End-to-End Pierced Carbon Nanosheets with Meso-Holes.

The remarkable properties of 2D nanomaterials are well known. However, their high interfacial adhesion energy often leads to restacking issues, limiting their potential in various applications. A strategic synthetic approach is presented to overcome this challenge.

Simultaneous generation of residue-free reactive oxygen species and bacteria capture for efficient electrochemical water disinfection.

Residue-free and highly efficient techniques for drinking water disinfection are urgently needed. Herein, we report an electrochemical water disinfection system equipped with atomically precise Ag nanoclusters (NCs) as electrode materials. The deployment of these Ag NCs not only provides sufficient electrosorption sites for intelligent microbe enrichment but also ensures high-efficiency dual-mode microbial killing through the in situ electrocatalytic production of residue-free reactive oxygen species (ROS) and the inherent antimicrobial activity of Ag NCs.

Mesoporous High-Entropy Alloy Films.

High-entropy alloys (HEAs) are promising materials for electrochemical energy applications due to their excellent catalytic performance and durability. However, the controlled synthesis of HEAs with a well-defined structure and a uniform composition distribution remains a challenge. Herein, a soft template-assisted electrodeposition technique is used to fabricate a mesoporous HEA (m-HEA) film with a uniform composition distribution of Pt, Pd, Rh, Ru, and Cu, providing a suitable platform for investigating structure-performance relationships.

Nanoarchitectonics of ultrafine molybdenum carbide nanocrystals into three-dimensional nitrogen-doped carbon framework for capacitive deionization.

Molybdenum carbide (MoC) has emerged as a promising material for capacitive deionization (CDI), but the poor electrochemical kinetics in conventional MoC owing to the bulk structure and low electric conductivity limit its CDI performance. To address this challenge, herein, we develop a novel strategy to synthesize ultrafine MoC nanocrystals that are embedded within a three-dimensional nitrogen-doped carbon framework (NC/MoC). This synthesis method involves the space-confined pyrolysis of molybdate precursors within metal-organic frameworks (MOFs).

Bridged Pt-OH-Mn Mediator in N-coordinated Mn Single Atoms and Pt Nanoparticles for Electrochemical Biomolecule Oxidation and Discrimination.

The rational design of efficient catalysts for uric acid (UA) electrooxidation, as well as the establishment of structure-activity relationships, remains a critical bottleneck in the field of electrochemical sensing. To address these challenges, herein, a hybrid catalyst that integrates carbon-supported Pt nanoparticles and nitrogen-coordinated Mn single atoms (Pt/MnNC) is developed. The metal-metal interaction during annealing affords the construction of metallic-bonded Pt-Mn pairs between Pt and Mn single atoms, facilitating the electron transfer from Pt to the support and thereby optimizing the electronic structure of catalysts.

Silica Confinement for Stable and Magnetic Co-Cu Alloy Nanoparticles in Nitrogen-Doped Carbon for Enhanced Hydrogen Evolution.

Ammonia borane (AB) with 19.6 wt % H content is widely considered a safe and efficient medium for H storage and release. Co-based nanocatalysts present strong contenders for replacing precious metal-based catalysts in AB hydrolysis due to their high activity and cost-effectiveness.

Synthesis of millimeter-scale ZIF-8 single crystals and their reversible crystal structure changes.

Among various metal-organic frameworks (MOFs), the zeolitic imidazole framework (ZIF), constructed by the regular arrangement of 2-methylimidazole and metal ions, has garnered significant attention due to its distinctive crystals and pore structures. Variations in the sizes and shapes of ZIF crystals have been reported by changing the synthesis parameters, such as the molar ratios of organic ligands to metal ions, choice of solvents, and temperatures. Nonetheless, the giant ZIF-8 single crystals beyond the typical range have rarely been reported.

Mesoporous Metastable CuTe Semiconductor.

Binary metastable semiconductor materials offer exciting possibilities in the field of optoelectronics, such as photovoltaics, tunable photosensors, and detectors. However, understanding their properties and translating them into practical applications can sometimes be challenging, owing to their thermodynamic instability. Herein, we report a temperature-controlled crystallization technique involving electrochemical deposition to produce metastable CuTe thin films that can reliably function under ambient conditions.

Composite polymer electrolytes with ionic liquid grafted-Laponite for dendrite-free all-solid-state lithium metal batteries.

