Customized Heteronuclear Dual Single-Atom and Cluster Assemblies via D-Band Orchestration for Oxygen Reduction Reaction.

Advanced oxygen reduction reaction (ORR) catalysts, integrating with well-dispersed single atom (SA) and atomic cluster (AC) sites, showcase potential in bolstering catalytic activity. However, the precise structural modulation and in-depth investigation of their catalytic mechanisms pose ongoing challenges. Herein, a proactive cluster lockdown strategy is introduced, relying on the confinement of trinuclear clusters with metal atom exchange in the covalent organic polymers, enabling the targeted synthesis of a series of multicomponent ensembles featuring FeCo (Fe or Co) dual-single-atom (DSA) and atomic cluster (AC) configurations (FeCo-DSA/AC) via thermal pyrolysis.

Formulating Self-Repairing Solid Electrolyte Interface via Dynamic Electric Double Layer for Practical Zinc Ion Batteries.

Zinc ion batteries (ZIBs) encounter interface issues stemming from the water-rich electrical double layer (EDL) and unstable solid-electrolyte interphase (SEI). Herein, we propose the dynamic EDL and self-repairing hybrid SEI for practical ZIBs via incorporating the horizontally-oriented dual-site additive. The rearrangement of distribution and molecular configuration of additive constructs the robust dynamic EDL under different interface charges.

In-Situ Solid Electrolyte Interface via Dual Reaction Strategy for Highly Reversible Zinc Anode.

In situ construction of solid electrolyte interfaces (SEI) is an effective strategy to enhance the reversibility of zinc (Zn) anodes. However, in situ SEI to afford high reversibility under high current density conditions (≥20 mA cm) is highly desired yet extremely challenging. Herein, we propose a dual reaction strategy of spontaneous electrostatic reaction and electrochemical decomposition for the in situ construction of SEI, which is composed of organic-rich upper layer and inorganic-rich inner layer.

Single-Anion Conductive Solid-State Electrolytes with Hierarchical Ionic Highways for Flexible Zinc-Air Battery.

Flexible zinc-air batteries are leading power sources for next-generation smart wearable electronics. However, flexible zinc-air batteries suffer from the highly-corrosive safety risk and limited lifespan due to the absence of reliable solid-state electrolytes (SSEs). Herein, a single-anion conductive SSE with high-safety is constructed by incorporating a highly amorphous dual-cation ionomer into a robust hybrid matrix of functional carbon nanotubes and polyacrylamide polymer.

Biomass Solid-State Electrolyte with Abundant Ion and Water Channels for Flexible Zinc-Air Batteries.

Flexible zinc-air batteries are the leading candidates as the next-generation power source for flexible/wearable electronics. However, constructing safe and high-performance solid-state electrolytes (SSEs) with intrinsic hydroxide ion (OH) conduction remains a fundamental challenge. Herein, by adopting the natural and robust cellulose nanofibers (CNFs) as building blocks, the biomass SSEs with penetrating ion and water channels are constructed by knitting the OH-conductive CNFs and water-retentive CNFs together via an energy-efficient tape casting.

Steric-hindrance Effect Tuned Ion Solvation Enabling High Performance Aqueous Zinc Ion Batteries.

Despite many additives have been reported for aqueous zinc ion batteries, steric-hindrance effect of additives and its correlation with Zn solvation structure have been rarely reported. Herein, large-sized sucrose biomolecule is selected as a paradigm additive, and steric-hindrance electrolytes (STEs) are developed to investigate the steric-hindrance effect for solvation structure regulation. Sucrose molecules do not participate in Zn solvation shell, but significantly homogenize the distribution of solvated Zn and enlarge Zn solvation shell with weakened Zn-HO interaction due to the steric-hindrance effect.

Selective and Scalable CO Electrolysis Enabled by Conductive Zinc Ion-Implanted Zeolite-Supported Cadmium Oxide Nanoclusters.

Catalyst supports play an essential role in catalytic reactions, hinting at pronounced metal-support effects. Zeolites are a propitious support in heterogeneous catalysts, while their use in the electrocatalytic CO reduction reaction has been limited as yet because of their electrically insulating nature and serious competing hydrogen evolution reaction (HER). Enlightened by theoretical prediction, herein, we implant zinc ions into the structural skeleton of a zeolite Y to strategically tailor a favorable electrocatalytic platform with remarkably enhanced electronic conduction and strong HER inhibition capability, which incorporates ultrafine cadmium oxide nanoclusters as guest species into the supercages of the tailored 12-ring window framework.

Polysulfide regulation by defect-modulated TaN electrocatalyst toward superior room-temperature sodium-sulfur batteries.

Resolving low sulfur reaction activity and severe polysulfide dissolution remains challenging in metal-sulfur batteries. Motivated by a theoretical prediction, herein, we strategically propose nitrogen-vacancy tantalum nitride (TaN) impregnated inside the interconnected nanopores of nitrogen-decorated carbon matrix as a new electrocatalyst for regulating sulfur redox reactions in room-temperature sodium-sulfur batteries. Through a pore-constriction mechanism, the nitrogen vacancies are controllably constructed during the nucleation of TaN.

