Pd Single-Atoms Doped CuP Quantum Dots with Moderately Optimized H* Sorption Behaviors for Actualizing the Multifunctional "Formaldehyde-Nitrate" Galvanic System.

Nitrate and formaldehyde, which are substantial wastes in industrial and agricultural effluents, pose significant hazards to the human health and ecosystem. Current purification technologies remain great challenges due to the unsatisfactory energy-intensive, time-consuming and noticeably costly reasons. Herein, a bifunctional electrocatalysts of Pd single-atoms doped CuP quantum dots (Pd-CuP SA-QDs) are reported to moderately optimize the H* sorption behaviors for accelerating the kinetics of nitrate reduction (NORR) and formaldehyde oxidation (FOR) reactions in a dual-directional way, thus realizing the high activity and selectivity for both cathodic ammonia (NH) synthesis and anodic H production concurrently.

Reversed linkage-oriented intermolecular electron-transfer in isomeric covalent organic frameworks for electrochemical CO reduction.

Designing specific electroactive sites and modulating their local microenvironments of covalent organic frameworks (COFs) toward electrochemical CO reduction (ECR) have received increasing attention. However, the underlying impact of the change in intramolecular electron-transfer capability, caused by the tuning in electronic state of active sites, on the redox-mediated catalytic process still remains inadequately understood. In this work, we constructed a metalloporphyrin-based COF as the isomer of the representative COF-367-Co, with an identical chemical composition but a reversed imine-linkage orientation via Schiff-base condensation reaction using [meso-tetrakis(4-formylphenyl)porphyrin]cobalt (CoTFPP) and Benzidine (BD) as the precursors, denoted as CoTFPP-BD-COF, to exclusively investigate the linkage orientation as an individual variable for enhanced electron transmission efficiency toward ECR.

Nickel-Coated Copper Foam Electrocatalytic Electrode for Energy-Saving Hydrogen Evolution and Value-Added Chemical Co-Generation.

Developing cost-effective, eco-friendly electrocatalysts with strong electrochemical performance is essential for advancing in water electrolysis. Noble metal-based catalysts offer excellent activity, but due to less availability and more expenses leads to an urgent demand for efficient, affordable, and earth-abundant alternatives. In this study, a bimetallic foam architecture (CuF@Ni) was fabricated by electrodeposition of Ni on CuF.

Unraveling Double-Exchange Effect Coupling Spin Modulation of SrFeMoO Electrocatalyst for Solid Oxide Cells.

Perovskites are promising electrocatalysts for solid oxide cells (SOCs) due to their tunable structures. The reactivity/stability can be effectively enhanced by tuning the spin, whereas few studies have been able to elucidate the correlation between spin and reactivity/stability. Herein, the double-exchange effect coupling spin modulation is studied for SrFeNiMoO, which exhibits a current density of 2.

Manipulation of Hydrogen Transfer Behaviors by RhCu Alloying Enables an All-in-one Sustainable "Furfural-Nitrate" System.

Nitrate and furfural are typical wastes mainly from industrialization and agriculturalization progresses, and their clean conversions are still very challenging for a sustainable future. Nevertheless, scant attention has been devoted to the core issues: the rational integration of two wastes recycling and the targeted manipulation of hydrogen (H*) transfer behaviors to address their sluggish reaction kinetics. Herein, we report an all-in-one electrochemical energy system that is thermodynamically designed by coupling nitrate reduction (NORR) and furfural oxidation reactions (FORs) together.

Correction: Advanced fabrication techniques for polymer-metal nanocomposite films: state-of-the-art innovations in energy and electronic applications.

[This corrects the article DOI: 10.1039/D4SC04600E.].

Golden Single-Atom Alloys Selectively Boosting Oxygen Reduction and Methanol Oxidation.

Engineering electrocatalysts at a single-atomic site can enable unprecedented atomic utilization and catalytic activity, yet it remains challenging in multimetallic active centers to simultaneously achieve high catalytic selectivity and stability. Herein, the atomic design and control of golden single-atom alloys (PdAu and PtAu SAAs) based on fully ordered PdBi and PtBi matrixes is presented, serving as highly selective, active, and stable cathode and anode electrocatalysts, respectively, to trigger direct methanol fuel cell (DMFC). The octahedral PdAu SAA exhibits ultrahigh mass-activity of 5.

Boosting Alcohol Oxidation Electrocatalysis with Multifactorial Engineered Pd/Pt Single-Atom Alloy-BiO Adatoms Surface.

