Interfacial Diffusion-Reaction Coupling Strategy for CO Reduction on Copper Surface in Acidic Medium.

CO electroreduction reaction in acid medium to produce multicarbon (C) products has gained attention as an alternative to the traditional processes in neutral or alkaline solutions which often suffer from low single-pass conversion efficiency due to (bi)carbonate accumulation at the cathode. However, the CO conversion efficiency in acid remains unsatisfactory. Herein, a strong-polarized layer-covered Cu catalyst is developed as electrode for CO reduction reaction (CORR) in acid.

Pt-Decorated NiMo/Carbon Hybrid Catalysts for High-Current-Density Hydrogen Evolution: Synergistic Electronic Modulation and Industrial Application Potential.

In response to the urgent demand for sustainable hydrogen production under industrial high-current-density conditions, this study presents the development of a Pt-decorated NiMo-based carbon-supported catalyst (Pt-NiMo/C) for efficient alkaline hydrogen evolution reaction (HER). The catalyst was synthesized via a solvent evaporation method followed by high-temperature pyrolysis, achieving uniform dispersion of Pt-NiMo nanoparticles on conductive carbon. Electrochemical evaluations revealed exceptional HER performance with ultralow overpotentials of 20 and 170 mV versus RHE at current densities of 10 and 100 mA cm⁻, respectively, surpassing commercial Pt/C benchmarks.

Rational Synthesis of Isomeric Graphdiyne Frameworks toward Single-Ruthenium Catalysts and High-Performance Nitrogen Reduction.

Graphdiynes (GDYs), synthesized via direct coupling of arylacetylenes, have attracted great attention due to their unique electronic properties and structural diversity, typically forming 2D layered frameworks. However, crystalline GDY-like frameworks with 3D topology remain challenging to synthesize. Here, the study reports two highly crystalline, isomeric GDY-like frameworks with ThSi2 topology, constructed from 2,2'-binaphthalene and 6,6'-biazulene-based monomers.

Anion-Exchange Strategy for Ru/RuO-Embedded N/S--Doped Porous Carbon Composites for Electrochemical Nitrogen Fixation.

Ionic porous polymers have been widely utilized efficiently to anchor various metal atoms for the preparation of metal-embedded heteroatom-doped porous carbon composites as the active materials for electrocatalytic applications. However, the rational design of the heteroatom and metal elements in HPC-based composites remains a significant challenge, due to the tendency of the aggregation of metal nanoparticles during pyrolysis. In this study, a nitrogen (N)- and sulfur (S)-enriched ionic covalent organic framework (COF) incorporating viologen and thieno[3,4-b] thiophene (TbT) was constructed via Zincke-type polycondensation.

Integrated Electrochemical Biomass Oxidation and CO Reduction over Ultra-wide Potential Window.

Electrochemical reduction of carbon dioxide (CO) coupled with biomass oxidation using renewable electricity is considered as a promising strategy for carbon management. However, achieving both high selectivity and large current density over wide potential window remains a significant challenge, hindering practical applications. In this study, a Ni/Fe dual metal-atom catalyst is developed for CO reduction, achieving nearly 100 % CO selectivity across an ultra-wide potential window of 1.

Heteroarchitectural Gas Diffusion Layer Promotes CO Reduction Coupled with Biomass Oxidation at Ampere-Level Current Density.

Achieving high product selectivity at ampere-level current densities is essential for the industrial application of electrochemical CO reduction. However, the operational stability of CO electrolyzers at large current density has long been hindered by flooding of gas diffusion layer (GDL). Herein, a new heteroarchitectural GDL is designed to overcome flooding.

Large Dipole Moment Enhanced CO Adsorption on Copper Surface: Achieving 68.9% Catalytic Ethylene Faradaic Efficiency at 1.0 A cm.

The electrochemical conversion of carbon dioxide (CO) into hydrocarbon products emerges as a pivotal sustainable strategy for carbon utilization. Cu-based catalysts are currently prioritized as the most effective means for this process, yet it remains a long-term goal to achieve high product selectivity at elevated current densities. This study delved into exploring the influence of a topological poly(2-aminoazulene) with a substantial dipole moment on modulating the Cu surface dipole field to augment the catalytic activity involved in CO reduction.

