Rapid thermal ramping and cooling processes enable the formation of monodisperse nanomaterials. Specifically, the thermal plasma spark technique, characterized by high energy density and ultrafast heating and cooling rates, represents a highly effective strategy for nanomaterial synthesis. Herein, we employ this approach to synthesize Ni nanoparticles embedded within a monolithic porous carbon film. With peak temperatures reaching ∼2400 K within 3 ms, the resulting Ni nanoparticles exhibit an average diameter of 6 nm. As a proof of concept, the as-synthesized samples serve as cathodes in Li-CO2 batteries. The uniform Ni nanoparticles promote the reversible reaction between Li2CO3 and CO2, thereby enhancing catalytic performance. Density functional theory (DFT) calculations reveal that the monolithic porous carbon film facilitates CO2 adsorption and Li2CO3 formation on the Ni(111) surface, consistent with the experimental results. This work offers a general strategy for synthesizing highly active nanomaterials supported on monolithic porous carbon via the high-temperature thermal plasma spark method.

Abstract Seawater electrolysis is promising for green hydrogen production but suffers from chloride-induced anodic corrosion. Herein, a dual-anion synergistic protection strategy is proposed for durable alkaline seawater oxidation over V2O5 nanolayer coated NiFe layered double hydroxide nanosheets on Ni foam (V2O5@NiFe LDH/NF). During seawater oxidation process, the surface V2O5 component is reconstructed into adsorbed VO43– species as an anion-enriched protective interface capable of electrostatically repelling Cl– and mitigating chloride attack. In parallel, the interlayer CO32– confined within NiFe LDH acts as an internal anionic barrier, suppressing Cl– penetration into the LDH galleries and inhibiting its adsorption on catalytically active sites. The cooperative action of external VO43– protection and internal CO32– shielding endows V2O5@NiFe LDH/NF with robust catalytic activity and exceptional durability, delivering an overpotential of 370 mV at 1000 mA cm–2 and maintaining stable operation for 1000 h under industrial-level current density. Furthermore, an anion-exchange membrane electrolyzer assembled with V2O5@NiFe LDH/NF as the anode and Pt/C/NF as the cathode requires only 2.02 V to achieve 500 mA cm–2 and operates continuously for 1000 h. This study provides a rational dual-anion interfacial engineering strategy for developing durable electrodes under harsh chloride-containing environments.

As a representative of Generation IV advanced nuclear energy systems, the Lead-cooled Fast Reactor (LFR) has attracted considerable attention owing to its inherent safety features. The lead-bismuth eutectic (LBE), as one of the potential optional coolants for LFR, has good thermal performance and stable chemical properties. However, the potential corrosion of structural steels remains a major challenge to long-term operational safety, closely associated with the dissolved oxygen concentration in the coolant. To address this issue, this paper proposes an intelligent early cognition and classification approach for potential corrosion, termed the Interactive Dual-stream Separation Transformer (IDST) with soft labeling. The proposed method is specifically designed to recognize and classify transient processes of oxygen concentration in the LBE, represented by electromotive force (EMF) measurements, with temperature serving as an auxiliary parameter. The classification encompasses saturated and unsaturated states as well as oxygen sensor anomalies. Approximate coefficient mean features of EMF and temperature time series are extracted using a sliding window and wavelet transform, and subsequently converted into soft labels to capture the inherent ambiguity of transition phases. Experimental data were obtained from a self-developed LBE testing facility. Extensive validation experiments, including model comparisons and ablation studies, were conducted to evaluate the effectiveness of the proposed gating and cross-attention mechanisms. The results demonstrate that the IDST model achieves an overall classification accuracy of 97.91%, with 100% accuracy in detecting sensor anomalies. This approach provides an efficient and reliable framework for the cognition and classification of oxygen concentration transients, contributing to the intelligent monitoring and maintenance of advanced nuclear energy systems.