Composite polymer electrolytes (CPEs) with high ionic conductivity and favorable electrolyte/electrode interfacial compatibility are promising alternatives to liquid electrolytes. However, severe parasitic reactions in the Li/electrolyte interface and the air-unstable inorganic fillers have hindered their industrial applications. Herein, surface-edge opposite charged Laponite (LAP) multilayer particles with high air stability were grafted with imidazole ionic liquid (IL-TFSI) to enhance the thermal, mechanical, and electrochemical performances of polyethylene oxide (PEO)-based CPEs.

Materials Space-Tectonics: Atomic-level Compositional and Spatial Control Methodologies for Synthesis of Future Materials.

Reactions occurring at surfaces and interfaces necessitate the creation of well-designed surface and interfacial structures. To achieve a combination of bulk material (i.e.

Mesoporous multimetallic nanospheres with exposed highly entropic alloy sites.

Multimetallic alloys (MMAs) with various compositions enrich the materials library with increasing diversity and have received much attention in catalysis applications. However, precisely shaping MMAs in mesoporous nanostructures and mapping the distributions of multiple elements remain big challenge due to the different reduction kinetics of various metal precursors and the complexity of crystal growth. Here we design a one-pot wet-chemical reduction approach to synthesize core-shell motif PtPdRhRuCu mesoporous nanospheres (PtPdRhRuCu MMNs) using a diblock copolymer as the soft template.

Water Activation in Solar-Powered Vapor Generation.

Solar-powered vapor evaporation (SVG), based on the liquid-gas phase conversion concept using solar energy, has been given close attention as a promising technology to address the global water shortage. At molecular level, water molecules escaping from liquid water should overcome the attraction of the molecules on the liquid surface layer to evaporate. For this reason, it is better to reduce the energy required for evaporation by breaking a smaller number of hydrogen bonds or forming weak hydrogen bonds to ensure efficient and convenient vapor production.

Nanoarchitectonics of Metallene Materials for Electrocatalysis.

Controlling the synthesis of metal nanostructures is one approach for catalyst engineering and performance optimization in electrocatalysis. As an emerging class of unconventional electrocatalysts, two-dimensional (2D) metallene electrocatalysts with ultrathin sheet-like morphology have gained ever-growing attention and exhibited superior performance in electrocatalysis owing to their distinctive properties originating from structural anisotropy, rich surface chemistry, and efficient mass diffusion capability. Many significant advances in synthetic methods and electrocatalytic applications for 2D metallenes have been obtained in recent years.

Insights into alloy/oxide or hydroxide interfaces in Ni-Mo-based electrocatalysts for hydrogen evolution under alkaline conditions.

Nickel-molybdenum (Ni-Mo) alloys are promising non-noble metal electrocatalysts for the hydrogen evolution reaction (HER) in alkaline water; however, the kinetic origins of their catalytic activities still remain under debate. In this perspective, we systematically summarize the structural characteristics of Ni-Mo-based electrocatalysts recently reported and find that highly active catalysts generally have alloy-oxide or alloy-hydroxide interface structures. Based on the two-step reaction mechanism under alkaline conditions, water dissociation to form adsorbed hydrogen and combination of adsorbed hydrogen into molecular hydrogen, we discuss in detail the relationship between the two types of interface structures obtained by different synthesis methods and their HER performance in Ni-Mo based catalysts.

Extraordinary Acceleration of an Electrophilic Reaction Driven by the Polar Surface of 2D Aluminosilicate Nanosheets.

To increase chemical reaction rates, general solutions include increasing the concentration/temperature and introducing catalysts. In this study, the rate constant of an electrophilic metal coordination reaction is accelerated 23-fold on the surface of layered aluminosilicate (LAS), where the reaction substrate (ligand molecule) induces dielectric polarization owing to the polar and anionic surface. According to the Arrhenius plot, the frequency factor (A) is increased by almost three orders of magnitude on the surface.

Tuning iron spin states in single-atom nanozymes enables efficient peroxidase mimicking.

The large-scale application of nanozymes remains a significant challenge owing to their unsatisfactory catalytic performances. Featuring a unique electronic structure and coordination environment, single-atom nanozymes provide great opportunities to vividly mimic the specific metal catalytic center of natural enzymes and achieve superior enzyme-like activity. In this study, the spin state engineering of Fe single-atom nanozymes (FeNC) is employed to enhance their peroxidase-like activity.

