Nitrate reduction to ammonia represents a promising route for wastewater treatment and valorizing ammonia recovery, yet faces persistent challenges such as dependence on external power supplies, low production rates, and difficult separation of dilute aqueous ammonia. Herein, we develop a self-powered closed-loop system that couples efficient nitrate reduction with simultaneous NH3 recovery as crystalline MgNH4PO4 (MAP). A Mg anode functions as both sacrificial source and Mg2+ supplier, paired with a CuS-decorated nickel foam (CuS@NF) cathode for nitrate-to-NH3 conversion. The generated NH3 is efficiently separated in situ through a PTFE gasdiffusion membrane and precipitates as solid MAP in external crystallizer. This system achieves a MAP production rate of 4.38 mg center dot cm- 2 center dot h- 1 and an OCV exceeding 8 V. The CuS@NF exhibits 97.13 % Faradaic efficiency and 98.8 % NH3 selectivity. DFT calculations reveal that high electronic density near the Fermi level in the Cu d and S p orbitals facilitates electron transfer, weakens the N-O bonds, and suppresses competing H2O dissociation, thereby enhancing nitrate adsorption, promoting deoxygenation pathway. Spatial decoupling of electrolysis and crystallization mitigates catalyst fouling and improves reduction efficiency by 11.37-fold compared to the coupled baseline. Economic analysis shows a 372.7-fold enhancement in potential revenue, highlighting the techno-economic feasibility of this integrated strategy for simultaneous wastewater purification and resource recovery.

A circular two-stage process is proposed to upcycling silicon-rich hazardous liquid waste into high-value three-dimensional graphene foams (3DGFs). Owing to the silicon contained in the waste, conventional pyrolysis often leads to incomplete detoxification, while directly using it as a carbon feedstock may introduce Si-containing impurities into graphene products. Herein, the process begins with steam-assisted gasification of dimethyldiethoxysilane (DOMS) at 900 degrees C (liquid:steam = 1:2), generating syngas at 68.6 mmol/h with high concentration of H-2, CH4 and C2H4. By increasing the N-2 carrier-gas flow rate, the H-2/CH4/C2H4 ratio can be precisely tuned with higher ethylene fraction for downstream low-defect graphene synthesis. In the second stage, the purified syngas directly serves as the carbon precursor for atmospheric-pressure chemical vapor deposition (APCVD) on nickel-foam templates, facilitating the growth of multilayer 3DGFs with minimal structural defects. Under optimized conditions (900 degrees C, 500 sccm, 30 min), the resulting 3DGFs exhibit a well-defined multilayer architecture (similar to 20 layers), high electrical conductivity (1.18 x 10(3) S/m), and exceptional electromagnetic interference (EMI) shielding effectiveness of nearly 50 dB in the X-band (similar to 99.999 % attenuation). Life-cycle assessment shows that relative to conventional methane-based CVD, this waste-derived route reduces CO2-equivalent emissions and cumulative energy demand by 45 % and 40 %, respectively, and lowers the monetized environmental cost to 8.50 x 10(3) $ per kg 3DGF. This work demonstrates a sustainable pathway for valorizing hazardous siloxane waste into functional graphene materials, supporting circular carbon utilization and carbon mitigation.

Selective resource recovery from waste streams is essential for sustainable nitrogen management. However, conventional ammonia recovery from ammonium (NH4+)-and volatile organic compound (VOC)-containing wastewater is highly energy-intensive, and VOC-NH3 coevaporation further undermines product purity. Here we report an advanced oxidation processes-interfacial solar steam generation (AOPs-ISSG) platform based on a cobalt oxide-loaded nitrogen-doped carbon catalyst (Co-NC) that integrates photothermal conversion and catalytic oxidation. By exploiting the differing adsorption, electron-transfer, and reactive oxygen species (ROS) reactivity of VOCs and NH3, the system achieves selective VOC oxidation while preserving ammonia. Combined with alkaline solar interfacial evaporation, this selectivity supports concurrent VOC removal and efficient NH3 recovery. Under simulated wastewater conditions (pH = 9), the Co-NC/AOPs-ISSG system achieves 90.1% NH3 recovery and 95.3% VOC removal. It also demonstrates broad operational resilience across pH 7-10 and solar intensities up to 1.4 kW m-2, consistently yielding high-purity ammonia suitable for direct reuse, as validated by plant experiments in which recovered-ammonia irrigation promoted ∼40% greater pea seedling growth compared with untreated wastewater. Solar utilization and process integration reduce operating cost and carbon emissions by 23.2% and 27.7% compared with conventional NH3 recovery. These results highlight a low-carbon, economically viable pathway for selective ammonia recovery and sustainable nitrogen management.