Regulation of Outer Solvation Shell Toward Superior Low-Temperature Aqueous Zinc-Ion Batteries.

Aqueous Zn-ion batteries are well regarded among a next-generation energy-storage technology due to their low cost and high safety. However, the unstable stripping/plating process leading to severe dendrite growth under high current density and low temperature impede their practical application. Herein, it is demonstrated that the addition of 2-propanol can regulate the outer solvation shell structure of Zn by replacing water molecules to establish a "eutectic solvation shell", which provides strong affinity with the Zn (101) crystalline plane and fast desolvation kinetics during the plating process, rendering homogeneous Zn deposition without dendrite formation.

Dual-Scale Integration Design of Sn-ZnO Catalyst toward Efficient and Stable CO Electroreduction.

Electrochemical CO reduction to CO is a potential sustainable strategy for alleviating CO emission and producing valuable fuels. In the quest to resolve its current problems of low-energy efficiency and insufficient durability, a dual-scale design strategy is proposed by implanting a non-noble active Sn-ZnO heterointerface inside the nanopores of high-surface-area carbon nanospheres (Sn-ZnO@HC). The metal d-bandwidth tuning of Sn and ZnO alters the extent of substrate-molecule orbital mixing, facilitating the breaking of the *COOH intermediate and the yield of CO.

"Tree-Trunk" Design for Flexible Quasi-Solid-State Electrolytes with Hierarchical Ion-Channels Enabling Ultralong-Life Lithium-Metal Batteries.

The construction of robust (quasi)-solid-state electrolyte (SSE) for flexible lithium-metal batteries is desirable but extremely challenging. Herein, a novel, flexible, and robust quasi-solid-state electrolyte (QSSE) with a "tree-trunk" design is reported for ultralong-life lithium-metal batteries (LMBs). An in-situ-grown metal-organic framework (MOF) layer covers the cellulose-based framework to form hierarchical ion-channels, enabling rapid ionic transfer kinetics and excellent durability.

Bioinspired Tough Solid-State Electrolyte for Flexible Ultralong-Life Zinc-Air Battery.

Manufacturing advanced solid-state electrolytes (SSEs) for flexible rechargeable batteries becomes increasingly important but remains grand challenge. The sophisticated structure of robust animal dermis and good water-retention of plant cell in nature grant germane inspirations for designing high-performance SSEs. Herein, tough bioinspired SSEs with intrinsic hydroxide ion (OH ) conduction are constructed by in situ formation of OH conductive ionomer network within a hollow-polymeric-microcapsule-decorated hydrogel polymer network.

Emerging Trends in Sustainable CO -Management Materials.

With the rising level of atmospheric CO worsening climate change, a promising global movement toward carbon neutrality is forming. Sustainable CO management based on carbon capture and utilization (CCU) has garnered considerable interest due to its critical role in resolving emission-control and energy-supply challenges. Here, a comprehensive review is presented that summarizes the state-of-the-art progress in developing promising materials for sustainable CO management in terms of not only capture, catalytic conversion (thermochemistry, electrochemistry, photochemistry, and possible combinations), and direct utilization, but also emerging integrated capture and in situ conversion as well as artificial-intelligence-driven smart material study.

Porous organic polymers for Li-chemistry-based batteries: functionalities and characterization studies.

Porous organic polymers (POPs), a versatile class of materials that possess many tunable properties such as high chemical absorptivity and ionic conductivity, are emerging candidate electrode materials, permselective membranes, ionic conductors, interfacial stabilizers and functional precursors to synthesize advanced porous carbon. Based on their crystal structure features, the emerging POPs can be classified into two subclasses: amorphous POPs (hyper cross-linked polymers, polymers with intrinsic microporosity, conjugated microporous polymers, porous aromatic frameworks, ) and crystalline POPs (covalent organic frameworks, ). This tutorial review provides a brief introduction of different types of POPs in terms of their classification and functions for tackling the remaining challenges in various types of Li-chemistry-based batteries.

Hierarchically Nanostructured Solid-State Electrolyte for Flexible Rechargeable Zinc-Air Batteries.

The construction of safe and environmentally-benign solid-state electrolytes (SSEs) with intrinsic hydroxide ion-conduction for flexible zinc-air batteries is highly desirable yet extremely challenging. Herein, hierarchically nanostructured CCNF-PDIL SSEs with reinforced concrete architecture are constructed by nanoconfined polymerization of dual-cation ionic liquid (PDIL, concrete) within a robust three-dimensional porous cationic cellulose nanofiber matrix (CCNF, reinforcing steel), where plenty of penetrating ion-conductive channels are formed and undergo dynamic self-rearrangement under different hydrated levels. The CCNF-PDIL SSEs synchronously exhibit good flexibility, mechanical robustness, superhigh ion conductivity of 286.

2D Materials for All-Solid-State Lithium Batteries.

