Chiral Inorganic Polar BaTiO/BaCO Nanohybrids with Spin Selection for Asymmetric Photocatalysis.

Chirality-dependent photocatalysis is an emerging domain that leverages unique chiral light-matter interactions for enabling asymmetric catalysis driven by spin polarization induced by circularly polarized light selection. Herein, we synthesize chiral inorganic polar BaTiO/BaCO nanohybrids for asymmetric photocatalysis via a hydrothermal method employing chiral glucose as a structural inducer. When excited by opposite circularly polarized light, the same material exhibits significant asymmetric catalysis, while enantiomers present an opposite polarization preference.

Enhancing the efficiency of PVDF-based piezoelectric catalysis through water-induced polarization and a micro-nano-composite strategy.

Polyvinylidene fluoride (PVDF)-based piezoelectric catalysts show promise in mechanical force-driven catalysis due to their good biocompatibility, flexibility, and ease of fabrication. However, the catalytic activity of pristine PVDF is limited due to its low piezoelectric phase content (<20%), poor orientation, and low surface carrier concentration. Here, we introduce an efficient PVDF-based composite nano-catalyst (rGO/PVDF) with high piezoelectric catalytic performance.

Integrated MXene and metal oxide electrocatalysts for the oxygen evolution reaction: synthesis, mechanisms, and advances.

Electrochemical water splitting is a promising approach to produce H through renewable electricity, but its energy efficiency is severely constrained by the kinetically slow anodic oxygen evolution reaction (OER), which uses about 90% of the electricity in the water-splitting process due to its multistep proton (H)-coupled electron (e) transfer process, high overpotential (), and low energy efficiency. Therefore, the quest for efficient, sustainable, and cost-effective electrocatalysts for hydrogen production through water electrolysis has intensified, highlighting the potential of two-dimensional (2D) MXenes. MXenes have emerged as a promising class of materials characterized by excellent stability, hydrophilicity, and conductivity.

Magnetic Hydrogel Microbots for Efficient Pollutant Decontamination and Self-Catalyzed Regeneration in Continuous Flow Systems.

The efficient removal of organic pollutants from water is crucial for protecting human health and the ecosystem. While adsorbent-based approaches offer advantages over traditional chemical and thermal methods, they still suffer from slow adsorption kinetics, high energy demand, and limited material lifespan. Herein, an efficient decontamination platform is introduced, using magnetic hydrogel microbots (MHMs) made from picolitre-sized hydrogel droplets coated with multifunctional magnetic nanoparticles.

Effective Interfacing of Surface Homojunctions on Chemically Identical g-CN for Efficient Visible-Light Photocatalysis without Sacrificial Agents.

Developing efficient homojunctions on g-CN promises metal-free photocatalysis to realize truly sustainable artificial photosynthesis. However, current designs are limited by hindered charge separation due to inevitable grain boundaries and random formation of ineffective homojunctions embedded within the photocatalyst. Here, efficient photocatalysis is driven by introducing effective surface homojunctions on chemically and structurally identical g-CN through leveraging its size-dependent electronic properties.

Lithiophilic Hydrogen-Substituted Graphdiyne Aerogels with Ionically Conductive Channels for High-Performance Lithium Metal Batteries.

Lithium (Li) metal stands as a promising anode in advancing high-energy-density batteries. However, intrinsic issues associated with metallic Li, especially the dendritic growth, have hindered its practical application. Herein, we focus on molecular combined structural design to develop dendrite-free anodes.

Harmonizing Plasmonic and Photonic Effects to Boost Photocatalytic H Production over 550 mmol ⋅ h ⋅ g .

Integrating plasmonic nanoparticles with photonic crystals holds immense potential to enhance green hydrogen photosynthesis by amplifying localized electromagnetic field through generating surface plasmons and slow photons. Current plasmonic photonic designs primarily employ semiconductor-based structural backbone deposited with plasmonic nanoparticles. However, the competition between various optical phenomena in these ensembles hinders effective field enhancement rather than facilitating it.