Plasma-catalytic ammonia synthesis (PCAS) offers a sustainable pathway to decarbonize the energy-intensive Haber-Bosch process; however, its optimization remains hindered by the complex synergy between plasma physics and catalytic chemistry. Herein, we present a machine learning (ML)-driven framework integrating highdimensional parameter optimization with experimental validation to advance Ru-based catalyst design for PCAS. A comprehensive dataset of 457 data points, specifically focused on cylindrical dielectric barrier discharge (DBD) systems spanning 16 key parameters including catalyst properties, reactor configuration, and operational variable was constructed from published literatures. Among five ML models evaluated, the Random Forest (RF) algorithm achieved superior predictive accuracy for ammonia synthesis rate (R2=0.987) and energy yield (R2=0.887). SHAP (SHapley Additive exPlanations) analysis identified the total gas flow rate as the dominant parameter, revealing its dual regulatory role in modulating radical density and residence time. Systematic optimization determined the optimal ranges for reaction temperature (250-350 degrees C), total gas flow rate (200-300 mL/min), Ru loading (1-3 wt%), and calcination time (4-5 h). Notably, Co doping enhanced catalytic performance by improving Ru dispersion and increasing specific surface area, achieving the metrics of 3455.63 mu mol center dot g-1 center dot h-1 and 1.73 g/kWh. Experimental validation confirmed model robustness, with deviations between predicted and measured NH3 yields predominantly below 10 %. This study establishes a paradigm shift in catalyst development, combining interpretable ML with plasma-catalysis fundamentals to unlock scalable green ammonia production.

The massive accumulation of electronic waste (e-waste) urgently demands innovative recycling technologies to overcome the limitations of traditional methods. Here, we report an ultrafast halogen-assisted indirect Joule heating (HIJH) strategy to achieve the concurrent high-efficiency recovery of precious metals and the upcycling of hazardous residues into high-performance functional materials. Within a 3-s reaction window, the HIJH process facilitates the selective volatilization of 90% Ag and 56% Au through tailored chlorination and iodination pathways, the latter governed by Hard-Soft Acid-Base (HSAB) interactions. Concurrently, toxic heavy metals, including Zn (99%) and Pb (90%), are effectively stripped from the matrix, yielding a decontaminated silicon‑carbon precursor. Crucially, the extreme thermal environment triggers an in-situ carbothermal and silicidation transformation, converting the mineral residue into a composite comprising silicon carbide (SiC), α‑iron (α-Fe) and copper silicide (Cu3Si). This unique phase evolution, combined with the rapid thermal quenching, creates a complex network of heterogeneous interfaces and structural defects. The derived residues exhibit exceptional electromagnetic wave (EMW) absorption, achieving an ultra-low reflection loss (RLmin) of −60.8 dB and a broad effective absorption bandwidth (EAB) exceeding 2 GHz. RCS simulations demonstrate the effectiveness of the composite materials in reducing radar visibility. The energy consumption of HIJH process is merely 1/52 of traditional pyrometallurgy. This “one-stone-two-birds” approach not only mitigates environmental risks through deep detoxification, but also establishes a sustainable, high-value valorization route for urban mining, transforming environmental liabilities into strategic electromagnetic shielding resources.

