Fu Yang

A practical, efficient, and scalable procedure has been established for the general synthesis of 1,4-amino alcohols from anilines and dienes in a single operation. This method constitutes a valuable alternative to most existing processes based on nitrosobenzene. The ready availability of starting materials and the use of a readily accessible W(VI) precatalyst collectively render this approach attractive for library construction of 1,4-amino alcohol compounds. The results highlight a beneficial steric effect at the tungsten center, with bulkier groups correlating with improved catalytic performance.

The electrochemical reconstruction of the Cu(OH) _2, combined with highly redox-active Ce and Mo, enabled NO ₃ RR with near-unity *H utilization, delivering a yield of 26.5 mg h ⁻¹ mg _cat ⁻¹ and FE of 95.1%.

Photocatalytic nitrate reduction to ammonia (PcNRA) offers a sustainable route for nitrate remediation and green NH3 synthesis under mild conditions. BiOI has attracted attention due to its narrow band gap, strong visible-light absorption, layered structure, and suitable electronic structure for reduction reactions. However, rapid charge recombination limits its photocatalytic performance. Herein, a molecular dipole-induced interfacial regulation strategy was developed to construct an organic–inorganic hybrid photocatalyst (TP/BiOI) with polarization-related interfacial characteristics. The iron tetraphenylporphyrin (FeTPP) modified TP/BiOI interface promoted interfacial charge redistribution and directional carrier migration and optimized the surface potential to promote NO3– enrichment. In addition, FeTPP modified the interfacial wettability and enhanced the irradiation-induced thermal response of TP/BiOI, which may provide an additional favorable local microenvironment for interfacial reactions. These effects, together with improved charge utilization, contribute to enhanced *H-mediated nitrate hydrogenation. As a result, TP/BiOI achieved an NH3 production rate of 5718.9 μmol·g–1·h–1, 73.8% higher than that of pristine BiOI (3290.4 μmol·g–1·h–1), outperforming most reported state-of-the-art catalysts. This work demonstrates that molecular dipole-induced interfacial polarization can effectively regulate charge distribution and the interfacial microenvironment, providing a new strategy for designing efficient organic–inorganic hybrid photocatalysts for solar-driven nitrate-to-ammonia conversion.

Electrochemical nitrate reduction to ammonia (eNO3–RR) offers a sustainable route for nitrogen recovery and wastewater remediation, yet its efficiency at high reaction potentials is severely constrained by sluggish proton coupling of *NOx intermediates and the competitive hydrogen evolution reaction (HER). Herein, we report a local built-in-electric field (LBIEF)-modulated FeNi/NiFe2O4 heterojunction that overcomes these kinetic bottlenecks through interfacial electronic polarization and spatially coordinated dual-site catalysis. The optimized LBIEF induces spontaneous charge redistribution, generating electron-deficient Fe(II) sites that strengthen nitrate and *NOx adsorption and electron-rich Ni0 sites that promote efficient *H formation and transfer. This synergistic charge bifurcation significantly lowers the energy barrier of the rate-determining *NO to *NOH hydrogenation step, enabling near-unity hydrogen utilization (97.9%) and suppressing parasitic hydrogen evolution. As a result, the FeNi/NiFe2O4 catalyst achieves an exceptional NH3 yield of 91.2 ± 2.8 mg h–1 mgcat–1 with a Faradaic efficiency (FE) of 94.5 ± 1.6% at −1.4 V vs. RHE, alongside 96.3% nitrate removal and 98.8% NH3 selectivity, while maintaining stability over 200 h of continuous operation. Operando spectroscopy and density functional theory reveal that LBIEF-mediated electronic polarization governs intermediate adsorption, hydrogen transfer, and reaction pathway selectivity. This work establishes LBIEF engineering as a general strategy to synchronize nitrate activation and hydrogenation, offering a mechanistic blueprint for next-generation electrocatalysts for sustainable nitrogen valorization.