Integrating photothermal and plasmonic catalysis induced by near-infrared light for efficient reduction of 4-nitrophenol.

The reduction of 4-nitrophenol (4-NP) into 4-aminophenol (4-AP) is an important reaction in both chemical manufacturing and environmental protection. The design of a highly active, multifunctional and reusable catalyst for efficient 4-NP decontamination/valorization is therefore crucial to bring in economic and societal benefits. Herein, we achieve an efficient plasmonic-photothermal catalyst of Pd nanoparticles by growing them on graphene-polyelectrolytes self-assembly nanolayers via an in situ green reduction approach using polyelectrolyte as the reductant.

Chaotropic Nanoelectrocatalysis: Chemically Disrupting Water Intermolecular Network at the Point-of-Catalysis to Boost Green Hydrogen Electrosynthesis.

Efficient green hydrogen production through electrocatalytic water splitting serves as a powerful catalyst for realizing a carbon-free hydrogen economy. However, current electrocatalytic designs face challenges such as poor hydrogen evolution reaction (HER) performance (Tafel slope, 100-140 mV dec ) because water molecules are thermodynamically trapped within their extensive hydrogen bonding network. Herein, we drive efficient HER by manipulating the local water microenvironment near the electrocatalyst.

Catalyst-On-Hotspot Nanoarchitecture: Plasmonic Focusing of Light onto Co-Photocatalyst for Efficient Light-To-Chemical Transformation.

Plasmon-mediated catalysis utilizing hybrid photocatalytic ensembles promises effective light-to-chemical transformation, but current approaches suffer from weak electromagnetic field enhancements from polycrystalline and isotropic plasmonic nanoparticles as well as poor utilization of precious co-catalyst. Here, efficient plasmon-mediated catalysis is achieved by introducing a unique catalyst-on-hotspot nanoarchitecture obtained through the strategic positioning of co-photocatalyst onto plasmonic hotspots to concentrate light energy directly at the point-of-reaction. Using environmental remediation as a proof-of-concept application, the catalyst-on-hotspot design (edge-AgOcta@CuO) enhances photocatalytic advanced oxidation processes to achieve superior organic-pollutant degradation at ≈81% albeit having lesser CuO co-photocatalyst than the fully deposited design (full-AgOcta@CuO).

Surface-Degenerate Semiconductor Photocatalysis for Efficient Water Splitting without Sacrificial Agents via a Reticular Chemistry Approach.

The production of green hydrogen through photocatalytic water splitting is crucial for a sustainable hydrogen economy and chemical manufacturing. However, current approaches suffer from slow hydrogen production (<70 μmol ⋅ g  ⋅ h ) due to the sluggish four-electrons oxygen evolution reaction (OER) and limited catalyst activity. Herein, we achieve efficient photocatalytic water splitting by exploiting a multifunctional interface between a nano-photocatalyst and metal-organic framework (MOF) layer.

Incorporating Chaotropic/Kosmotropic Chemistries onto Plasmonic Nanoheater to Boost Steam Generation Beyond its Photothermal Property.

Photothermal steam generation promises decentralized water purification, but current methods suffer from slow water evaporation even at high photothermal efficiency of ≈98%. This drawback arises from the high latent heat of vaporization that is required to overcome the strong and extensive hydrogen bonding network in water for steam generation. Here, light-to-vapor conversion is boosted by incorporating chaotropic/kosmotropic chemistries onto plasmonic nanoheater to manipulate water intermolecular network at the point-of-heating.

Superlattice-based Plasmonic Catalysis: Concentrating Light at the Nanoscale to Drive Efficient Nitrogen-to-Ammonia Fixation at Ambient Conditions.

