Electrocatalytic nitrate reduction reaction (NO3-RR) powered by renewable energy sources offers a promising approach to achieve ammonia (NH3) synthesis with zero-carbon emission. However, sluggish proton-coupled electron transfer and byproduct formation challenge efficient NH3 synthesis. Here, we construct an integrated cascade catalytic system to elucidate the governing principles of active hydrogen (*H) generation and utilization during NO3-RR. A representative catalyst, composed of atomically dispersed Fe sites anchored on an N-doped carbon matrix and encapsulated Ru nanoparticles, exhibits an NH3 yield up to 2336.43 μgNH3 h-1 mgcat-1 while maintaining a Faradaic efficiency of 96.03% at a low potential of 0 V vs RHE. In addition, operando SR-FTIR spectroscopy and DFT calculations reveal that electron transfer from Fe atom to Ru particle not only enhances the affinity of Fe sites for NOx- species but also enriches H coverage on Ru sites, thereby accelerating hydrogenation steps and sustaining a steady *H generation-consumption cycle. This work reveals the mechanistic origin of active hydrogen in tandem catalytic structures and provides fundamental insights for advancing highly selective, energy efficient, and durable NH3 electrosynthesis and wastewater treatment.

ABSTRACT Industrial countries are moving toward digitizing the manufacturing processes in their factories by integrating the expected next‐generation technologies such as software‐defined networking (SDN), cloud computing, and industrial Internet‐of‐Things (IIoT). However, developing smart factories that combine these physical and cyber components faces critical challenges, particularly regarding the efficiency and security domains. For example, Distributed Denial of Service (DDoS) attacks in industrial environments could impact the progress of the automated processes and the availability of SDN‐based networks. In this paper, we present a novel collaborative intrusion detection system (CIDS) approach for SDN‐based industrial environments that integrates edge computing techniques to enhance security and operational efficiency. Our model optimizes resource utilization across dispersed industrial sites by uniquely combining three different IDSs: centralized‐based IDS, edge‐based Anomaly IDS (AIDS), and signature‐based IDS (SIDS). The proposed approach establishes consistent, network‐wide security policies to accommodate the varying processing capabilities. Moreover, the use of edge computing techniques minimizes the overhead introduced by the SDN controller located in the cloud layer and addresses scalability challenges in large‐scale networks with heavy traffic loads. Evaluation is performed using the Mininet emulator, and the results reveal a detection accuracy of up to 98%. Furthermore, profiling outcomes of the centralized controller indicate a 50% reduction in traffic monitoring function calls, highlighting the efficiency and superiority of the proposed methodology, particularly for geographically dispersed industrial sites.

Ag single-atom catalysts (SACs) are promising for electrochemical CO2 reduction reaction (e-CO2RR) due to their high atom utilization and CO selectivity, yet they often suffer from agglomeration and instability. Here, we employ hydrogen-substituted graphdiyne (HGDY) as a robust support, where abundant alkyne groups strongly coordinate and stabilize atomically dispersed Ag sites. By systematically tuning Ag loading (0.3-10 wt.%), we achieve precise control over active sites and product distribution. The optimized Ag3.7-HGDY catalyst achieves a remarkable CO Faradaic efficiency (FECO) of 98.1% with a turnover frequency (TOF) of 26.5 s-1, maintaining a FECO of ≥97% across a wide potential window (-0.7 to -1.2 V vs RHE). Moreover, Ag loading enables dynamic modulation of CO/H2 ratios in syngas, highlighting the tunability of the system. This work demonstrates an effective strategy for anchoring noble metals via alkyne coordination, offering a generalizable pathway toward the rational design of stable and scalable single-atom catalysts for CO2 conversion.