Engineering nanomaterials at single-atomic sites could enable unprecedented catalytic properties for broad applications, yet it remains challenging to do so on the surface of multimetallic nanocrystals. Herein, we present the multifactorial engineering (size, shape, phase, and composition) of the fully ordered PtBi nanoplates at atomic level, achieving a unique catalyst surface where the face-centered cubic (fcc) Pt edges are modified by the isolated Pd atoms and BiO adatoms. This Pd/Pt-BiO electrocatalyst exhibits an ultrahigh mass activity of 16.

Highly Diluted Pt Atoms Modified RhBi Intermetallic Nanoplates Boost Ethanol Oxidation Electrocatalysis.

Engineering Pt-based multimetallic nanoalloys could boost electrocatalysis in broad applications, yet it remains challenging in terms of its rational design and synthesis of a highly diluted alloy with unprecedented Pt atomic utilization. Herein, atomically dispersed Pt anchored on the surface of novel RhBi intermetallic nanoplates (RhBi-Pt) is achieved by atomic replacement, which transforms into a tensile-strained and highly diluted RhPt alloy (RhBi@RhPt) via electrochemical dealloying. Due to the diluted Pt atoms and tensile-strained Rh shell, the RhBi@RhPt electrocatalyst exhibits a remarkably enhanced peak mass activity of 32459.

Lattice Oxygen-Driven Co-Adsorption of Carbon Dioxide and Nitrate on Copper: A Pathway to Efficient Urea Electrosynthesis.

The electrochemical coupling of CO and NO on copper-based catalysts presents a sustainable strategy for urea production while simultaneously addressing wastewater denitrification. However, the inefficient random adsorption of CO and NO on the copper surface limits the interaction of the key carbon and nitrogen intermediates, thereby impeding efficient C-N coupling. In this study, we demonstrate that the residual lattice oxygen in oxide-derived copper nanosheets (O-Cu) can effectively tune the electron distribution, thus activating neighboring copper atoms and generating electron-deficient copper (Cu) sites.

Advanced fabrication techniques for polymer-metal nanocomposite films: state-of-the-art innovations in energy and electronic applications.

Polymer-metal nanocomposites are a fascinating class of materials that synergize the distinct properties of polymers and metals. Incorporating metal nanofillers into polymer matrices significantly enhances electrical conductivity, mechanical strength, and thermal stability through intricate chemical interactions. This review provides an in-depth understanding of current and emerging fabrication techniques for polymer-metal nanocomposite films, with a particular focus on advanced chemical mechanisms and the resulting material properties.

Phase-Engineered Bi-RuO Single-Atom Alloy Oxide Boosting Oxygen Evolution Electrocatalysis in Proton Exchange Membrane Water Electrolyzer.

Engineering nanomaterials at single-atomic sites can enable unprecedented catalytic properties for broad applications, yet it remains challenging to do so on RuO-based electrocatalysts for proton exchange membrane water electrolyzer (PEMWE). Herein, the rational design and construction of Bi-RuO single-atom alloy oxide (SAAO) are presented to boost acidic oxygen evolution reaction (OER), via phase engineering a novel hexagonal close packed (hcp) RuBi single-atom alloy. This Bi-RuO SAAO electrocatalyst exhibits a low overpotential of 192 mV and superb stability over 650 h at 10 mA cm, enabling a practical PEMWE that needs only 1.

Integrated "Two-in-One" Strategy for High-Rate Electrocatalytic CO Reduction to Formate.

The electrochemical CO reduction reaction (ECR) is a promising pathway to producing valuable chemicals and fuels. Despite extensive studies reported, improving CO adsorption for local CO enrichment or water dissociation to generate sufficient H* is still not enough to achieve industrial-relevant current densities. Herein, we report a "two-in-one" catalyst, defective Bi nanosheets modified by CrO (Bi-CrO), to simultaneously promote CO adsorption and water dissociation, thereby enhancing the activity and selectivity of ECR to formate.

Strong effect-correlated electrochemical CO reduction.

Electrochemical CO reduction (ECR) holds great potential to alleviate the greenhouse effect and our dependence on fossil fuels by integrating renewable energy for the electrosynthesis of high-value fuels from CO. However, the high thermodynamic energy barrier, sluggish reaction kinetics, inadequate CO conversion rate, poor selectivity for the target product, and rapid electrocatalyst degradation severely limit its further industrial-scale application. Although numerous strategies have been proposed to enhance ECR performances from various perspectives, scattered studies fail to comprehensively elucidate the underlying effect-performance relationships toward ECR.

Local hydroxide ion enrichment at the inner surface of lacunaris perovskite nanotubes facilitates the oxygen evolution reaction.

Numerous strategies have been devised to optimize the intrinsic activity of perovskite oxides for the oxygen evolution reaction (OER). However, conventional synthetic routes typically yield limited numbers of active sites and low mass activities. More critically, the sluggish mass transfer poses a huge challenge, particularly under high polarization conditions, which impedes the overall reaction kinetics.