Developing a simple and efficient method for synthesizing single-atom catalysts is of great significance in promoting the advancement of this field. Here, a one-pot synthesis strategy was successfully employed to fabricate an iridium single-atom catalyst supported on ordered mesoporous carbon-based material. During the preparation process, carbon and nitrogen elements spontaneously anchored iridium species from the initial mixing of reactants, ultimately forming atomically dispersed active sites. The as-prepared catalyst exhibits ordered mesoporous architecture, which not only facilitates rapid reactant contact and mass transfer of reactants, but also stabilizes active centers through spatial confinement effects. The catalyst demonstrates superior catalytic performance and stability in lower alkane dehydrogenation reactions, achieving an isobutane conversion of 35.3% with 98.7% selectivity for iso-butene at 450 degrees C (substantially lower than the operating temperature required by conventional Pt-based catalysts). This method provides a novel approach for large-scale preparation of single-atom catalysts and has important application prospects, which are expected to play a significant role in the field of energy catalysis.

Plasmon-enhanced photocatalysis revolutionizes solar energy conversion but faces material limitations. While Au dominates for its superior plasmonics, its high cost and poor catalytic activity hinder practical deployment. High-D-band Ni emerges as a promising alternative with intrinsic catalytic activity, broadband plasmonic response, and high work function, but suffers from strong D-electron correlations that compromise plasmonic efficiency and hot electron mobility. Moreover, while nanocavity integration can enhance optical confinement, it aggravates hot-electron localization, creating a fundamental dilemma for practical implementation. Herein, we present a Nimediated plasmonic cascade (Pt-TiO2-Ni/SiO2/Al) that tackles the hot-electron spatial localization challenge in traditional plasmonic nanocavities, significantly enhancing photocatalytic hydrogen evolution from glucose wastewater (47.68 mmol g-1 h-1). The Ni/SiO2/Al Fabry-Perot cavity provides strong optical confinement, while the upper Pt-TiO2-Ni structure enables robust D-band-matched Pt-Ni coupling, facilitating spatial extension of the resonant electromagnetic field toward the Pt-TiO2 and enabling directional hot-electron injection from Ni to Pt-TiO2 (verified by in-situ X-ray photoelectron spectroscopy). This yields a 6.4-times enhancement in visible-near-infrared light hydrogen evolution, outperforming conventional TiO2-Ni/SiO2/Al cavities in hot-electron utilization efficiency. This cascaded design harmonizes light-harvesting (68.3 % efficiency) with hot electron extraction exhibiting 3.7-times and 5.4-times hydrogen generation rates improvements over TiO2-Ni/SiO2/Al and Pt-TiO2, respectively, alongside extended carrier lifetime. This work presents a universal strategy to overcome the persistent trade-off between plasmonic light confinement and charge extraction in photocatalysis, ingeniously converting Ni's inherent limitations into design merits to enable practical solar-driven waste-to-energy conversion.

ABSTRACT Herein, we discover a robust emission control catalyst featuring Ru single‐atom sites even undergoing thermal oxidative aging at 850°C in a 10%H 2 O/10%O 2 /N 2 mixture gas stream, expecting to substitute the traditional Rh catalysts by cutting ∼73% of the total cost. The stability challenges in elevated‐temperature oxidizing environments were overcome via constructing the isolated Ru atoms anchored by square‐planar coordination with four lattice oxygen in ceria and suppressing Ru atom migration toward the single Ru─O x ─Ce catalytic centers by introducing the Zr‐rich materials, which are conducive to inhibiting the formation of undesirable N 2 O by‐products during catalytic NO reduction. More importantly, the challenge of low‐temperature C─H bond activation in short‐chain alkanes on the isolated single‐atom sites was broken through by constructing the CeZrO–Ru SA –CeO 2 three‐phase interfaces to promote the H‐spillover. The low‐cost Ru SA –CeO 2 /CZ single‐atom catalyst exhibited much better stability, lower selectivity of N 2 O and NH 3 by‐products, and higher activity for CO conversion under oxygen‐lean conditions compared to commercial Rh catalysts for automotive emission control applications. This work opens new avenues for developing the new generation of low‐cost, robust emission control catalysts in the future.