Proton Exchange Membrane Water Electrolysis (PEMWE) device with merits of high energy efficiency, rapid response, and operational flexibility represents one of the most promising technologies for green hydrogen production. However, the overall hydrogen production efficiency in PEMWEs is frequently constrained by kinetic limitations of the anodic oxygen evolution reaction (OER), due to intricate multi‐step proton‐electron transfer processes. RuO ₂ ‐based catalysts remain limited stability, primarily due to intrinsic Ru site overoxidation and lattice oxygen loss during operation, which motivates intensive study into their understanding and mitigating these inactivation mechanisms. Different from traditional surface scale optimization, recent advances in RuO ₂ catalyst have focused on mechanism‐driven atomic‐level engineering modification of both Ru sites and coordination environment to simultaneously enhance catalytic activity and stability. However, a comprehensive understanding that bridges the mechanistic complexity of OER with targeted atomic‐scale intervention remains elusive, in response, this review provides a comprehensive overview of recent advances in RuO ₂ ‐based nanocatalysts, with an emphasis on OER mechanisms, advanced in‐situ/operando characterizations in PEMWE, and mechanism‐based strategies for regulating stability at the atomic scale. Ultimately, this review concludes by delineating the primary challenges and outlining promising future research directions essential for advancing the practical application of RuO ₂ catalysts in PEMWEs.

Precise control over interfacial charge-transfer pathways is pivotal for the rational design of high-efficiency heterojunction photocatalysts yet remains a formidable challenge, primarily owing to the scarcity of atomic-level modulation strategies. Here, we demonstrate that the pendant amino groups (-NH₂) of the metal-organic framework UiO-66-NH₂ spontaneously form dative coordination bonds (N-bridges) with surface Pb atoms of CsPbBr₃ perovskite, thereby engendering a well-defined heterojunction interface. By combining X-ray photoelectron spectroscopy binding-energy shift analysis with density functional theory (DFT) calculations, we reveal that this interfacial N-bridge fulfills a dual function: it templates the preferential exposure of the catalytically active (040) facet of CsPbBr₃ and concurrently serves as a directional conduit for interfacial electron transfer. DFT calculations further predict a ground-state charge redistribution of approximately 0.80 e^- from the metal-organic framework (MOF) to the perovskite. Critically, this atomic-scale bridge preferentially channels the charge flow into a direct Z-scheme pathway, a mechanism strongly corroborated by the transition of the dominant reactive species from superoxide radicals (·O₂^-) in pristine CsPbBr₃ to hydroxyl radicals (·OH) in the heterojunction. This N bridge-mediated Z scheme configuration affords exceptional spatial charge separation while preserving robust redox potentials, yielding a net photocurrent response approximately 3.5-4.0-fold and 2.8-3.3-fold higher than those of pristine CsPbBr₃ and UiO-66-NH₂, respectively, under identical measurement conditions. The functional efficacy of this interface design is substantiated by photoelectrochemical measurements and the efficient degradation of model organic pollutants─tetracycline and ciprofloxacin, employed as mechanistic probes─with the composite retaining high activity upon immobilization on porous substrates in real water matrices. This work establishes interfacial N-bridging as a generalizable atomic-scale design paradigm for governing charge-transfer kinetics in heterojunction systems, thereby transcending empirical optimization toward the rational engineering of interfaces.

Addressing the dual challenges of organic wastewater purification and freshwater regeneration requires innovative materials capable of multifunctional integration. This study presents a tactical design of metallic Cu-interfaced FeO composites (Fe/Cu-x) synthesized via a synergistic self-assembly and pyrolysis strategy. The interfacial Cu/FeO pairs, featuring electron-deficient Cu(II) and Fe(II) pairs along with promoted oxygen vacancies, afford abundant redox cycles to enable exceptional electron transfer and peroxymonosulfate (PMS) activation. The optimized Fe/Cu-800 catalyst achieved an excellent tetracycline (TC) degradation efficiency (k_obs = 0.235 min⁻¹) within 20 min, far outperforming the other controls including the Cu-free one and different temperature-derived, retained robust performance across wide pH ranges and in real water matrices, and exhibited rational recyclability. The dominant ·OH alongside other free radicals synergistically contribute to the TC degradation. Beyond catalysis, this study demonstrates the customizable integration of the powder catalyst into a monolithic form evaporator through a Ca²⁺-triggered hydrogel crosslinking strategy. This uniquely integrated system simultaneously accomplishes pollutant degradation and solar-driven clean water production. Under 1 sun irradiation, the evaporator achieved a TC degradation rate of 94.4% within 20 minutes and simultaneously realized a high-water evaporation rate of 1.313 kg m⁻² h⁻¹, demonstrating a significant dual-functional synergy effect. This research breaks the conventional single-function limitation by offering a novel “degrade-and-evaporate” platform, which emerges from precise interfacial engineering and modular device integration. It provides a sustainable and efficient technical pathway for integrated wastewater treatment and water resource regeneration.

