Implanting Colloidal Nanoparticles into Single-Crystalline Zeolites for Catalytic Dehydration.

The encapsulation of functional colloidal nanoparticles (100 nm) into single-crystalline ZSM-5 zeolites, aiming to create uniform core-shell structures, is a highly sought-after yet formidable objective due to significant lattice mismatch and distinct crystallization properties. In this study, we demonstrate the fabrication of a core-shell structured single-crystal zeolite encompassing an FeO colloidal core via a novel confinement stepwise crystallization methodology. By engineering a confined nanocavity, anchoring nucleation sites, and executing stepwise crystallization, we have successfully encapsulated colloidal nanoparticles (CN) within single-crystal zeolites.

Boosted Oxygen Kinetics of Hierarchically Mesoporous MoC/C for High-current-density Zn-air Battery.

The high-current-density Zn-air battery shows big prospects in next-generation energy technologies, while sluggish O reaction and diffusion kinetics barricade the applications. Herein, the sequential assembly is innovatively demonstrated for hierarchically mesoporous molybdenum carbides/carbon microspheres with a tunable thickness of mesoporous carbon layers (Meso-MoC/C-x, where x represents the thickness). The optimum Meso-MoC/C-14 composites (≈2 µm in diameter) are composed of mesoporous nanosheets (≈38 nm in thickness), which possess bilateral mesoporous carbon layers (≈14 nm in thickness), inner MoC/C layers (≈8 nm in thickness) with orthorhombic MoC nanoparticles (≈2 nm in diameter), a high surface area of ≈426 m g, and open mesopores (≈6.

Solvent Effect on the Nanotextural Formation of Reduced Graphene Oxide Membranes.

Solvent is involved in many wet-chemical synthesis and bottom-up assembly processes. Understanding its influence on the nanotextural formation of the resultant assemblies is essential for the design and control of the properties for targeted applications. With wet chemically reduced graphene oxide (rGO) membranes as a materials platform, this study investigates the solvent effect on nanotexture formation in 2D nanomaterial-based membranes through light scattering and electrochemical characterization.

Subnanometric Stacking of Two-Dimensional Nanomaterials: Insights from the Nanotexture Evolution of Dense Reduced Graphene Oxide Membranes.

Assembling two-dimensional (2D) nanomaterials into laminar membranes with a subnanometer (subnm) interlayer spacing provides a material platform for studying a range of nanoconfinement effects and exploring the technological applications related to the transport of electrons, ions and molecules. However, the strong tendency for 2D nanomaterials to restack to their bulk crystalline-like structure makes it challenging to control their spacing at the subnm scale. It is thus necessary to understand what nanotextures can be formed at the subnm scale and how they can be engineered experimentally.

Mechanistic Principles for Engineering Hierarchical Porous Metal-Organic Frameworks.

Metal-organic frameworks (MOFs) have generated tremendous research interest in the past two decades, due to their high surface areas, tailorable active sites, and tunable structures. Hierarchical porous MOFs (HP-MOFs) with two or more pore systems are particularly attractive, benefiting from improved active site accessibility and enhanced mass diffusivity in applications involving bulk molecules. This review outlines the mechanistic principles used for the rational design of HP-MOFs, current techniques used to measure their hierarchical porosities, as well as their emerging applications.

Constructing Unique Mesoporous Carbon Superstructures via Monomicelle Interface Confined Assembly.

Constructing hierarchical three-dimensional (3D) mesostructures with unique pore structure, controllable morphology, highly accessible surface area, and appealing functionality remains a great challenge in materials science. Here, we report a monomicelle interface confined assembly approach to fabricate an unprecedented type of 3D mesoporous N-doped carbon superstructure for the first time. In this hierarchical structure, a large hollow locates in the center (∼300 nm in diameter), and an ultrathin monolayer of spherical mesopores (∼22 nm) uniformly distributes on the hollow shells.

