recent progress in the fields of metal-ion batteries, metal-air batteries, water splitting, and other related electrochemical devices has been summarized. Overall, this review provides guidance on the preparation of electroactive CPMs via rational design and modulation of active sites such as redox-active metal clusters and organic ligands, and the space around the electrochemically active sites, and their applications in electrochemical energy storage and conversion systems.

Electrochemically active sites inside crystalline porous materials for energy storage and conversion.

Polymer electrolytes (PEs), a type of solid-state electrolytes (SSEs), have been in contention for nearly half a century to replace organic liquid electrolytes (LEs) that are used in state-of-the-art lithium-ion batteries (LIBs). They are envisaged to accelerate the industrial-scale production of safe, energy-dense, flexible, and thin lithium polymer batteries (LPBs). LPBs are expected to be widely employed for electric propulsion and other futuristic applications, such as flexible electronics and the Internet of Things (IoT). Even though several polymer architectures and chemistries have been attempted so far, PEs that can outperform LEs remain a real challenge. Apart from inadequate Li+-ion transport properties, challenges concerning the integration of PEs and the engineering of compatible, robust, and durable interfaces and interphases at both the electrodes of LPBs must be appropriately addressed. Recently, the in situ polymerization process has been widely employed as a robust fabrication tool for surpassing the intricacies related to the integration of PEs in LPBs. Hence, in this review, we focus on the in situ polymerization processes that employ various polymerization methods (e.g., free-radical polymerization, ionic polymerization, electropolymerization, condensation polymerization, etc.), functional monomers and oligomers (e.g., acrylate, methacrylate, allyl and vinyl ethers, epoxides, etc.), and PE integration strategies for the fabrication of lithium (ion and metal) polymer batteries (LIPBs and LMPBs). Additionally, this review also evaluates the approaches that have been developed until now to implement the in situ processing of LPBs from large-sized pouch cells to flexible-/printable-batteries and even microbatteries.

/pdf/in-situ-polymerization-process-an-essential-design-tool-for-2797gs7ozq.pdf

In situ polymerization process: an essential design tool for lithium polymer batteries

Emerging Functional Porous Polymeric and Carbonaceous Materials for Environmental Treatment and Energy Storage

Covalent Organic Frameworks for Batteries

Porous covalent organic frameworks for high transference number polymer-based electrolytes.

Dry reforming of methane (DRM) on Ni-based catalysts provides an economically and environmentally pivotal route to generate synthesis gas. However, coke formation on Ni surface by the growth of carbon atoms is the main reason for catalyst deactivation and reactor blockage. Here, we propose a reaction-induced method to incorporate and store active carbon atoms into nickel octahedral sites in core-shell Ni 3 ZnC 0.7 /Al 2 O 3 . This strategy can fundamentally avoid C−C bond formation and feasible oxidation of Ni 3 ZnC 0.7 in low-temperature DRM under CO 2 -rich condition. About 2 nm of thin-layer Al 2 O 3 encapsulated Ni 3 ZnC 0.7 is explored as the carbon reservoir to accommodate sufficient interstitial carbon atoms, and less than 5% Ni 3 Zn was observed under CH 4 /CO 2 < 1/1 for 100 h. The dynamic balance of carbon atom storage and conversion in robust Ni 3 ZnC 0.7 contributes to the enhanced activity, stability, coke and oxidation resistance, and distinct reaction pathway in low-temperature DRM. About 2 nm of thin-layer Al 2 O 3 encapsulated Ni 3 ZnC 0.7 with 54.4 wt% of Ni content is explored as carbon reservoir to accommodate sufficient carbon atoms in the interstitial sites, and effectively avoid the C−C bond formation and the catalyst oxidation during LT-DRM under a CO 2 -rich feed. • Core-shell Ni 3 ZnC 0.7 /Al 2 O 3 catalyst was designed for DRM. • Ni 3 ZnC 0.7 is explored as carbon reservoir for sufficient carbon atoms. • Ni 3 ZnC 0.7 /Al 2 O 3 exhibited superior activity and stability in CO 2 -rich conditions. • Ni 3 ZnC 0.7 /Al 2 O 3 tailored the evolution of carbon atoms under CH 4 /CO 2 < 1/1. • Carbon atom were stored and converted in interstitial sites in robust Ni 3 ZnC 0.7 /Al 2 O 3 . 

Effect of Interstitial Carbon Atoms in Core-shell Ni3ZnC0.7/Al2O3 Catalyst for High-performance Dry Reforming of Methane

Structural evolution of robust Ni3Fe1 alloy on Al2O3 in dry reforming of methane: Effect of iron-surplus strategy from Ni1Fe1 to Ni3Fe1

The typical polymer electrolyte matrix has been limited to the chains consisting of -C-C- or -C-O-C- or -Si-O- backbone with different solvating groups for decades. In this work, the polymeric sulfur consisting of -(S-S)n- backbone with a high sulfur content (up to 90 wt % S) was reported for the first time. The flexible -(S-S)n- chains with high S atom density create an intense "solvating" environment for Li+ conduction, achieving an excellent Li+ conductivity of 1.69 × 10-3 S cm-1 at 80 °C. Benefiting from its unique thermoplasticity, a hot-rolling process was also developed for fabricating the poly-S membrane. The symmetric solid-state Li cell using the membrane showed a high cycling stability over 300 h. The work offers a novel platform for chemists to design new polymer electrolytes that are quite different with conventional carbon-based polymer electrolytes.

Polymeric Sulfur as a Li Ion Conductor

Well-defined bimetallic heterogeneous catalysts are not only difficult to synthesize in a controlled manner, but their elemental distributions are also notoriously challenging to define. Knowledge of these distributions is required for both the as-synthesized catalyst and its activated form under reaction conditions, where various types of reconstruction can occur. Success in this endeavor requires observation of the active catalyst via in situ analytical methods. As a step toward this goal, we present a composite material composed of bimetallic nickel-ruthenium nanoparticles supported on a protonated zeolite (Ni-Ru/HZSM-5) and probe its evolution and function as a photoactive carbon dioxide methanation catalyst using in situ X-ray absorption spectroscopy (XAS). The working Ni-Ru/HZSM-5, as a selective and durable photothermal CO2 methanation catalyst, comprises a corona of Ru nanoparticles decorating a Ni nanoparticle core. The specific Ni-Ru interactions in the bimetallic particles were confirmed by in situ XAS, which reveals significant electron transfer from Ni to Ru. The light-harvesting Ni nanoparticle core and electron-accepting Ru nanoparticle corona serve as the CO2 and H2 dissociation centers, respectively. These Ni and Ru nanoparticles also promote synergistic photothermal and hydrogen atom transfer effects. Collectively, these effects enable an associative CO2 methanation reaction pathway while hindering coking and fostering high selectivity toward methane.

Visualizing the Birth and Monitoring the Life of a Bimetallic Methanation Catalyst.

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