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.

Co-expression of multi-genes for polynary perovskite electrocatalysts for reversible solid oxide cells.

High-entropy LnBaCoO perovskites are explored as rSOC air electrodes, though high configuration entropy (S) alone poorly correlates with performance due to multifactorial interactions. We systematically engineer LnBaCoO perovskites (Ln = lanthanides) with tunable S and 20 consistent parameters, employing Bayesian-optimized symbolic regression to decode activity descriptors. The model identifies synergistic contributions from S, ionic radius, and electronegativity, enabling screening of 177,100 compositions.

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.

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.

Enhanced Interface with Strong Charge Delocalization toward Ultralow Overpotential CO Electroreduction.

The construction of an interface has been demonstrated as one of the most insightful strategies for designing efficient catalysts toward electrochemical CO reduction (CORR). However, the weak interfacial interaction and inherent instability inevitably hinder a further performance enhancement in CORR attributable to the interface effect. Herein, 2 nm Ag nanoclusters (Ag NCs) are embedded onto CeO nanospheres (CeO NSs) with highly interconnected porosity (Ag NCs@CeO NSs) to exclusively study the pure interface effect toward CORR.

Oxygen vacancy-mediated peroxydisulfate activation and singlet oxygen generation toward 2,4-dichlorophenol degradation on specific CuO nanosheets.

Durable and stable removal of 2,4-dichlorophenpl (2,4-DCP) by CuO nanosheets is reported. CuO nanosheets were fabricated by a simple defect engineering strategy and greatly increased the efficiency of peroxydisulfate (PDS) activation to improve 2,4-DCP removal by introducing abundant oxygen vacancy (V) to produce an electron-rich surface. Results showed that CuO nanosheets exposed more V as active sites for PDS activation as compared with that of CuO nanoparticles, giving rise to dramatic enhancement of catalytic performance with ultrahigh reaction rate that is qualified for serving in flow filtration system, completely degrading 100 mg L of 2,4-DCP within 3 s of residence time.

Theory-Guided Modulation of Optimal Silver Nanoclusters toward Efficient CO Electroreduction.

Electrochemical CO reduction reaction (CORR), when powered with intermittent but renewable energies, holds an attractive potential to close the anthropogenic carbon cycle through efficiently converting the exorbitantly discharged CO to value-added fuels and/or chemicals and consequently reduce the greenhouse gas emission. Through systematically integrating the density functional theory calculations, the modeling statistics of various proportions of CORR-preferred electroactive sites, and the theoretical work function results, it is found that the crystallographically unambiguous Ag nanoclusters (NCs) hold a high possibility to enable an outstanding CORR performance, particularly at an optimal size of around 2 nm. Motivated by this, homogeneously well-distributed ultrasmall Ag NCs with an average size of ∼2 nm (2 nm Ag NCs) were thus synthesized to electrochemically promote CORR, and the results demonstrate that the 2 nm Ag NCs are able to achieve a significantly larger CO partial current density [], an impressively higher CO Faraday efficiency of over 93.

Interface-Induced Electrocatalytic Enhancement of CO -to-Formate Conversion on Heterostructured Bismuth-Based Catalysts.

Electrochemical CO reduction reaction (CO RR) is a promising approach to convert CO to carbon-neutral fuels using external electric powers. Here, the Bi S -Bi O nanosheets possessing substantial interface being exposed between the connection of Bi S and Bi O are prepared and subsequently demonstrate to improve CO RR performance. The electrocatalyst shows formate Faradaic efficiency (FE) of over 90% in a wide potential window.

Hexagonal Zn Nanoplates Enclosed by Zn(100) and Zn(002) Facets for Highly Selective CO Electroreduction to CO.

Electrochemical reduction of CO to carbon-neutral fuels is a promising strategy for renewable energy conversion and storage. However, developing earth-abundant and cost-effective electrocatalysts with high catalytic activity and desirable selectivity for the target fuel is still challenging and imperative. Herein, hexagonal Zn nanoplates (H-Zn-NPs) enclosed by Zn(100) and Zn(002) facets were successfully synthesized and studied for their feasibility toward the CO reduction reaction (CORR).

Bi O Nanosheets Grown on Multi-Channel Carbon Matrix to Catalyze Efficient CO Electroreduction to HCOOH.

Bi O nanosheets were grown on a conductive multiple channel carbon matrix (MCCM) for CO RR. The obtained electrocatalyst shows a desirable partial current density of ca. 17.

Achieving Efficient CO Electrochemical Reduction on Tunable In(OH)-Coupled CuO-Derived Hybrid Catalysts.

Tunable In(OH)-coupled CuO-derived hybrid catalysts are facilely synthesized to boost the selectivity and efficiency of the electrochemical CO reduction reaction (CORR). The maximum faradaic efficiency (FE) of 90.37% for CO production is achieved at -0.

Efficient Electrochemical Reduction of CO to HCOOH over Sub-2 nm SnO Quantum Wires with Exposed Grain Boundaries.

Electrochemical reduction of CO could mitigate environmental problems originating from CO emission. Although grain boundaries (GBs) have been tailored to tune binding energies of reaction intermediates and consequently accelerate the CO reduction reaction (CO RR), it is challenging to exclusively clarify the correlation between GBs and enhanced reactivity in nanostructured materials with small dimension (<10 nm). Now, sub-2 nm SnO quantum wires (QWs) composed of individual quantum dots (QDs) and numerous GBs on the surface were synthesized and examined for CO RR toward HCOOH formation.

Insights into the Interfacial Process in Electroless Ni-P Coating on Supercritical CO Transport Pipeline as Relevant to Carbon Capture and Storage.

To reduce the amount of greenhouse gas emissions and remedy related environmental damage, the research on carbon capture and storage (CCS) is gaining momentum and so is the search for a more effective way to control corrosion of pipeline steel used to transport impure supercritical (SC) CO. Herein, we prepared an electroless high-phosphorus Ni-P coating and, for the first time, systematically explored the underlying mechanism of the interfacial process in applying Ni-P coating to protect pipeline steel that transports impure SC CO. It is found that, benefiting from the formation of a protective surface film, Ni-P coating significantly mitigates the corrosion effects from SC CO and impurities (e.

Shape-Dependent Electrocatalytic Reduction of CO to CO on Triangular Silver Nanoplates.

Electrochemical reduction of CO (CORR) provides great potential for intermittent renewable energy storage. This study demonstrates a predominant shape-dependent electrocatalytic reduction of CO to CO on triangular silver nanoplates (Tri-Ag-NPs) in 0.1 M KHCO.