The electrochemically upgrading sulfate to high-value persulfate (PS) offers significant potential but suffers from impaired selectivity due to competing oxygen evolution reactions (OER). Boron-doped diamond (BDD) electrodes serve as ideal anodes for PS electrosynthesis due to their wide electrochemical window, low adsorption propensity, and superior hydroxyl radical (center dot OH) generation capacity. Herein, we engineered BDD anodes via a facile one-pot deposition-calcination strategy to construct a Ce0.1Sn2.2Sb0.25Oxcatalytic layer, dramatically enhancing center dot OH production. The modified electrode exhibited substantially elevated oxygen evolution potential (increasing from 2.726 to 2.905 V vs. RHE), achieved a record Faradaic efficiency (FE) of 90.22 % for PS synthesis at 250 mA/cm2, and reached 66.7 mu mol/min/cm2. The resulting PS solution was concentrated to 1.16 mol/L (15.3 wt %), the highest value reported to date for electrochemical PS synthesis. Electron paramagnetic resonance (EPR) studies confirmed the significant augmentation in center dot OH yields. The incorporation of Sb refined SnO2 crystallites and strengthened H2O adsorption, whereas trace Ce doping markedly improved the stability of catalytic layer and facilitated electron transfer, as evidenced by only a 0.95 % activity loss after 30 successive electrolysis cycles. Mechanistic investigations reveal that the catalytic layer preferentially promotes the indirect oxidation pathways via center dot OH mediation, leading to a marked increase in PS selectivity. This work establishes a simple, cost-effective, and scalable BDD modification strategy with significant industrial potential for electrochemical PS synthesis and waste sulfate resource valorization.

The electrocatalytic N-2 reduction reaction (ENRR) for sustainable NH3 synthesis remains constrained by the inertness of the N=N bond and strong competition from the hydrogen evolution reaction. We present a gas-liquid plasma-electrocatalytic tandem reactor that integrates non-thermal plasma (NTP) activation of N-2 with efficient H2O-derived proton utilization over a Cu catalyst, enabling one-step NH3 synthesis under ambient conditions. This system simultaneously dissociates N2 into active nitrogen components (ANCs) and optimizes atomic hydrogen (*H) adsorption in strong acid (pH <= 1). The synergistic NTP-ERR process demonstrates a record NH3 production rate of 150.2 mu mol/h at similar to 20 mA/cm(2)-exceeding conventional ENRR by over 150-fold and surpassing the sum of separate NTP and ERR processes. Mechanism studies indicate NH3 forms mainly via direct coupling of ANCs with *H on Cu(111), with a secondary pathway involving NOx- reduction. The system's specific energy consumption (1161 kWh/kg NH3) outperforms existing plasma-assisted technologies. Compatible with renewable electricity, this strategy overcomes key limitations in nitrogen fixation and HER suppression, offering a practical route to decentralized ammonia production.

The rapid expansion of wind energy has intensified end-of-life challenges associated with retired wind turbine blades (WTBs). Here we report an electricity-driven upcycling strategy based on indirect Joule heating (IJH) that converts WTBs powders into high-performance electromagnetic wave-absorber, while co-producing high-purity syngas. IJH enables millisecond-to-second thermal transients, reaching peak temperatures of up to 3400 degrees C within 0.5 s at 80 A, thereby driving carbothermal conversion and solid-state reactions among inorganic constituents within energization times below 2 s. Ultrafast reduction of glass-fiber SiO2 by resin-derived carbon forms crystalline SiC with concurrent CO evolution, while a coupled redox cascade converts trace Fe species into FeSi, jointly constructing dense SiC/FeSi heterointerfaces that promote interfacial polarization. As a result, the composites exhibit dielectric-loss-dominated dissipation and exceptional thin-layer microwave absorption, achieving a minimum reflection loss of -62.18 dB at a thickness of 2.4 mm with an effective absorption bandwidth of 3.54 GHz. In parallel, the gaseous products contain up to 94 vol% H2 and CO. Life-cycle assessment shows that IJH substantially reduces environmental burdens, with a greenhouse-gas emissions of 722.2 kg CO2eq t- 1 (1.7% lower than solvolysis and 87% lower than incineration), alongside a total revenue of approximately $14,082.6 t- 1. Together, these results establish IJH as a power-tunable, low-carbon route for converting composite waste into functional materials, advancing circularity in wind-energy infrastructure.