Zero-Strain High-Capacity Silicon/Carbon Anode Enabled by a MOF-Derived Space-Confined Single-Atom Catalytic Strategy for Lithium-Ion Batteries.

Developing zero-strain electrode materials with high capacity is crucial for lithium-ion batteries (LIBs). Here, a new zero-strain composite material made of ultrasmall Si nanodots (NDs) within metal organic framework-derived nanoreactors (Si NDs⊂MDN) through a novel space-confined catalytic strategy is reported. The unique Si NDs⊂MDN anode features a low strain (<3%) and a high theoretical lithium storage capacity (1524 mAh g ) which far surpasses the traditional single-crystal counterparts that suffer from a low capacity delivery.

Self-Assembly of Ir-Based Nanosheets with Ordered Interlayer Space for Enhanced Electrocatalytic Water Oxidation.

Iridium (Ir)-based electrocatalysts are widely explored as benchmarks for acidic oxygen evolution reactions (OERs). However, further enhancing their catalytic activity remains challenging due to the difficulty in identifying active species and unfavorable architectures. In this work, we synthesized ultrathin Ir-IrO/C nanosheets with ordered interlayer space for enhanced OER by a nanoconfined self-assembly strategy, employing block copolymer formed stable end-merged lamellar micelles.

Precisely Designed Mesoscopic Titania for High-Volumetric-Density Pseudocapacitance.

Surface redox pseudocapacitance, which enables short charging times and high power delivery, is very attractive in a wide range of sites. To achieve maximized specific capacity, nanostructuring of active materials with high surface area is indispensable. However, one key limitation for capacitive materials is their low volumetric capacity due to the low tap density of nanomaterials.

Ultrapermeable Composite Membranes Enhanced Via Doping with Amorphous MOF Nanosheets.

Thin-film composite (TFC) polymeric membranes have attracted increasing interest to meet the demands of industrial gas separation. However, the development of high-performance TFC membranes within their current configuration faces two key challenges: (i) the thickness-dependent gas permeability of polymeric materials (mainly poly(dimethylsiloxane) (PDMS)) and (ii) the geometric restriction effect due to the limited pore accessibility of the underlying porous substrate. Here we demonstrate that the incorporation of trace amounts (∼1.

CoPSe: A New Ternary Anode Material for Stable and High-Rate Sodium/Potassium-Ion Batteries.

The exploration of ideal electrode materials overcoming the critical problems of large electrode volume changes and sluggish redox kinetics induced by large ionic radius of Na /K ions is highly desirable for sodium/potassium-ion batteries (SIBs/PIBs) toward large-scale applications. The present work demonstrates that single-phase ternary cobalt phosphoselenide (CoPSe) in the form of nanoparticles embedded in a layered metal-organic framework (MOF)-derived N-doped carbon matrix (CoPSe/NC) represents an ultrastable and high-rate anode material for SIBs/PIBs. The CoPSe/NC is fabricated by using the MOF as both a template and precursor, coupled with in situ synchronous phosphorization/selenization reactions.

Covalent Assembly of MoS Nanosheets with SnS Nanodots as Linkages for Lithium/Sodium-Ion Batteries.

Weak van der Waals interactions between interlayers of two-dimensional layered materials result in disabled across-interlayer electron transfer and poor layered structural stability, seriously deteriorating their performance in energy applications. Herein, we propose a novel covalent assembly strategy for MoS nanosheets to realize unique MoS /SnS hollow superassemblies (HSs) by using SnS nanodots as covalent linkages. The covalent assembly based on all-inorganic and carbon-free concept enables effective across-interlayer electron transfer, facilitated ion diffusion kinetics, and outstanding mechanical stability, which are evidenced by experimental characterization, DFT calculations, and mechanical simulations.

TiCT MXene Nanosheets as a Robust and Conductive Tight on Si Anodes Significantly Enhance Electrochemical Lithium Storage Performance.