Electrocatalytic nitrate reduction reaction (NITRR) is promising but severely limited by sluggish reaction kinetics and inefficient proton coupling. Herein, we report a lattice‐confinement strategy triggering ruthenium doping embedded in Fe ₃ O ₄ nanocrystals anchored on porous N‐doped carbon nanofibers, creating self‐adaptive electron‐deficient Fe(II)‐oxygen vacancy‐Ru (Fe(II)‐Ov‐Ru) atomic interfaces, which simultaneously enhances water dissociation for active hydrogen ( ^* H) supply. This atomic‐scale division of labor enables efficient nitrate adsorption and activation at Fe(II)‐Ov sites, coupled with accelerated proton delivery from neighboring Ru centers, thereby overcoming kinetic bottlenecks and suppressing nitrite accumulation and hydrogen evolution. As a result, the optimized catalyst achieves an outstanding ammonia yield of 49.2 mg h ^{− 1} mg _cat ^{− 1} and a Faradaic efficiency of 92.8% at −1.4 V vs. RHE in neutral electrolyte, with excellent cycling stability (>20 cycles) and high selectivity (FE > 80%) across a wide pH range (1–14), outperforming most state‐of‐the‐art NITRR catalysts. Operando spectroscopy, ^* H monitoring, and density functional theory calculations identify ^* NO ₂ reduction as the rate‐determining step and reveal its substantial energy barrier lowering via Ru‐induced electronic modulation. Furthermore, the catalyst delivers stable operation for over 50 h at an industrial‐grade current density of 400 mA cm ^{− 2} in a flow‐cell electrolyzer. By integrating urea oxidation at the anode and recovering ammonia as high‐purity struvite fertilizer, this work establishes a scalable and energy‐efficient platform for sustainable nitrate valorization.

Single-atom catalysts (SACs) have demonstrated immense potential in the fields of energy and biochemical conversions. Their unique properties make them particularly efficient and selective. Characterized by their unique isolated state on supports, SACs often showcase poor synergy in the multiple molecule conversion because of the infrequent communications with others. Recently, some interesting synergetic processes of SACs in some special reactions have been found; however, to our best knowledge, the synergetic catalytic effect of SACs has not been systematically summarized. This article comprehensively overviews the basic concepts, mainstream synthetic methods, and modification strategies of SACs and emphasizes the synergetic catalysis effect in biomass conversion, CO2 reduction, and cascade reaction by itself or other media. To maximize the advantage of SACs, various synthetic methods for them, including impregnation, co-impregnation, co-precipitation, atomic layer deposition, electrochemical methods, photochemical methods, pyrolysis synthesis, spray pyrolysis method, ball-milling and chemical vapor deposition method are discussed. This review provides a comprehensive discussion concerning the dynamic interplay between precisely engineered atomic architectures and their synergistic functionalities in modulating catalytic efficacy, with focused exploration of activity enhancement strategies and operational stability optimization. Distinctively, it pioneers the establishment of comprehensive theoretical frameworks that unify SAC-driven synergistic catalytic mechanisms across three critical domains: biomass valorization, electrochemical CO2 conversion, and multi-step cascade processes. Through systematic synthesis of cutting-edge developments in coordination microenvironment modulation, inter-site electronic communication, and fundamental mechanistic studies, this work affords some interesting insight into rational design of synergistic SAC systems, thereby addressing current challenges in translating atomic-scale precision to heterogeneous catalytic performance.