High-temperature gasification is currently an effective technology for the resource utilization of organic wastewater. However, the reaction mechanisms and product distributions of different waste liquids in hightemperature furnaces remain unclear. This work uses water-containing methanol as a typical material and establishes a computational framework utilizing detailed mechanistic model to study its gasification in an industrial entrained-bed gasifier. A discrete phase model was employed to simulate the vaporization process. By integrating the GRI-Mech 3.0 and AramcoMech 3.0 reaction mechanisms and implementing dynamic trimming, the computational efficiency was enhanced while maintaining the integrity of the mechanisms. The results indicated that when the oxygen-to-fuel ratio (OFR) was 0.6 and the water content was below 10 wt%, and the average droplet diameter ranged from 100 to 300 mu m, complete conversion of methanol can be achieved. The total concentration of syngas components H2 and CO exceeded 60 %. The lower heating value (LHV) can reach 6.6 MJ/Nm3, and the total LHV of the gasifier was 46 MW. Further increases or decreases in OFR, larger droplet sizes, or increased water content all lead to flame contraction, increased wall temperature, or a decline in syngas quality. The methods described in this work have the potential for extension to multi-carbon organic waste liquids, providing a feasible path for the precise design and operational optimization of industrial entrained-bed reactors.

Developing highly efficient piezocatalytic systems requires effectively synchronizing mechanical energy harvesting with surface redox chemistry. Herein, we report a dual-regulatory strategy utilizing a spinel ZnCo₂O₄ piezoelectric catalyst for ultrasound-assisted peroxymonosulfate (PMS) activation. We demonstrate that Zn substitution within the Co₃O₄ lattice precisely modulates both its physical and chemical properties. Physically, Zn-induced lattice distortion significantly enhances the piezoelectric response (d₃₃ = 95.8 pm/V), providing a robust driving force for charge separation. Chemically, it upshifts the Co d-band center and promotes oxygen vacancy formation, optimally tuning PMS adsorption. Consequently, the optimized ZnCo₂O₄ exhibits exceptional piezocatalytic activity, degrading 2,4-dichlorophenol at a rate 3.6 times faster than pristine Co₃O₄. Crucially, quantitative analyses and density functional theory calculations reveal a non-radical pathway largely mediated by high-valent Co(IV)=O species. The synergy between this tailored electronic structure and external stress drastically lowers the energy barrier for the rate-determining O-O bond cleavage to merely 0.52 eV during Co(IV)=O formation. Demonstrating robust practical viability, this system achieves >97% chemical oxygen demand removal in real landfill leachate concentrate. This study provides fundamental atomic-level insights into coupling piezoelectricity with intrinsic catalytic activity, establishing a powerful paradigm for mechanical-energy-driven environmental remediation.

Per- and polyfluoroalkyl substances (PFAS) are known for their strong C-F bonds, which make them highly persistent in the environment and resistant to degradation. Among PFAS, perfluorobutane sulfonate (PFBS), a short-chain PFSA widely used as a replacement for long-chain PFAS like perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS), has garnered attention due to its environmental persistence and toxicity. Although PFBS has lower bioaccumulation potential than its long-chain counterparts, it remains a significant pollutant with limited data available on its degradation mechanisms. To address this, the present study investigates PFBS degradation under subcritical water hydrothermal conditions. Various alkaline substances and additives were tested, and degradation products were analyzed by liquid and gas chromatography-mass spectrometry. Results show that 2 M NaOH at 325°C achieved an ∼99.4 % PFBS removal rate, and the degradation pathway began with the breakdown of the S-C bond, followed by C-F bond cleavage, resulting in the formation of smaller fluorinated compounds, including trifluoroacetic acid. Density functional theory (DFT) calculations provided detailed insights into the degradation mechanism, identifying hydroxide ion attack on the sulfonic acid group as the initial step and elucidating three distinct pathways for subsequent reactions. This study provides key insights into PFBS degradation mechanisms, emphasizing the synergistic effect of alkaline bases and additives. The findings support the optimization of subcritical hydrothermal treatment for PFAS removal, providing a scalable and environmentally sustainable solution.