Herein, two Cu-based model electrocatalysts, Cu nanosheets modified with Cd single atoms (Cd-SACs@Cu NS) and unmodified Cu nanosheets (Cu NS), were rationally designed to investigate the C-C coupling to C2+ alcohols mechanisms in CORR. Compared to Cu NS, Cd-SACs@Cu NS exhibits a significantly enhanced Faradaic efficiency (FE) for C2+ alcohols of nearly 70% at an unprecedented current density of 1100mA cm-2 and maintains a higher FE (>50%) over a broad range of current densities (100-2100mA cm-2) under alkaline conditions in a flow cell. In situ characterizations and theoretical studies reveal that the enhanced selectivity toward C2+ alcohols on Cd-SACs@Cu NS is attributed to the improved H2O dissociation at atomically dispersed Cd sites and enhanced CO adsorption on the paired Cu atoms adjacent to single Cd atoms. These effects synergistically facilitate the spillover of hydrogen atoms from Cd to Cu sites, thereby promoting the protonation at the β-carbon of *CH2CHO, which leads to the selective formation of C2+ alcohols. In contrast, the unmodified Cu NS is prone to promoting the cleavage of the C─O bond, thereby facilitating the generation of C2H4.

Achieving stereoselective alkyne semi-hydrogenation to E-alkenes remains a persistent challenge due to inherent limitations of conventional catalysts in controlling stereochemistry and suppressing over-hydrogenation. Herein, we resolve this fundamental dilemma through a rationally designed brominated Pd-on-Au nanocatalyst (Pd0.03-Br1^Au/TiO2) featuring spatially segregated active sites operating via reductive relay isomerization. This sophisticated architecture enables unprecedentedly efficient E-alkene synthesis (>96% selectivity for trans-stilbene at near-quantitative conversion). Fabricated by sequentially depositing Au nanoparticles on TiO2, with tiny Pd loading on Au, and controlled surface bromination, the catalyst leverages synergistic cooperativity: The TiO2-Au interface primarily activates formic acid (FA) to generate reactive surface-bound hydride species (H*) while minimizing unproductive H2 formation; concurrently, atomically dispersed Pd1 sites on Au nanoparticles exclusively mediate rapid Z-to-E isomerization, whereas bromide-capped Pd nanoclusters kinetically regulate FA dissociation kinetics at TiO2-Au interface and sterically block overhydrogenation adsorption geometries. This spatially orchestrated multisite system decisively overcomes classical activity-selectivity trade-offs, establishing a universally applicable framework for decoupling and optimizing individual catalytic functions in heterogeneous design. Our work delivers both a sustainable strategy for scalable trans-alkene production and fundamental mechanistic insights into complex cooperative reaction networks.

Abstract Herein, two Cu‐based model electrocatalysts, Cu nanosheets modified with Cd single atoms (Cd‐SACs@Cu NS) and unmodified Cu nanosheets (Cu NS), were rationally designed to investigate the C–C coupling to C 2+ alcohols mechanisms in CORR. Compared to Cu NS, Cd‐SACs@Cu NS exhibits a significantly enhanced Faradaic efficiency (FE) for C 2+ alcohols of nearly 70% at an unprecedented current density of 1100 mA cm −2 and maintains a higher FE (>50%) over a broad range of current densities (100–2100 mA cm −2 ) under alkaline conditions in a flow cell. In situ characterizations and theoretical studies reveal that the enhanced selectivity toward C 2+ alcohols on Cd‐SACs@Cu NS is attributed to the improved H 2 O dissociation at atomically dispersed Cd sites and enhanced CO adsorption on the paired Cu atoms adjacent to single Cd atoms. These effects synergistically facilitate the spillover of hydrogen atoms from Cd to Cu sites, thereby promoting the protonation at the β‐carbon of *CH 2 CHO, which leads to the selective formation of C 2+ alcohols. In contrast, the unmodified Cu NS is prone to promoting the cleavage of the C─O bond, thereby facilitating the generation of C 2 H 4 .

The transformation of lignocellulosic biomass into long-chain aliphatic hydrocarbons (C7–C9) represents a pivotal route for fuel/additive production, yet conventional processes often suffer from low carbon efficiency due to uncontrolled C–C cleavage. Herein, we report an innovative sequentially coupled coupling–hydrodeoxygenation strategy that enables the complete conversion of furfural and short-chain alcohols (C2–C4) into corresponding aliphatic hydrocarbons with 100% carbon atom economy. A triple single-atom catalyst (Co/Cu/Ni–TSA), featuring atomically dispersed Co, Cu, and Ni sites on a hierarchical N-doped carbon framework, was designed to catalyze both the oxidative coupling and subsequent hydrodeoxygenation steps in a continuous flow system. Mechanistic studies unveil synergistic interactions among the metal single atoms, wherein Co and Cu facilitate substrate activation and coupling, while Ni modulates electronic structures to lower energy barriers. The integrated process demonstrates good stability and scalability, converting 32.4 g of furfural with isopropanol into 39.1 g of n-octane at 99% selectivity over 216 h of continuous operation. This work establishes a paradigm for efficient and atom-economical biomass upgrading to drop-in hydrocarbon fuels.

