Xin Ding

Coupling CO2 reduction with thermodynamically favorable anodic oxidation offers a promising route for lowering the energy demand of paired electrosynthesis. Herein, we report a bismuth-based paired electrosynthesis system (Bi NSs/CF || Bi/NF-20) for the simultaneous coproduction of high value formate at both electrodes via cathodic CO2 reduction (CO2RR) and anodic methanol oxidation (MOR). Crucially, these self-supported electrodes are rationally constructed through a spontaneous galvanic replacement strategy, offering a sustainable alternative to conventional energy intensive fabrication. Consequently, the integrated two-electrode electrolyzer operates stably at 3 V for 50 h, yielding a combined FE exceeding 185% and impressive production capacities of more than 400 g kWh–1. Combined in situ Raman spectroscopy and theoretical calculations reveal that the intrinsic electronic properties of the Bi NSs/CF facilitate the rate-determining step by lowering the *OCHO formation barrier, and elucidate the dynamic evolution of active sites during the MOR. This study offers a compelling strategy for designing integrated electrolyzers toward CO2 valorization with high atom economy.

Traditional crystalline MCOFs often sacrifice catalytic activity to achieve long-range order, limiting microenvironment tunability. Here, we used the high-performance Ru(bda)(pyCHO)₂ complex and ETTA linker to construct two amorphous materials AMCOF-X via coordination and dehydration assembly. Structural characterization and performance tests show that dehydration assembly strategy expands the framework and reduces particle size, greatly improving the accessibility of Ru active sites. In a Ru(bpy)₃²⁺ photocatalytic water oxidation system, AMCOF-2 achieves a first-order rate constant of 68.11 μmol g^–1 s^–1─an exponential enhancement over most COF-based catalysts. The flexible microenvironment and accessible metal sites in the amorphous skeleton promote a water nucleophilic attack pathway, facilitating efficient O═O bond formation. Our modular assembly enables efficient integration of molecular catalysts within metal–organic covalent frameworks, offering a novel design route for combining molecular catalysis with framework materials.

Direct photocatalytic nitrogen fixation from air under mild conditions (compared to the harsh conditions of the Haber–Bosch process) remains a fundamental challenge due to the inertness of NN bonds and the lack of controllable activation pathways.

Photothermal catalysis offers a promising route for CO₂ cycloaddition with epoxides, yet efficient charge utilization and mechanistic clarity remain challenging. Traditional thermal catalysis typically requires harsh conditions (high temperature and pressure) and suffers from low energy efficiency, while single photocatalysis is limited by rapid charge recombination and insufficient activation of inert CO₂. Herein, we develop a photothermal dual-responsive catalyst, ZnNCN/NaK-CN, by integrating photo-active NaK-doped g-C₃N₄ with zinc cyanamide (ZnNCN). This catalyst achieves a high productivity of 147.3 mmol g⁻¹ h⁻¹ under full-spectrum illumination and delivers 84.8–99.4% yields for various cyclic carbonates, surpassing most recently reported catalysts and commercial benchmarks. Notably, the apparent activation energy is reduced from 40.9 kJ mol⁻¹ (thermal-only) to 33.4 kJ mol⁻¹ under photothermal conditions. Mechanistic studies reveal that CO₂ preferentially adsorbs on the ZnNCN framework, and photogenerated electrons driven by the built-in electric field (BEF) transfer from NaK-CN to CO₂ adsorbed on ZnNCN, forming highly reactive •CO₂⁻ radicals that accelerate the ring-closing step. This work not only presents a robust catalyst for photothermal CO₂ conversion but also provides a mechanistic framework for photogenerated electron-mediated CO₂ activation in cycloaddition reactions.

Fe-doped TiO ₂ enables the photocatalytic conversion of N ₂ O to NH ₃ under light irradiation, delivering an NH ₃ production rate of 218.39 μmol h ⁻¹ g _cat ⁻¹ .

Oxygen evolution reaction (OER), a pivotal half-reaction in water splitting and renewable energy conversion, suffers from intrinsically sluggish kinetics, necessitating robust electrocatalysts to lower overpotential and enhance energy efficiency. Nickel-based substrates are particularly appealing due to their ability to form compact and stable oxide layers; however, rationally constructing high-surface-area Ni supports remains a substantial challenge. Here, we develop a synergistic electrodeposition–etching strategy to fabricate clustered NiZn alloy nanowires on Ni foils, followed by mild chemical oxidation. This treatment that induces surface oxidation, promotes Fe incorporation, and drives in situ reconstruction into a nanosheet-like NiFeZn(OH)_x catalytic layer. This integrated approach overcomes common issues associated with electrodeposited coatings on NiZn nanowire clusters, including poor hydrophilicity, weak adhesion, and uncontrollable morphology. The optimized NiFeZn(OH)_x/NiZn/Ni electrode delivers outstanding OER performance in 1 M KOH, requiring only 229 mV to reach 100 mA cm⁻², with a low Tafel slope of 31.6 mV dec⁻¹, and demonstrates exceptional durability over 180 h of continuous operation without performance degradation. The superior catalytic behavior originates from the synergistic interplay between the high-surface-area NiZn nanowire scaffold and the dynamically reconstructed NiFeZn(OH)_x active phase. This work provides a generalizable strategy for engineering efficient and durable OER electrodes, offering new design principles for Ni-based alloy supports in advanced electrocatalysis.

To elucidate the “reversed proton relay” mechanism in neutral water oxidation , we designed two Ru( ii ) complexes: Ru1 with pendant carboxylate, and Ru1′ without it.

Electrocatalytic nitrogen oxidation emerges as a promising approach for the eco-friendly synthesis of nitrate, achieving remarkable progress in recent years. However, the precise oxidation mechanism remains poorly understood due to the complex interactions among the catalyst, electrolyte, and various intermediates, making it difficult to fully unravel the reaction pathways. Herein, we employed a Fe-TiO₂ catalyst in electrolytes enriched with SO₄^2-/HSO₅^-, significantly enhancing the nitrogen oxidation process through the in situ generation of *SO₅H. Remarkably, an astounding 404-fold improvement over HClO₄ in a saturated potassium monopersulfate (PMS) system under a constant current density of 0.40 mA/cm² was achieved. Furthermore, an H₂SO₄-mediated electrochemical oxidation mechanism, characterized by the high efficacy and stability of *SO₅H, was proposed and validated through the identification of key intermediates, comprehensive operational experiments, and in situ detection of the catalyst's active sites.