Lignocellulosic biomass offers a carbon-neutral pathway to produce renewable chemicals and advanced materials. Here, we present an innovative tandem strategy integrating catalytic hydrothermal conversion and flash Joule heating (FJH) to co-produce furfural and structurally optimized graphene from sugarcane bagasse. Utilizing a gamma-valerolactone (GVL)/CoCl2 catalytic system, a high furfural yield of 65 % was achieved directly from solid biomass residues, surpassing conventional acidic hydrolysis systems. Concurrently, hydrothermal residues from GCo were tailored into aromatic-rich precursors enabling high-quality flash graphene synthesis. Raman analysis revealed the GCo-derived graphene exhibited exceptionally low defect density (ID/IG = 0.65 vs 0.85 in non-catalytic (BK) system) and enhanced 2D crystallinity (I2D/IG = 1.8), attributed to optimized oxygen functionalities removal during catalytic hydrothermal reactions. The resultant graphene demonstrated superior photothermal performance, achieving a solar vaporization rate of 1.99 kg & sdot;m-2 & sdot;h-1 under 1-sun irradiation, which is higher than state-of-the-art biomass-derived carbon evaporators. Techno-economic analysis underscored the viability of this approach, with the GCo-FJH route generating a net profit of $3937.08 per ton of biomass, 1.98-fold greater than BK-FJH pathway. This work bridges biomass refining and advanced material synthesis, offering a profitable, zero-waste solution for sustainable biorefineries.

Boron-doped diamond (BDD) electrodes represent high-performance promising anodes for electrochemical wastewater oxidation. While boron-doped microcrystalline diamond (BDMD) electrodes are well-established, the transition to nanocrystalline diamond (BDND) anodes lacks systematic understanding of growth kinetics, degradation performance, and failure behavior. This work fabricates BDND anodes via hot filament chemical vapor deposition (HFCVD), elucidating the synergistic effects of CH4 concentration (2-15 %), reaction pressure (3000-6000 Pa), and substrate temperature (700-1000 degrees C) on the film characteristics. Experimentally synthesized 1*1 cm BDND and successfully enlarged it to phi 100 mm BDND. A predictive growth kinetics model was established with 7.28 % fitting error, enabling precise nanodiamond synthesis control. Comparative electrochemical mineralization studies using artificial wastewater revealed equivalent mineralization efficiency (>95 % TOC removal) between BDND and BDMD anodes, while accelerated lifetime testing demonstrated 32.8 % extended service life (2.66 years vs. 2 years at 100 mA/cm(2)) for BDND. The BDND mineralization pollutant capacity synthesized was significantly higher than that of the control active anode, and had a similarly high removal capacity for actual urine. This durability enhancement originates from nanoscale homogeneity distributing interfacial stresses, suppressing delamination. Our findings establish fundamental synthesis-structure-durability relationships and provide an optimal synthesis window for BDND electrodes, advancing their implementation in industrial electrochemical oxidation systems.

This study presents a sustainable approach to producing geopolymer foam concrete by incorporating sewage sludge ash (SSA), a porous, aluminosilicate-rich byproduct of sewage sludge incineration. The effects of SSA dosage, alkaline activator modulus, and foam stabilizer content on the physical properties, microstructure, phase composition, carbon footprint, and thermal insulation performance of SSA-enhanced geopolymer foam concrete (SGFC) were systematically investigated. The results indicated that the SGFC exhibited optimal performance with a 30 % SSA dosage, an alkali activator modulus of 1.4, and 2 % foam stabilizer content. Under these conditions, SGFC achieved a significantly improved thermal insulation performance due to its optimized pore structure, with a thermal conductivity of 0.081 W/m·K and an exterior wall energy consumption of 39.0 W/m2, while carbon emissions were as low as 136 kg CO2/m3. These findings underscore the potential of SSA as a reactive and eco-friendly precursor for high-performance, low-carbon construction materials.