Exploring Si-based anode materials with high electrical conductivity and electrode stability is crucial for high-performance lithium-ion batteries (LIBs). Herein, we propose the fabrication of a Si-based composite where Si porous nanospheres (Si p-NSs) are tightly wrapped by TiCT (T stands for the surface groups such as -OH, -F) MXene nanosheets (TNSs) through an interfacial assembly strategy. The TNSs as a conductive and robust tight of the Si p-NSs can effectively improve electron transport and electrode stability, as revealed by substantial characterizations and mechanical simulations.

Three-Dimensional Hierarchical Porous Nanotubes Derived from Metal-Organic Frameworks for Highly Efficient Overall Water Splitting.

Effective design of bifunctional catalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is important but remains challenging. Herein, we report a three-dimensional (3D) hierarchical structure composed of homogeneously distributed Ni-Fe-P nanoparticles embedded in N-doped carbons on nickel foams (denoted as Ni-Fe-P@NC/NF) as an excellent bifunctional catalyst. This catalyst was fabricated by an anion exchange method and a low-temperature phosphidation of nanotubular Prussian blue analogue (PBA).

Space-Confined Atomic Clusters Catalyze Superassembly of Silicon Nanodots within Carbon Frameworks for Use in Lithium-Ion Batteries.

Incorporating nanoscale Si into a carbon matrix with high dispersity is desirable for the preparation of lithium-ion batteries (LIBs) but remains challenging. A space-confined catalytic strategy is proposed for direct superassembly of Si nanodots within a carbon (Si NDs⊂C) framework by copyrolysis of triphenyltin hydride (TPT) and diphenylsilane (DPS), where Sn atomic clusters created from TPT pyrolysis serve as the catalyst for DPS pyrolysis and Si catalytic growth. The use of Sn atomic cluster catalysts alters the reaction pathway to avoid SiC generation and enable formation of Si NDs with reduced dimensions.

Hybrid Anatase/Rutile Nanodots-Embedded Covalent Organic Frameworks with Complementary Polysulfide Adsorption for High-Performance Lithium-Sulfur Batteries.

The shuttling effect of polysulfides species seriously deteriorates the performance of Li-S batteries, representing the major obstacle for their practical use. However, the exploration of ideal cathodes that can suppress the shuttling of all polysulfides species is challenging. Herein, we propose an ingenious and effective strategy for constructing hybrid-crystal-phase TiO/covalent organic framework (HCPT@COF) composites where hybrid anatase/rutile TiO nanodots (10 nm) are uniformly embedded in the interlayers of porous COFs.

A polymer-direct-intercalation strategy for MoS/carbon-derived heteroaerogels with ultrahigh pseudocapacitance.

The intercalation strategy has become crucial for 2D layered materials to achieve desirable properties, however, the intercalated guests are often limited to metal ions or small molecules. Here, we develop a simple, mild and efficient polymer-direct-intercalation strategy that different polymers (polyethyleneimine and polyethylene glycol) can directly intercalate into the MoS interlayers, forming MoS-polymer composites and interlayer-expanded MoS/carbon heteroaerogels after carbonization. The polymer-direct-intercalation behavior has been investigated by substantial characterizations and molecular dynamic calculations.

Mesoporous TiO/TiC@C Composite Membranes with Stable TiO-C Interface for Robust Lithium Storage.

Transition metal oxides/carbon (TMOs/C) composites are important for high-performance lithium-ion batteries (LIBs), but the development of interface-stable TMOs/C composite anodes for robust lithium storage is still a challenge. Herein, mesoporous TiO/TiC@C composite membranes were synthesized by an in situ carbothermic reduction method. TiC nanodots with high conductivity and electrochemical inactivity at the TiO-C interface can significantly enhance the electrical conductivity and structural stability of the membranes.