Two-Dimensional Silver-Isocyanide Frameworks.

Metal-organic frameworks (MOFs) have been widely studied due to their versatile applications and easily tunable structures. However, heteroatom-metal coordination dominates the MOFs community, and the rational synthesis of carbon-metal coordination-based MOFs remains a significant challenge. Herein, two-dimensional (2D) MOFs based on silver-carbon linkages are synthesized through the coordination between silver(I) salt and isocyanide-based monomers at ambient condition.

Well-defined asymmetric nitrogen/carbon-coordinated single metal sites for carbon dioxide conversion.

Asymmetric nitrogen/carbon-coordinated single metal sites (M-NC) outperform symmetric M-N sites in carbon dioxide (CO) electroreduction. However, the challenge of crafting well-defined M-NC sites complicates the understanding of their structure-catalytic performance relationship. In this study, we employ metallized N-confused tetraphenylporphyrin (M-NCTPP) to investigate CO conversion on M-NC sites using both density functional theory and experimental methods.

Well-defined N C -anchored Single-Metal-Sites for Oxygen Reduction Reaction.

N-, C-, O-, S-coordinated single-metal-sites (SMSs) have garnered significant attention due to the potential for significantly enhanced catalytic capabilities resulting from charge redistribution. However, significant challenges persist in the precise design of well-defined such SMSs, and the fundamental comprehension has long been impeded in case-by-case reports using carbon materials as investigation targets. In this work, the well-defined molecular catalysts with N C -anchored SMSs, i.

Isomeric Dual-Pore Two-Dimensional Covalent Organic Frameworks.

Two-dimensional (2D) covalent organic frameworks (COFs) with hierarchical porosity have been increasingly recognized as promising materials in various fields. Besides, the 2D COFs with kagome () topology can exhibit unique optoelectronic features and have extensive applications. However, rational synthesis of the COFs with topology remains challenging because of competition with a square-lattice topology.

Double-single-atom MoCu-embedded porous carbons boost the electrocatalytic N reduction reaction.

NH is an essential ingredient of chemical, fertilizer, and energy storage products. Industrial nitrogen fixation consumes an enormous amount of energy, which is counter to the concept of carbon neutrality, hence eNRR ought to be implemented as a clean alternative. Herein, we propose a double-single-atom MoCu-embedded porous carbon material derived from uio-66 (MoCu@C) by plasma-enhanced chemical vapor deposition (PECVD) to boost eNRR capabilities, with an NH yield rate of 52.

Single-Atom Anchored Curved Carbon Surface for Efficient CO Electro-Reduction with Nearly 100% CO Selectivity and Industrially-Relevant Current Density.

Although single metal atoms on porous carbons (PCs) are widely used in electrochemical CO reduction reaction, these systems have long relied on flat graphene-based models, which are far beyond reality because of abundant curved structures in PCs; the effect of curved surfaces has long been ignored. In addition, the selectivity generally decreases under high current density, which severely limits practical application. Herein, theoretical calculations reveal that a single-Ni-atom on a curved surface can simultaneously enhance the total density of states around Fermi level and decrease the energy barrier for *COOH formation, thereby enhancing catalytic activity.

Organic-moiety-engineering on copper surface for carbon dioxide reduction.

Electrochemical conversion of carbon dioxide (CO) into value-added products powered by sustainable electricity is considered as one of the most promising strategies for carbon neutrality. Among the products, hydrocarbons, especially ethylene and ethanol are the most desired species due to their wide industrial applications. Copper-based catalysts are currently the very limited option available for catalyzing the reduction of CO to multi-carbon products.

Longitudinally Grafting of Graphene with Iron Phthalocyanine-based Porous Organic Polymer to Boost Oxygen Electroreduction.

Iron phthalocyanine-based polymers (PFePc) are attractive noble-metal-free candidates for catalyzing oxygen reduction reaction (ORR). However, the low site-exposure degree and poor electrical conductivity of bulk PFePc restricted their practical applications. Herein, laminar PFePc nanosheets covalently and longitudinally linked to graphene (3D-G-PFePc) was prepared.

Asymmetric Push-Pull Type Co(II) Porphyrin for Enhanced Electrocatalytic CO Reduction Activity.