Plasmonic catalysis promises green ammonia synthesis but is limited by the need for co-catalysts and poor performances due to weak electromagnetic field enhancement. Here, we use two-dimensional plasmonic superlattices with dense electromagnetic hotspots to boost ambient nitrogen-to-ammonia photoconversion without needing co-catalyst. By organizing Ag octahedra into a square superlattice to concentrate light, the ammonia formation is enhanced by ≈15-fold and 4-fold over hexagonal superlattice and disorganized array, respectively.

Dynamic Liquid-Liquid Interface: Applying a Spinning Interfacial Microreactor to Actively Converge Biphasic Reactants for the Enhanced Interfacial Reaction.

A liquid-liquid interfacial reaction combines reactants with large polarity disparity to achieve greener and more efficient chemistry that is otherwise challenging in traditional single-phase systems. However, current interfacial approaches suffer from the need for a large amount of solvent/reactant/emulsifier and poor reaction performance arising from intrinsic thermodynamic constraints. Herein, we achieve an efficient interfacial reaction by creating a magnetic-responsive, microscale liquid-liquid interface and exploit its dynamic spinning motion to generate vortex-like hydrodynamic flows that rapidly converge biphasic reactants to the point-of-reaction.

An archetype of the electron-unobstructed core-shell composite with inherent selectivity: conductive metal-organic frameworks encapsulated with metal nanoparticles.

The acquisition of monodisperse metal nanoparticles covered by conductive metal-organic frameworks (cMOFs) is an archetype of an electron-unobstructed core-shell composite, valued for its potential electrocatalytic ability and selectivity enhancement. In this work, Pt@cMOF composites with direct interfaces showed better performance in the oxygen reduction reaction than composites with indirect interfaces or with lower electroconductivity shells. This composite was proved to exhibit the ability to expedite electron transfer with different thicknesses of electrode materials.

Cold-Starting All-Solid-State Batteries from Room Temperature by Thermally Modulated Current Collector in Sub-Minute.

All-solid-state batteries (ASSBs) show great potential as high-energy and high-power energy-storage devices but their attainable energy/power density at room temperature is severely reduced because of the sluggish kinetics of lithium-ion transport. Here a thermally modulated current collector (TMCC) is reported, which can rapidly cold-start ASSBs from room temperature to operating temperatures (70-90 °C) in less than 1 min, and simultaneously enhance the transient peak power density by 15-fold compared to one without heating. This TMCC is prepared by integrating a uniform, ultrathin (≈200 nm) nickel layer as a thermal modulator within an ultralight polymer-based current collector.

Noninvasive and Point-of-Care Surface-Enhanced Raman Scattering (SERS)-Based Breathalyzer for Mass Screening of Coronavirus Disease 2019 (COVID-19) under 5 min.

Population-wide surveillance of COVID-19 requires tests to be quick and accurate to minimize community transmissions. The detection of breath volatile organic compounds presents a promising option for COVID-19 surveillance but is currently limited by bulky instrumentation and inflexible analysis protocol. Here, we design a hand-held surface-enhanced Raman scattering-based breathalyzer to identify COVID-19 infected individuals in under 5 min, achieving >95% sensitivity and specificity across 501 participants regardless of their displayed symptoms.

Electrolyte-Resistant Dual Materials for the Synergistic Safety Enhancement of Lithium-Ion Batteries.

Safety issues associated with lithium-ion batteries are of major concern, especially with the ever-growing demand for higher-energy-density storage devices. Although flame retardants (FRs) added to electrolytes can reduce fire hazards, large amounts of FRs are required and they severely deteriorate battery performance. Here, we report a feasible method to balance flame retardancy and electrochemical performance by coating an electrolyte-insoluble FR on commercial battery separators.

Designing a Nanoscale Three-phase Electrochemical Pathway to Promote Pt-catalyzed Formaldehyde Oxidation.

Gas-phase heterogeneous catalysis is a process spatially constrained on the two-dimensional surface of a solid catalyst. Here, we introduce a new toolkit to open up the third dimension. We discovered that the activity of a solid catalyst can be dramatically promoted by covering its surface with a nanoscale-thin layer of liquid electrolyte while maintaining efficient delivery of gas reactants, a strategy we call three-phase catalysis.