Although one of the most mature battery technologies, lithium-ion batteries still have many aspects that have not reached the desired requirements, such as energy density, current density, safety, environmental compatibility, and price. To solve these problems, all-solid-state lithium batteries (ASSLB) based on lithium metal anodes with high energy density and safety have been proposed and become a research hotpot in recent years. Due to the advanced electrochemical properties of 2D materials (2DM), they have been applied to mitigate some of the current problems of ASSLBs, such as high interface impedance and low electrolyte ionic conductivity.

Thin Film Polyamide Nanocomposite Membrane Decorated by Polyphenol-Assisted TiCT MXene Nanosheets for Reverse Osmosis.

Transition-metal carbides (MXenes), multifunctional 2D materials, have caught the interest of researchers in the fabrication of high-performance nanocomposite membranes. However, several issues regarding MXenes still remain unresolved, including low ambient stability; facile restacking and agglomeration; and poor compatibility and processability. To address the aforementioned challenges, we proposed a facile, green, and cost-efficient approach for coating a stable layer of plant-derived polyphenol tannic acid (TA) on the surface of MXene (TiCT) nanosheets.

A Gas-Phase Migration Strategy to Synthesize Atomically Dispersed Mn-N-C Catalysts for Zn-Air Batteries.

Mn and N codoped carbon materials are proposed as one of the most promising catalysts for the oxygen reduction reaction (ORR) but still confront a lot of challenges to replace Pt. Herein, a novel gas-phase migration strategy is developed for the scale synthesis of atomically dispersed Mn and N codoped carbon materials (g-SA-Mn) as highly effective ORR catalysts. Porous zeolitic imidazolate frameworks serve as the appropriate support for the trapping and anchoring of Mn-containing gaseous species and the synchronous high-temperature pyrolysis process results in the generation of atomically dispersed Mn-N active sites.

Electrolyte Design for Lithium Metal Anode-Based Batteries Toward Extreme Temperature Application.

Lithium anode-based batteries (LBs) are highly demanded in society owing to the high theoretical capacity and low reduction potential of metallic lithium. They are expected to see increasing deployment in performance critical areas including electric vehicles, grid storage, space, and sea vehicle operations. Unfortunately, competitive performance cannot be achieved when LBs operating under extreme temperature conditions where the lithium-ion chemistry fail to perform optimally.

"Two Ships in a Bottle" Design for Zn-Ag-O Catalyst Enabling Selective and Long-Lasting CO Electroreduction.

Electrochemical CO reduction (CORR) using renewable energy sources represents a sustainable means of producing carbon-neutral fuels. Unfortunately, low energy efficiency, poor product selectivity, and rapid deactivation are among the most intractable challenges of CORR electrocatalysts. Here, we strategically propose a "two ships in a bottle" design for ternary Zn-Ag-O catalysts, where ZnO and Ag phases are twinned to constitute an individual ultrafine nanoparticle impregnated inside nanopores of an ultrahigh-surface-area carbon matrix.

Microporous framework membranes for precise molecule/ion separations.

Microporous framework membranes such as metal-organic framework (MOF) membranes and covalent organic framework (COF) membranes are constructed by the controlled growth of small building blocks with large porosity and permanent well-defined micropore structures, which can overcome the ubiquitous tradeoff between membrane permeability and selectivity; they hold great promise for the enormous challenging separations in energy and environment fields. Therefore, microporous framework membranes are endowed with great expectations as next-generation membranes, and have evolved into a booming research field. Numerous novel membrane materials, versatile manipulation strategies of membrane structures, and fascinating applications have erupted in the last five years.

Analogous Mixed Matrix Membranes with Self-Assembled Interface Pathways.

The implementation of mixed matrix membranes (MMMs) for sub-angstrom scale gas separations remains a grand challenge. Herein, a series of analogous mixed matrix membrane (AMMMs) were constructed via molecular-level hybridization by utilizing a reactive ionic liquid (RIL) as the continuous phase and graphene quantum dots (GQD) as nanofiller for sub-angstrom scale ethylene/ethane (0.416 nm/0.

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

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.

Membrane-Based Olefin/Paraffin Separations.

Efficient olefin/paraffin separation is a grand challenge because of their similar molecular sizes and physical properties, and is also a priority in the modern chemical industry. Membrane separation technology has been demonstrated as a promising technology owing to its low energy consumption, mild operation conditions, tunability of membrane materials, as well as the integration of physical and chemical mechanisms. In this work, inspired by the physical mechanism of mass transport in channel proteins and the chemical mechanism of mass transport in carrier proteins, recent progress in channel-based and carrier-based membranes toward olefin/paraffin separations is summarized.

Ternary Sn-Ti-O Electrocatalyst Boosts the Stability and Energy Efficiency of CO Reduction.

Simultaneously improving energy efficiency (EE) and material stability in electrochemical CO conversion remains an unsolved challenge. Among a series of ternary Sn-Ti-O electrocatalysts, 3D ordered mesoporous (3DOM) Sn Ti O achieves a trade-off between active-site exposure and structural stability, demonstrating up to 71.5 % half-cell EE over 200 hours, and a 94.