Molecular electrocatalysts for electrochemical carbon dioxide (CO) reduction has received more attention both by scientists and engineers, owing to their well-defined structure and tunable electronic property. Metal complexes via coordination with many π-conjugated ligands exhibit the unique electrocatalytic CO reduction performance. The symmetric electronic structure of this metal complex may play an important role in the CO reduction.

Isometric Covalent Triazine Framework-Derived Porous Carbons as Metal-Free Electrocatalysts for the Oxygen Reduction Reaction.

Covalent triazine frameworks (CTFs) and their derivative N-doped carbons have attracted much attention for application in energy conversion and storage. However, previous studies have mainly focused on developing new building blocks and optimizing synthetic conditions. The use of isometric building blocks to control the porous structure and to fundamentally understand structure-property relationships have rarely been reported.

CoN Sites Constructed by Anchoring Co Porphyrins on Vinylene-Linked Covalent Organic Frameworks for Electroreduction of Carbon Dioxide.

Developing effective electrocatalysts for CO reduction (CO RR) is of critical importance for producing carbon-neutral fuels. Covalent organic frameworks (COFs) are an ideal platform for constructing catalysts toward CO RR, because of their controllable skeletons and ordered pores. However, most of these COFs are synthesized from Co-porphyrins or phthalocyanines-based monomers, and the available building units and resulting catalytic centers in COFs are still limited.

Covalent Triazine Frameworks and Porous Carbons: Perspective from an Azulene-Based Case.

Covalent triazine frameworks (CTFs) are among the most valuable frameworks owing to many fantastic properties. However, molten salt-involved preparation of CTFs at 400-600 °C causes debate on whether CTFs represent organic frameworks or carbon. Herein, new CTFs based on the 1,3-dicyanoazulene monomer (CTF-Azs) are synthesized using molten ZnCl at 400-600 °C.

Simultaneously Integrate Iron Single Atom and Nanocluster Triggered Tandem Effect for Boosting Oxygen Electroreduction.

Atomically nitrogen-coordinated iron atoms on carbon (FeNC) catalysts are emerging as attractive materials to substitute precious-metal-based catalysts for the oxygen reduction reaction (ORR). However, FeNC usually suffers from unsatisfactory performance due to the symmetrical charge distribution around the iron site. Elaborately regulating the microenvironment of the central Fe atom can substantially improve the catalytic activity of FeNC, which remains challenging.

Modulating intramolecular electron and proton transfer kinetics for promoting carbon dioxide conversion.

A novel pentagon-heptagon paired azulene group that possesses a large dipole moment is immobilized onto a porphyrin. The as-prepared azulene iron porphyrin exhibits a narrower bandgap and higher electrocatalytic CO reduction activity than the pristine iron porphyrin. The maximum CO faradaic efficiency reaches 99.

Optimizing Microenvironment of Asymmetric N,S-Coordinated Single-Atom Fe via Axial Fifth Coordination toward Efficient Oxygen Electroreduction.

Single-atom catalysts (SACs) are attractive candidates for oxygen reduction reaction (ORR). The catalytic performances of SACs are mainly determined by the surrounding microenvironment of single metal sites. Microenvironment engineering of SACs and understanding of the structure-activity relationship is critical, which remains challenging.

Topological defect-containing Fe/N co-doped mesoporous carbon nanosheets as novel electrocatalysts for the oxygen reduction reaction and Zn-air batteries.

Developing effective electrocatalysts for the oxygen reduction reaction is of great significance for clean and renewable energy technologies, such as metal-air batteries and fuel cells. Defect engineering is the central focus of this field because the overall catalytic performance crucially depends on highly active defects. For the ORR, topological defects have been proven to have a positive effect.

A Terpyridine-Fe-Based Coordination Polymer Film for On-Chip Micro-Supercapacitor with AC Line-Filtering Performance.

The preparation of redox-active, ultrathin polymer films as the electrode materials represents a major challenge for miniaturized flexible electronics. Herein, we demonstrated a liquid-liquid interfacial polymerization approach to a coordination polymer films with ultrathin thickness from tri(terpyridine)-based building block and iron atoms. The as-synthesized polymer films exhibit flexible properties, good redox-active and narrow bandgap.