Persistent and mobile trace organic contaminants (TrOCs) in urban stormwater are difficult to remove through sedimentation- or sorption-based treatment and pose a risk to aquatic ecosystems and drinking water supplies. We demonstrate that the chemical oxidant peroxydisulfate (PDS) can be activated by shrimp shell biochar at pH 7 to form reactive species that selectively react with widespread stormwater contaminants. Of 11 TrOCs tested, oxidative transformation was observed for 1,3-diphenylguanidine, 2-hydroxybenzothiazole, 1H-benzotriazole, 5-methyl-benzotriazole, and diuron during water treatment with biochar and PDS. Laboratory batch experiments conducted with street runoff and a synthetic water showed that the water matrix, containing up to 7.5 mg L-1 dissolved organic carbon and 100 mM chloride, had a minor effect on the formation of reactive species and contaminant transformation. Using a set of scavengers and probe compounds, we provide evidence for singlet oxygen (1O2) as the predominant reactive species in the biochar/PDS system, which is in agreement with the selectivity of the process to oxidize electron-rich organic contaminants. The results of our study inform new strategies for stormwater treatment using heterogeneous oxidation processes for the abatement of persistent and mobile organic contaminants.

Sulfamethoxazole (SMX), a common broad-spectrum antibiotic, has received widespread attention due to its adverse effects and ecological risks. Herein, the UV/PMS/sulfite process was proposed to efficiently remove SMX in the aqueous solution. Under the conditions of pH 9.0, PMS concentration of 300 mu M, and sulfite concentration of 50 mu M, the removal rate of SMX reached 52.7 % within 13 min. There was a similar trend between the change in the degradation rate constants and the speciation of HSO3-, HSO5- as pH varied. HSO3- had a greater impact on the removal efficiency than SO32-, which implied that PMS might not be activated through the single electron transfer. The scavenging experiments and the electron paramagnetic resonance revealed that sulfate radicals (SO4 & sdot;-), peroxysulfate radicals (SO5 & sdot;-), hydroxyl radicals (OH & sdot;), and singlet oxygen (1O2) might lead to the degradation of SMX. The quantum chemical calculations showed that the efficient transformation of PMS was attributed to the nucleophilic addition of HSO5- to HSO3-, which precisely explained the reason for the highest kobs at pH 7.0. The cleavage of peroxide bond of the adduct led to the generation of sulfite radicals (SO3 & sdot; -) and SO4 & sdot; -. Then, SO3 & sdot; - could directly react with the dissolved oxygen in water to produce SO5 & sdot;-, and SO5 & sdot; - had the potential to convert into SO4 & sdot; - and 1O2 through the self-reaction. These studies may offer some understandings into the activation mechanism of PMS, and it has potential practical application for the degradation of other pollutants.

Geopolymers have emerged as promising low-carbon cementitious materials. This study investigated the use of geopolymer for the solidification/stabilization (S/S) of nickel-containing electroplating sludge (NES), focusing on the binding interactions between Ni2* and geopolymer, as well as evaluating the effectiveness of the S/S process. The results showed that Ni2 + incorporation promoted the geopolymerization, due to the substitution of Ca2+ by Ni2+ increased Ca2+ concentration in the pore solution, which in turn stimulated the nucleation and subsequent growth of C/N-A-S-H gels. The immobilization mechanism of Ni2+ in geopolymer including chemical binding and physical encapsulation. Geopolymer gels chemically immobilized Ni2+ through covalent bonding and ion exchange processes. Additionally, the higher alkalinity refined the pore structure of geopolymers and enhanced the physical encapsulation to Ni2+. The S/S results demonstrated that NES can be repurposed as lowgrade construction materials through geopolymerization. With a sludge content of 70 % in the high alkalinity geopolymer (HA) system, the compressive strengths of the mixture reached 5.2 MPa and the Ni2+ leaching concentration dropped from 946.17 mg/L to 2.69 mg/L, compared to the untreated NES. Moreover, the carbon emission of designed HA systems was 86 % lower than that of tradational Ordinary Portland Cement. This study provides valuable insights into how geopolymer respond to Ni2* incorporation and presents a low-carbon strategy for treating NES.