Modulating Orientational Order to Organize Polyhedral Nanoparticles into Plastic Crystals and Uniform Metacrystals.

In nanoparticle self-assembly, the current lack of strategy to modulate orientational order creates challenges in isolating large-area plastic crystals. Here, we achieve two orientationally distinct supercrystals using one nanoparticle shape, including plastic crystals and uniform metacrystals. Our approach integrates multi-faceted Archimedean polyhedra with molecular-level surface polymeric interactions to tune nanoparticle orientational order during self-assembly.

Differentiation of Multiplex Noncovalent Interactions Using SERS and Chemometrics.

Probing changes of noncovalent interactions is crucial to study the binding efficiencies and strengths of (bio)molecular complexes. While surface-enhanced Raman scattering (SERS) offers unique molecular fingerprints to examine such interactions , current platforms are only able to recognize hydrogen bonds because of their reliance on manual spectral identification. Here, we differentiate multiple intermolecular interactions between two interacting species by synergizing plasmonic liquid marble-based SERS platforms, chemometrics, and density functional theory.

Incorporating the Nanoscale Encapsulation Concept from Liquid Electrolytes into Solid-State Lithium-Sulfur Batteries.

Solid-state Li-S batteries are attractive due to their high energy density and safety. However, it is unclear whether the concepts from liquid electrolytes are applicable in the solid state to improve battery performance. Here, we demonstrate that the nanoscale encapsulation concept based on LiS@TiS core-shell particles, originally developed in liquid electrolytes, is effective in solid polymer electrolytes.

Applying a Nanoparticle@MOF Interface To Activate an Unconventional Regioselectivity of an Inert Reaction at Ambient Conditions.

Here we design an interface between a metal nanoparticle (NP) and a metal-organic framework (MOF) to activate an inert CO carboxylation reaction and in situ monitor its unconventional regioselectivity at the molecular level. Using a Kolbe-Schmitt reaction as model, our strategy exploits the NP@MOF interface to create a pseudo high-pressure CO microenvironment over the phenolic substrate to drive its direct C-H carboxylation at ambient conditions. Conversely, Kolbe-Schmitt reactions usually demand high reaction temperature (>125 °C) and pressure (>80 atm).

ZIF-Induced d-Band Modification in a Bimetallic Nanocatalyst: Achieving Over 44 % Efficiency in the Ambient Nitrogen Reduction Reaction.

The electrochemical nitrogen reduction reaction (NRR) offers a sustainable solution towards ammonia production but suffers poor reaction performance owing to preferential catalyst-H formation and the consequential hydrogen evolution reaction (HER). Now, the Pt/Au electrocatalyst d-band structure is electronically modified using zeolitic imidazole framework (ZIF) to achieve a Faradaic efficiency (FE) of >44 % with high ammonia yield rate of >161 μg mg  h under ambient conditions. The strategy lowers electrocatalyst d-band position to weaken H adsorption and concurrently creates electron-deficient sites to kinetically drive NRR by promoting catalyst-N interaction.

Multiplex Surface-Enhanced Raman Scattering Identification and Quantification of Urine Metabolites in Patient Samples within 30 min.

Successful translation of laboratory-based surface-enhanced Raman scattering (SERS) platforms to clinical applications requires multiplex and ultratrace detection of small biomarker molecules from a complex biofluid. However, these biomarker molecules generally exhibit low Raman scattering cross sections and do not possess specific affinity to plasmonic nanoparticle surfaces, significantly increasing the challenge of detecting them at low concentrations. Herein, we demonstrate a "confine-and-capture" approach for multiplex detection of two families of urine metabolites correlated with miscarriage risks, 5β-pregnane-3α,20α-diol-3α-glucuronide and tetrahydrocortisone.