Ni-Fe nanoframes a unique structural formation induced by sonochemical etching.

A uniform nanoframe structure derived from a Prussian blue analogue (PBA) with an internal cavity is successfully synthesized by sonochemical etching. The uniquely structured PBA nanoframes possess a three-dimensional open structure and high surface area, resulting in enhanced electrochemical properties for the oxygen evolution reaction as a model reaction.

New Trends in Nanoarchitectured SERS Substrates: Nanospaces, 2D Materials, and Organic Heterostructures.

This article reviews recent fabrication methods for surface-enhanced Raman spectroscopy (SERS) substrates with a focus on advanced nanoarchitecture based on noble metals with special nanospaces (round tips, gaps, and porous spaces), nanolayered 2D materials, including hybridization with metallic nanostructures (NSs), and the contemporary repertoire of nanoarchitecturing with organic molecules. The use of SERS for multidisciplinary applications has been extensively investigated because the considerably enhanced signal intensity enables the detection of a very small number of molecules with molecular fingerprints. Nanoarchitecture strategies for the design of new NSs play a vital role in developing SERS substrates.

Plasma-Induced Nanocrystalline Domain Engineering and Surface Passivation in Mesoporous Chalcogenide Semiconductor Thin Films.

The synthesis of highly crystalline mesoporous materials is key to realizing high-performance chemical and biological sensors and optoelectronics. However, minimizing surface oxidation and enhancing the domain size without affecting the porous nanoarchitecture are daunting challenges. Herein, we report a hybrid technique that combines bottom-up electrochemical growth with top-down plasma treatment to produce mesoporous semiconductors with large crystalline domain sizes and excellent surface passivation.

Adsorchromism: Molecular Nanoarchitectonics at 2D Nanosheets-Old Chemistry for Advanced Chromism.

Chromism induced by changes in the electronic states of dye molecules due to surface adsorption is termed "adsorchromism" in this article. These changes of molecular electronic states are induced by protonation, aggregation, intramolecular structural changes, and other processes, depending on the surface environment. Intramolecular structural changes, such as co-planarization and decreased molecular motion are the most characteristic and interesting behavior of dye molecules at the surfaces, resulting in spectral shift and/or emission enhancement.

Nanoarchitectured Porous Conducting Polymers: From Controlled Synthesis to Advanced Applications.

Conductive polymers (CPs) integrate the inherent characteristics of conventional polymers and the unique electrical properties of metals. They have aroused tremendous interest over the last decade owing to their high conductivity, robust and flexible properties, facile fabrication, and cost-effectiveness. Compared to bulk CPs, porous CPs with well-defined nano- or microstructures possess open porous architectures, high specific surface areas, more exposed reactive sites, and remarkably enhanced activities.

Enantioselective SERS sensing of pseudoephedrine in blood plasma biomatrix by hierarchical mesoporous Au films coated with a homochiral MOF.

Here, we present a new family of hierarchical porous hybrid materials as an innovative tool for ultrasensitive and selective sensing of enantiomeric drugs in complex biosamples via chiral surface-enhanced Raman spectroscopy (SERS). Hierarchical porous hybrid films were prepared by the combination of mesoporous plasmonic Au films and microporous homochiral metal-organic frameworks (HMOFs). The proposed hierarchical porous substrates enable extremely low limit of detection values (10 M) for pseudoephedrine in undiluted blood plasma due to dual enhancement mechanisms (physical enhancement by the mesoporous Au nanostructures and chemical enhancement by HMOF), chemical recognition by HMOF, and a discriminant function for bio-samples containing large biomolecules, such as blood components.

Nanoarchitectured porous carbons derived from ZIFs toward highly sensitive and selective QCM sensor for hazardous aromatic vapors.

Metal-organic frameworks (MOFs) are a versatile source of carbon nanoarchitectures in gas sensing applications (Torad et al., 2019). Herein, several types of nanoporous carbons (NPCs) have been prepared by in-situ carbothermal treatment of zeolitic imidazolate frameworks (ZIFs) under different inert atmospheres to achieve a highly sensitive discrimination of vaporized aromatic compounds.