The electrochemical NO reduction reaction (NORR) toward NH3 synthesis not only helps address issues of air pollution but also holds significant energy and economic value, making it an innovative method with broad application prospects. However, designing NORR electrocatalysts that are both highly active and selective remains a formidable challenge. Herein, we study the main-group p-block metal (M = Al, Ga, and In)-doped C3N monolayers as promising single-atom catalysts (SACs) for NORR through spin-polarized first-principles calculations. Our results show that Al@VCC, Al@VCN, Ga@VCC, and Ga@VCN systems are not only stable but also exhibit metallic characteristics, ensuring effective charge transfer during the NORR process. Moreover, nitric oxide (NO) can be strongly chemisorbed and activated on all four candidates with adsorption free energies ranging from -0.83 to -1.59 eV and then spontaneously converted into NH3 without the need for any applied voltage. More importantly, Ga@VCN possesses a well-suppressed ability for the formation of H2/N2O/N2 byproducts, indicating excellent NH3 selectivity. These findings not only offer a promising electrocatalyst for the NO-to-NH3 conversion but also highlight the great potential of main-group metals as SACs for electrochemical reactions.

In this study, we synthesized Co3O4 nanoparticles with distinct morphologies, including nanocube, nanotruncated octahedron, and nanopolyhedron with featured exposure of (001), (111), and (112) facets, respectively. The Co3O4-NC/CNTs-PMS (peroxymonosulfate) system demonstrated a significantly higher steady-state O-1(2) concentration of 8.84x10(-10) M with 99.5 % selectivity, marking a 462-fold increase compared to Co3O4-NP/CNTs-PMS. Density Functional Theory (DFT) calculations revealed that the (001) facet facilitates O-1(2) production by lowering the energy barrier for the rate-determining step from *OH to *O. Furthermore, we introduced the sum of Hammett sigma-para constants (Sigma sigma(p)) as a predictive descriptor, capable of estimating degradation rates with 87 % accuracy. This study systematically elucidates the influence of Co3O4 crystal facets on O-1(2) generation, providing valuable insights into the design of catalysts and optimization of PMS activation strategies for the efficient degradation of recalcitrant pollutants in complex water matrices.

The efficient catalytic elimination of chlorinated volatile organic compounds (CVOCs) at low temperature and low energy consumption remains a significant challenge, and significant breakthroughs are difficult to achieve by optimizing the composition and structure of catalysts. In this study, significant advancements in the catalytic activity of chlorobenzene (CB) and energy consumption reduction are achieved by replacing the traditional external heating mode (tube furnace) with Joule heating. A porous MnOx-CeO2 (MnCe) active layer is constructed on the surface of nickel foam (NF) by the spray method, and a Joule heating-driven MnCe-NF catalytic system is successfully developed. Compared with the external heating method, the electric effect of Joule heating enhances the activation capacity of lattice oxygen and the surface acidity, thus promoting redox properties and inhibiting chlorine deposition. Hence, the T-90 of CB conversion and COx yield under Joule heating are reduced by 10 degrees C and 24 degrees C, respectively. Excellent long-term catalytic stability (>48 h) and water tolerance (5 vol%, 10 vol%, and 15 vol%) are demonstrated by the MnCe-NF under Joule heating. Moreover, the formation of toxic polychlorinated by-products (e.g., dioxins) is reduced from 0.74 ng I-TEQ Nm(-3) (External heating) to 0.089 ng I-TEQ Nm(-3) (Joule heating). The rapid temperature response (<10 s) of Joule heating enables dynamic adaptive degradation of 50-400 ppm CB with energy consumption lower than 11 W, resulting in at least a 92.7 % reduction in energy consumption compared to external heating. The Joule heating also possesses promising advantages of being driven by clean and renewable electricity. This work provides an innovative solution for green net-zero emissions of industrial CVOCs.