This work presents a novel microwave‐assisted solvothermal method for decorating nanoflakes of transition‐metal carbides (MXenes) Ti3C2 and V2C with highly dispersed rhodium catalytic sites, significantly enhancing the electrocatalytic efficiency of the hydrogen evolution reaction (HER). The results indicate that microwave treatment does not significantly alter the nanoflake structure but promotes the formation of subnanometer‐sized Rh catalytic sites. A combined analysis of density functional theory‐calculated core‐level shifts and experimental X‐ray photoelectron (XPS) spectra identifies the most likely structures of the Rh catalytic centers formed through the microwave‐assisted solvothermal process. Rh anchored to the oxygen‐terminated MXene nanoflake surface, bonded to two or three oxygen atoms (RhOn), explains the Rh 3d XPS band with a notable chemical shift. Rh‐decorated nanoflakes display superior catalytic performance in acidic, basic, and neutral media compared to pure MXenes. Turnover frequencies (TOF) suggest that the HER catalytic activity of Rh sites is comparable to or exceeds that of pure platinum surface atoms. Using rhodium catalytic site structures as an example, it is demonstrated that the mutual arrangement of the Gibbs free energy of hydrogen adsorption on the catalytic site, in cases with protonated and non‐protonated terminal groups of the nanoflake, can serve as a criterion for electrocatalytic efficiency.

On-site hydrogen production from methanol decomposition has attracted interest in an energy-sustainable society, which compensates for the shortcomings of unsafe hydrogen storage and inconvenient transportation. Here, we constructed Cu1Co single atom alloy (SAA) catalysts containing atomically dispersed Cu sites coupled with Co sites serving as intrinsic Cu-Co active sites for hydrogen production from methanol decomposition. It was demonstrated that the reduction temperatures of CuCo precursors induced the generation of distinct crystalline structures and mixed-phase interfaces of Cu1Co SAA catalysts, thereby efficiently modulating the electronic structures of the active centers and the surface adsorption and desorption behaviors of the reactants during methanol decomposition. The as-fabricated Cu1Co SAA catalyst featuring both the dominant hcp metallic Co phase and abundant hcp/fcc mixed-phase interfaces significantly facilitated a series of dehydrogenation processes of methanol and reaction intermediates and desorption of CO and H2 products and achieved excellent catalytic performance, with an unprecedentedly high hydrogen production rate of 659.8 mol·molCu-1·h-1 at complete methanol conversion. By combining structural characterization, in situ spectroscopic analysis, and density functional theory calculations, it was unveiled that atomically dispersed Cu-Co active sites both in the absolutely predominant hcp phase and at the hcp/fcc mixed-phase interfaces on Cu1Co SAA catalysts played crucial roles in boosting hydrogen production from methanol decomposition. The present study provides a promising single atomic Cu site-mediated crystal phase and phase interface engineering strategy for developing high-performance and economical Co-based catalysts for methanol decomposition to produce hydrogen.