A titanium-based photo-Fenton bifunctional catalyst of mp-MXene/TiO nanodots for dramatic enhancement of catalytic efficiency in advanced oxidation processes.

mp-MXene/TiO2-x nanodots (NDs) structurally composed of microporous MXene monolayers embedded with Ti3+-doped TiO2 nanodots were developed for the first time. The drastically enhanced catalytic efficiency (as much as 13 times higher than that of P25) in degrading dye molecules over mp-MXene/TiO2-x NDs is due to a synergistic effect of the pseudo-Fenton reaction and photocatalysis.

Hydrogen evolution reactions boosted by bridge bonds between electrocatalysts and electrodes.

The interfacial interactions between nanostructured electrode materials and electrodes play an important part in the performance enhancement of electrochemical energy devices. However, the mechanism of interfacial interactions, as well as its influence on device performance, still remains unclear and is rarely studied. In this work, a CoS nanobelt catalyst assembled on Ti foil (CoS nanobelts/Ti) is prepared through in situ chemical conversions and chosen as an example to probe the interfacial interactions between the CoS catalyst and the Ti electrode, and the correlation between the interfacial interaction and the hydrogen evolution reaction (HER) performance.

One-pot mass preparation of MoS/C aerogels for high-performance supercapacitors and lithium-ion batteries.

In this paper, we report the successful design and synthesis of a hierarchically porous MoS/C composite aerogel by simple one-pot mass preparation. The synthesis involves the in situ formation of MoS nanosheets on agarose molecular chains, the gelation of MoS-deposited agarose monomers to generate a composite hydrogel, and in situ transformation of the composite hydrogel into a MoS/C composite aerogel through carbonization. This composite aerogel can be used as a high-performance electrode material for supercapacitors and lithium-ion batteries.

Antipulverization Electrode Based on Low-Carbon Triple-Shelled Superstructures for Lithium-Ion Batteries.

The realization of antipulverization electrode structures, especially using low-carbon-content anode materials, is crucial for developing high-energy and long-life lithium-ion batteries (LIBs); however, this technology remains challenging. This study shows that SnO triple-shelled hollow superstructures (TSHSs) with a low carbon content (4.83%) constructed by layer-by-layer assembly of various nanostructure units can withstand a huge volume expansion of ≈231.

Direct Superassemblies of Freestanding Metal-Carbon Frameworks Featuring Reversible Crystalline-Phase Transformation for Electrochemical Sodium Storage.

High-power sodium-ion batteries (SIBs) with long-term cycling attract increasing attention for large-scale energy storage. However, traditional SIBs toward practical applications still suffer from low rate capability and poor cycle induced by pulverization and amorphorization of anodes at high rate (over 5 C) during the fast ion insertion/extraction process. The present work demonstrates a robust strategy for a variety of (Sb-C, Bi-C, Sn-C, Ge-C, Sb-Bi-C) freestanding metal-carbon framework thin films via a space-confined superassembly (SCSA) strategy.

Amorphous Semiconductor Nanowires Created by Site-Specific Heteroatom Substitution with Significantly Enhanced Photoelectrochemical Performance.

Semiconductor nanowires that have been extensively studied are typically in a crystalline phase. Much less studied are amorphous semiconductor nanowires due to the difficulty for their synthesis, despite a set of characteristics desirable for photoelectric devices, such as higher surface area, higher surface activity, and higher light harvesting. In this work of combined experiment and computation, taking Zn2GeO4 (ZGO) as an example, we propose a site-specific heteroatom substitution strategy through a solution-phase ions-alternative-deposition route to prepare amorphous/crystalline Si-incorporated ZGO nanowires with tunable band structures.

Preparation of Ag@Ag₃PO₄@ZnO ternary heterostructures for photocatalytic studies.

In this article, we report a novel Ag@Ag3PO4@ZnO ternary heterostructures synthesized through a three-step approach. Firstly, single-crystalline Ag nanorods are fabricated and served as the templates for subsequent Ag3PO4 deposition. Secondly, Ag3PO4 crystals are grown around Ag core nanorods through a solution co-precipitation process, leading to the Ag@Ag3PO4 binary heterostructures.