In the reductive amination of furfural (FF), controlling the hydrogenation performance of the catalyst is crucial for achieving high selectivity for primary amines. In this work, Ru/CeMOF materials with highly dispersed Ru nanoparticles (NPs) were synthesized using CeMOF nanoislands supports. Characterization revealed that the N/S groups on isolated CeMOF nanoislands stabilize the Ru species. When Ru/CeMOF was used in the reductive amination of FF to furfurylamine (FUA), the selectivity of Ru1/CeMOF reached 93.8 %, which was 13 times that of Ru0.5/CeMOF and 4.6 times that of Ru3/CeMOF. A series of characterizations and DFT calculations demonstrated that the interactions between the metal and CeMOF support were optimized by modulating the Ru loading amount, achieving highly dispersed Ru species and an appropriate Ru0/Ru3+ ratio, which lead to suitable hydrogenation activity and acidity, thereby promoting the highly selective synthesis of FF to FUA. Among them, Ru0 served as the H2 activation site, possessing suitable electron density and relative content, thereby endowing it with appropriate hydrogenation capacity. Meanwhile, the enhanced Lewis acid (Ru3+) facilitated the C--N bond activation of the imine intermediate. The paper also proposed the reaction mechanism of the reductive amination from FF to FUA. Finally, interactions of metal-support ensured the high stability of the Ru/CeMOF catalyst during the recycling process. This work provides valuable guidance for the rational design of MOF-based catalysts used in efficient reductive amination reactions.

Hydrogen energy is regarded as an ideal energy carrier due to its advantages such as high energy density, environmental friendliness, and wide availability. The storage and release of hydrogen using liquid organic hydrogen carriers (LOHCs) such as N-ethylcarbazole (NECZ) offer distinct advantages for safe hydrogen transport and storage. Developing efficient catalysts for this reversible process remains a critical challenge. At present, the high cost of noble metal catalysts hinders their widespread application, and most of the non-noble metal catalysts are not efficient in reversible hydrogenation storage of NECZ. In this study, a silica supported non-noble Ni was prepared by the wet-kneading method, which successfully achieved the reversible hydrogen storage of NECZ. The catalyst exhibited high activity and moderate stability, achieving hydrogen storage of 5.77 wt% within 6 h under 6 MPa of H2 at 150 degrees C, and hydrogen release of 5.77 wt% within 1.5 h at 200 degrees C during 5 cycles. XPS studies identified Ni0 as the main active site for hydrogenation-dehydrogenation cycles. IR and kinetic studies further revealed that the same Ni0 sites are poisoned by the intermediate 4H-NECZ. This work might pave the way for designing high-performance non-noble catalysts for reversible chemical hydrogen storage.

Developing seawater-oxidation anodes that combine high activity with long-term durability requires reconciling efficient oxygen evolution with resistance to chloride-induced degradation. Here we report a Ni-Fe sulfate hydrate pre-catalyst, Fe-NiSO4·6H2O (FNS), grown on nickel foam within 5min at 25 °C by propylene-oxide-assisted heterogeneous nucleation. Under alkaline oxygen evolution conditions, FNS rapidly reconstructs into a sulfate-modified (Fe)NiOOH phase. In-situ Raman spectroscopy and synchrotron X-ray analyses show that retained sulfate accelerates reconstruction and suppresses chloride-driven degradation. Operando 18O-labelled differential electrochemical mass spectrometry and ATR-SEIRAS reveal coupled adsorbate-evolution and lattice-oxygen pathways on reconstructed (Fe)NiOOH@SO4. Density functional theory indicates that sulfate raises the O 2p band centre towards the Fermi level to promote lattice-oxygen activation, whereas Fe optimizes the adsorption energetics of oxygen-evolution intermediates. In alkaline natural seawater, the catalyst delivers overpotentials of 246 and 285mV at 500 and 1000mAcm-2, respectively, and remains stable for 1754h. In an anion-exchange-membrane flow cell, it sustains 1100mAcm-2 for 310h. Our results establish Fe-sulfate modulation as a route to self-reconstructing, corrosion-resistant anodes for industrial seawater electrolysis.

ABSTRACT Water oxidation is vital for renewable energy conversion but remains kinetically complex due to the strong coupling of electron transfer with proton‐involved chemical processes of bond formation and rupture, which are not fully captured by phenomenological Tafel analyses. Here, we design CeO 2 nanorod‐supported iridium atomic arrays (Ir/CeO 2 ) as model catalyst to elucidate the molecular‐scale information about the kinetics mechanism. We reveal that the applied bias does not directly act on the reaction coordinate but regulates electrocatalytically generated current through oxidative charge accumulation. This build‐up of oxidized states significantly reduces the activation energy for *OOH formation by facilitating the O─O coupling step. Meanwhile, the electron‐buffering capacity of CeO 2 support prevents Ir over‐oxidation and dissolution during charge accumulation, thereby enhancing catalyst stability. As a result, the Ir/CeO 2 catalyst delivers superior activity and durability in proton exchange membrane water electrolyzers, achieving industrial‐level current densities at low cell voltages. These findings provide molecular insights into charge‐controlled water oxidation kinetics and highlight the essential role of purely chemical steps in describing the kinetics of multi‐electron reactions.