Maping Phosphate Mine operates as a large-scale mining complex characterized by a multi-mining area strip mining layout. This configuration exhibits expansive operational zones, numerous dispersed mining sites, and inherent systemic complexity, collectively complicating ventilation system management. The optimization of ventilation processes across multiple mining areas constitutes a critical measure for enhancing operational safety and efficiency within resource-constrained scenarios. This investigation specifically targets four adjacent mining zones—340B, 380B, 380C, and 420D—where three distinct ventilation schemes were formulated and evaluated. A process-oriented simulation-optimization model combining Ventsim and TOPSIS was developed to evaluate the ventilation systems. The ventilation network architecture and airflow distribution characteristics of the target mining areas were comprehensively simulated, establishing a decision optimization framework for the ventilation system that successfully identified the optimal solution. The results demonstrate minimal error between the simulated and measured data of the mine ventilation network model, validating the accuracy of its system parameter estimations. Simulations of diverse ventilation schemes generated airflow distribution parameters and dust concentration data for each mining area. Subsequently, a TOPSIS-integrated process optimization model was developed to comprehensively evaluate the ventilation schemes against eight quantitative indicators. Evaluation results identified Scheme Two as the optimal solution, as it demonstrates a balanced optimization of safety, efficiency, and cost-effectiveness. This scheme achieves a significant enhancement of the underground ventilation environment and a marked suppression of dust diffusion, with only a marginal increase in overall ventilation costs. By elevating the air volume from an initial less than 1.0 m3/s to a precisely regulated range of 5.0–13.0 m3/s, the scheme fundamentally eliminated ventilation dead zones. This intervention resulted in a significant reduction in dust concentrations across multiple working faces, consistently maintaining levels below the 4 mg/m3 national exposure limit (GBZ 2.1-2019), and ultimately ensured a safer and healthier working environment. The attainment of these practical outcomes, which directly correspond to the optimization objectives of the TOPSIS method, confirms its efficacy and practical value in guiding ventilation strategy selection.

Catalytic conversion of acid waste gases into value-added chemicals is crucial for sustainable carbon and sulfur utilization, and designing efficient and stable catalysts shows great significance in achieving this goal. Herein, we report an olefin-linked, bipyridine-functionalized COF with atomically dispersed Cu active sites (xCu@COF-PzBpy) that combines high specific surface area, robust stability, and an asymmetric Cu-N4 coordination geometry induced by the interlayer stress effect. The newly engineered Cu-N4 active centers demonstrate enhanced activation capability for both acid gases and epoxides, endowing xCu@COF-PzBpy with an exceptional catalytic performance for their upcycling under ambient conditions. This performance outperforms nearly all previously reported catalysts. Similarly, the high catalytic activities of xCu@COF-PzBpy can be extended to the COS and SO2 cycloaddition. No activity loss, Cu leaching, and/or aggregation were observed over 10 cycles. This work provides a new strategy for developing efficient and reusable catalysts for acid waste gas upcycling, addressing environmental challenges while enabling green and sustainable cycles.

While Zn-doping significantly enhances the electrochemical performance of RuO2 for the acidic oxygen evolution reaction (OER), the underlying mechanisms and the optimal design principles remain unclear. Here, we employ a cluster expansion (CE) model based on density functional theory (DFT) calculations to systematically explore energetically favorable configurations of Ru1-xZnxO2 with Zn concentrations ranging from 4.2% to 25%. Our results reveal that varying Zn doping levels can both induce uniform Zn dispersion to create abundant atomically dispersed Ru-Zn dual-metal sites on the RuO2(110) surface and enable precise tuning of Ru-Zn intersite distance to promote oxide path mechanism (OPM) in the OER. Moreover, the operating potential dynamically modulates the electronic structure of these dual-sites, adjusting adsorption energies of the OER intermediates and enabling precise control over reaction pathways. Additionally, the structural stability of Ru1-xZnxO2 during the OER is positively correlated with the Zn-doping concentration and no longer significantly increased when the Zn concentration is >12.5%. Our findings establish two key design strategies for optimizing OPM: (1) maintaining low operating potentials and (2) controlling Zn doping at ∼12.5%. Under such conditions, OPM overcomes the theoretical limitations of conventional adsorbate evolution mechanism (AEM), achieving significantly reduced overpotentials and enhanced durability in acidic OER.