Oxygen Vacancy-Driven Heterointerface Breaks the Linear-Scaling Relationship of Intermediates toward Electrocatalytic CO Reduction.

Smart metal-metal oxide heterointerface construction holds promising potentials to endow an efficient electron redistribution for electrochemical CO reduction reaction (CORR). However, inhibited by the intrinsic linear-scaling relationship, the binding energies of competitive intermediates will simultaneously change due to the shifts of electronic energy level, making it difficult to exclusively tailor the binding energies to target intermediates and the final CORR performance. Nonetheless, creating specific adsorption sites selective for target intermediates probably breaks the linear-scaling relationship.

Visualizing Electrochemical CO Conversion via the Emerging Scanning Electrochemical Microscope: Fundamentals, Applications and Perspectives.

With the rapid development and maturity of electrochemical CO conversion involving cathodic CO reduction reaction (CORR) and anodic oxygen evolution reaction (OER), conventional ex situ characterizations gradually fall behind in detecting real-time products distribution, tracking intermediates, and monitoring structural evolution, etc. Nevertheless, advanced in situ techniques, with intriguing merits like good reproducibility, facile operability, high sensitivity, and short response time, can realize in situ detection and recording of dynamic data, and observe materials structural evolution in real time. As an emerging visual technique, scanning electrochemical microscope (SECM) presents local electrochemical signals on various materials surface through capturing micro-current caused by reactants oxidation and reduction.

Perovskite Oxides Toward Oxygen Evolution Reaction: Intellectual Design Strategies, Properties and Perspectives.

Developing electrochemical energy storage and conversion devices (e.g., water splitting, regenerative fuel cells and rechargeable metal-air batteries) driven by intermittent renewable energy sources holds a great potential to facilitate global energy transition and alleviate the associated environmental issues.

Surface-Enriched Single-Bi-Atoms Tailoring of Pt Nanorings for Direct Methanol Fuel Cells with Ultralow-Pt-Loading.

Single-atom decorating of Pt emerges as a highly effective strategy to boost catalytic properties, which can trigger the most Pt active sites while blocking the smallest number of Pt atoms. However, the rational design and creation of high-density single-atoms on Pt surface remain as a huge challenge. Herein, a customized synthesis of surface-enriched single-Bi-atoms tailored Pt nanorings (SE-Bi/Pt NRs) toward methanol oxidation is reported, which is guided by the density functional theory (DFT) calculations suggesting that a relatively higher density of Bi species on Pt surface can ensure a CO-free pathway and accelerate the kinetics of *HCOOH formation.

Atomic Diffusion Engineered PtSnCu Nanoframes with High-Index Facets Boost Ethanol Oxidation.

Electrochemical ethanol oxidation is crucial to directly convert a biorenewable liquid fuel with high energy density into electrical energy, but it remains an inefficient reaction even with the best catalysts. To boost ethanol oxidation, developing multimetallic nanoalloy has emerged as one of the most effective strategies, yet faces a challenge in the rational engineering of multimetallic active-site ensembles at atomic-level. Herein, starting from typical PtCu nanocrystals, an atomic Sn diffusion strategy is developed to construct well-defined PtSnCu octopod nanoframes, which is enclosed by high-index facets of n (111)-(111), such as {331} and {221}.

Emerging Nanomaterials toward Uranium Extraction from Seawater: Recent Advances and Perspectives.

Nuclear energy holds great potential to facilitate the global energy transition and alleviate the increasing environmental issues due to its high energy density, stable energy output, and carbon-free emission merits. Despite being limited by the insufficient terrestrial uranium reserves, uranium extraction from seawater (UES) can offset the gap. However, the low uranium concentration, the complicated uranium speciation, the competitive metal ions, and the inevitable marine interference remarkably affect the kinetics, capacity, selectivity, and sustainability of UES materials.

Interfacial Electronic Modulation of Dual-Monodispersed Pt-NiS as Efficacious Bi-Functional Electrocatalysts for Concurrent H Evolution and Methanol Selective Oxidation.

Constructing the efficacious and applicable bi-functional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction (OER) are critical to the development of electrochemically-driven technologies for efficient hydrogen production and avoid CO emission. Herein, the hetero-nanocrystals between monodispersed Pt (~ 2 nm) and NiS (~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H generation.

Capturing critical gem-diol intermediates and hydride transfer for anodic hydrogen production from 5-hydroxymethylfurfural.

The non-classical anodic H production from 5-hydroxymethylfurfural (HMF) is very appealing for energy-saving H production with value-added chemical conversion due to the low working potential (~0.1 V vs RHE). However, the reaction mechanism is still not clear due to the lack of direct evidence for the critical intermediates.