This study evaluated the strategy of employing metals with moderate *OOH adsorption strength (copper) coordinated by high-electronegativity ligands (oxygen) to tune the *OOH binding for selective H2O2 electrosynthesis. A uniform four-coordinated Cu-O-4 single-atom catalyst (Cu-SAO) was synthesized via ligand-assisted pyrolysis. Density functional theory calculations indicated that because of the synergy of weak-oxophilicity metal and strong-electronegativity ligands, the Cu-O-4 motif exhibits optimally attenuated *OOH binding and inhibits O-O bond scission. The Cu-SAO catalyst showed an ORR onset potential of 0.72 V and a H2O2 selectivity of 96.2% in rotating ring-disk electrode tests. In addition, it achieved >90% Faradaic efficiency over 50-500 mA cm(-2) and maintained stable H2O2 production for 430 h during flow-cell tests, yielding a high H2O2 yield of up to 47.23 mol g(-1) h(-1). This work establishes a facile first-shell coordination strategy to simplify the design of efficient 2e(-) ORR catalysts and advances practical H2O2 electrosynthesis.

For successful implementation in large-scale lead-bismuth eutectic (LBE) systems, it is imperative to enhance the oxygen transfer rate of electrochemical oxygen pump (EOP). This research delves into the effect of temperature on oxygen transport within EOP. Temperature plays a pivotal role by affecting the ionic conductivity of yttria partially stabilized zirconia (YPSZ), a solid electrolyte, and the rate at which oxygen diffuses in LBE. However, the oxidation of metal wires can lead to increased resistance, thereby affecting the current within the EOP. Consequently, selecting wire materials with high resistance to corrosion at elevated temperatures is essential. The change of oxygen concentration in LBE is not only affected by the pump oxygen rate, but also by the oxygen concentration difference caused by the corrosion of molybdenum. The experimental results indicate that the oxygen transfer rate in LBE can be significantly improved by carefully adjusting these external conditions.

The electrochemical reduction of CO2 to methanol (CH3OH) offers a highly promising avenue for zero-emission carbon recycling and renewable energy storage. However, achieving high CH3OH selectivity and long-term stability in catalysts remains rare, presenting central challenges on the path to their commercialization. It is emerging to make multiscale design of metal centers of active sites and their surrounding environments under the crucial mechanism of pathway selection. Herein, the gridized nanomolecular and nanopolymer catalysts are reported for high effective electroreduction of CO2 to CH3OH. An A-type nanogrid (AG) and its organic nanopolymers with atomically dispersed iron (Fe) are well identified with the unique catalytic active sites of Fe-N1C3Cl1. Notably, Fe-based AG nanopolymer (FePAG) catalyst exhibits a CH3OH Faradaic efficiency of 60.5%, a CH3OH selectivity of 98.3%, and a stability of up to 100 h, outperforming currently reported molecular catalysts. The superior selectivity is probably attributed to the cooperation between the stronger *CO adsorption and the super-hindrance that suppresses aggregates to guarantee the dispersion of single active sites. This study provides new insights in the exploration of nanomolecular and nanopolymer catalysis.

H2O2, a vital industrial material, poses a huge explosion risk due to its residual presence. Under acidic conditions, its stable peroxy-bond hinders efficient decomposition into H+ or HO2-. In this study, we prepared a Fe-N-C single-atom catalyst via molecular self-assembly and argon pyrolysis, regulating reactive oxygen species to convert H(2)O(2 )into O-2. In situ FTIR confirmed atomically dispersed iron significantly enhanced the end-adsorption of H(2)O(2 )and in situ formed Fe-OOH, achieving a 100% decomposition rate and 98% O-2 selectivity, while minimizing the formation of harmful center dot OH radicals. Furthermore, we constructed a flow-through amplification reactor that maintained a conversion rate of 100% even at a high space velocity of 75 h(-1). This work provides a novel approach for H(2)O(2 )decomposition reaction and offers a valuable reference in further developing systems for the decomposition of H(2)O(2 )into O-2.