The widespread application of Pt-based catalysts in fuel cells is limited by their high cost and insufficient durability for both the oxygen reduction reaction (ORR) and alcohol oxidation reactions (AOR). Herein, we designed a bifunctional catalyst featuring Pt nanoparticles anchored on the nitrogen-doped carbon support engineered with atomically dispersed Fe-N4 and Co-N4 dual sites (Pt/FeCoNC) for efficient ORR and AOR. For the acidic ORR, Pt/FeCoNC delivers a half-wave potential of 0.90 V vs RHE, with mass and specific activities 5.6 and 5.1 times higher than commercial Pt/C. Impressively, it retains nearly 60% of its initial mass activity after 30,000 durability cycles, far exceeding Pt/C (∼33% retention). Furthermore, the prepared catalyst demonstrates exceptional AOR activity, with mass activities for methanol and ethanol oxidation over 3 times greater than Pt/C. The prepared catalyst utilizes a strong synergistic interaction between Pt and the bimetallic sites to induce electron delocalization, which downshifts the Pt d-band center. This electronic modulation simultaneously weakens the adsorption of poisoning intermediates and enhances nanoparticle stability. The results establish dual-atom site engineering as a highly effective approach to design durable and active bifunctional catalysts for energy conversion.

The development of efficient and sustainable heterogeneous catalysts remains central to the advancement of green oxidation chemistry. Herein, we report a Ni-salphen-derived metalated porous organic polymer (Ni@CAB), synthesized via a simple Friedel-Crafts alkylation strategy that integrates atomically dispersed Ni-N2O2 active sites into a robust carbazole-linked framework. A combination of 2D solid-state 13C-1H double cross-polarization (CP) correlation NMR, XPS, synchrotron-based XAS, and electron microscopy techniques confirmed the structural integrity, amorphous porous architecture, and uniform dispersion of Ni centers. Electronic analyses revealed reduced surface electron density at the Ni sites, enhancing their Lewis acidity and catalytic reactivity. Ni@CAB demonstrated exceptional performance in the aerobic allylic oxidation of cyclohexene under ambient conditions, affording complete conversion with high selectivity and remarkable recyclability over multiple cycles without detectable Ni leaching. Complementary DFT calculations unveiled favorable charge transfer and energetically viable pathways consistent with experimental observations. This study establishes surface electron density as a powerful activity descriptor and underscores the promise of rationally engineered metalated porous polymers for sustainable oxidation catalysis.

Electrochemical nitrate reduction to ammonia (ENRA) is a sustainable approach for the electrosynthesis of ammonia (NH3) and the purification of wastewater. Herein, three polyoxometalate-based (POM-based) mononuclear complexes, namely [M(HNCP)2(H2O)][PW12O40]·H2O (HNCP = 4-(1H-imidazo[4,5-f][1,10]phenanthrolin-2-yl)benzoic acid; M = Ni, Co, Zn, referred to as M-PW12), that feature atomically dispersed metal sites are prepared. Among them, Ni-PW12 exhibits outstanding ENRA performance, with a Faradaic efficiency (FE) of 90.3% and an NH3 yield rate of 11.2mg h-1 mgcat. -1 at -1.3V versus reversible hydrogen electrode (RHE). An in-depth computational study reveals that directional electron transfer from the POM cluster to the metal center diminishes the energy barrier associated with the rate-determining step (*N → *NH) and improves protonation energetics along the NO3 - to NH3 pathway. This study demonstrates that electron-transfer engineering via POM-metal-hybrid systems delivers a 24.1-39.3% enhancement in NH3 FE compared to a POM-only catalyst. The core mechanism lies in the electron transfer effect between POM and metal components: this effect optimizes the electronic structure of reaction active sites, suppresses the competitive hydrogen evolution reaction, and thus improves the selectivity of NH3 generation. This work provides a concrete strategy forhigh-performance POM-based electrocatalysts and advancessustainable ammonia production.

Molecular engineering and channel structure modulation for single-atom iron-embedded high-porosity carbon fibers with enhanced oxygen reduction reaction and zinc-air battery performance.

Anchoring ruthenium single atoms into the carbon nanotubes-supported nickel-based sulfides for enhanced electrocatalytic oxygen evolution.

Hetero-diatomic dispersed NiCo sites spark enhanced hydrogen evolution performance of PtNiCo nanoclusters via unusual sabatier principle

Increased formation of higher-valence nitrogen oxides: The catalytic effect of altered cobalt-loaded carbon on the thermal decomposition of ammonium perchlorate

Bimodal-Mesoporous hollow carbon nanoreactors with atomically dispersed Co sites for synergistically enhanced electrosynthesis of hydrogen peroxide