The integrated CO2 capture and conversion (ICCC) has emerged as a promising and cost-effective pathway for achieving carbon neutrality. However, limited energy-efficient pathways and durable materials for ICCC systems remains challenging. This study proposes a novel approach that synergistically integrates CO2 capture and conversion through a unified chemical framework. The method employs Li-based sorbents for CO2 capture, coupled with CH4-driven sorbent regeneration that is seamlessly integrated with chemical looping dry reforming of methane (CLDRM), enabling in-situ CO2 conversion. By coupling sorbent regeneration with CLDRM, this system enhances decarbonation kinetics through Le Chatelier's principle via continuous CO2 conversion. One-step calcination synthesized Li-based sorbents particles exhibit stable CO2 capture capacity of 5.25 mmolg(-1) within 15 min per cycle, maintaining 7.5-15 % operational efficiency over 40 cycles at 600 degrees C. In CLDRM, hydrogen radicals from CH4 dissociation promote the conversion of CO2 to intermediates, lowering the apparent activation energy of sorbents regeneration by 29.2 %. Through systematic optimization in a fixed-bed reactor, we achieved 90 % CO2 uptake and 85 % CH4 conversion, with syngas production rate reaching 13.71 mLmin(-1)g(-1). Notably, the H-2/CO molar ratio in syngas stabilizes similar to 1.6, aligns with iron-based Fischer-Tropsch and methanol synthesis to produce valuable fuels. This integrated system maintains >80 % syngas purity with <10 % performance decay over 10 consecutive cycles, demonstrating exceptional robustness for industrial-scale implementation. Our integrated approach provides an energy-efficient and durable pathway to convert dilute CO2 streams into value-added chemicals, offering valuable insights for advancing carbon capture and conversion technologies.

Cu-based catalysts are crucial for the dehydrogenation of ethanol (EtOH) to acetaldehyde (AcH); however, their performance decreases at higher temperatures due to the low Tammann temperature of Cu species. In this study, we synthesized silica-supported Cu catalysts using microwave-assisted wet-kneading. Characterizations revealed a typical core-shell structure (Cu@SiO2-WK), which demonstrated high activity, excellent selectivity, and superior stability for ethanol dehydrogenation. The Cu@SiO2-WK achieved 96.2 % EtOH conversion with 99.9 % selectivity to AcH at 260 degrees C. After 160 h of reaction, it maintained an EtOH conversion of 90.5 % and AcH selectivity of similar to 99.9 %. Following simple calcination, the catalyst's activity was fully regenerated to 96.1 %. Model catalysts and in situ FT-IR spectra indicate that the core-shell structure significantly enhances the catalyst's performance in the dehydrogenation of EtOH to AcH.

The atom arrangement in carbon electrocatalysts is crucial for enhancing the intrinsic activity toward oxygen reduction reactions (ORRs), a key process in multiple renewable energy systems. However, the challenge of designing electrocatalysts with improved performance by manipulating atomic arrangement has been limited by synthetic constraints and a lack of understanding of the catalytic phase formation. Herein, we gain atomic-level insight into the origin of a highly active site by creating a model catalyst with a heteroatom-decorated carbon matrix of a specific configuration. The introduction of fluorine (F) during the synthesis of the nitrogen (N)-decorated carbon matrix induces structural rearrangement, converting most pyrrolic-N (Pr-N) into highly stable graphitic-N (G-N), thereby achieving a N configuration predominantly composed of pyridinic nitrogen (Py-N) and G-N. The multidopant synergistic effect of F, Py-N, and G-N causes a destabilized π-conjugated electron network of the carbon matrix, resulting in a more localized electronic structure. As a result, multiple dopant configurations with high ORR activity have been explored, among which the asymmetric Py-N and G-N configurations feature the lowest theoretical ORR overpotential, ultimately enabling the optimized F@NC catalyst to exhibit excellent oxygen reduction activity. This work establishes a foundation for the rational design of metal-free carbon-based electrocatalysts toward ORR.