Co-Nx Sites Research Articles

Regulating the horizontal confined deposition of lithium metal by Co-Nx modified honeycomb-like carbon nanosheets

The uncontrollable Li dendrite growth as well as the severe volume expansion of Li metal anodes during cycling significantly impedes the practical applications of high-energy-density Li metal batteries. In this work, an innovative modulation strategy has been developed by constructing honeycomb-like nitrogen-doped carbon nanosheets with uniformly anchored cobalt nanoparticles (denoted as Co@HNC) for regulating the Li deposition behavior and meanwhile alleviating volume change during cycling. On one hand, the lithiophilic Co-Nx sites can largely reduce the energy barrier of Li nucleation and subsequently guide horizontal confined Li deposition in the honeycomb-like holes of Co@HNC, which is verified by the density functional theory calculations and in-situ optical microscopy observations. On the other hand, the honeycomb-like carbon framework with good structural integrity can endure the huge volume change during repeated Li plating/stripping processes. Consequently, the optimized Co@HNC electrode delivered a promoted cycling life for over 600 times with high Coulombic efficiency of 98.5 % at 1 mA cm−2. When matched with the high-mass-loading LiFePO4 (20 mg cm−2) or high-voltage LiNi0.8Mn0.1Co0.1O2 cathode, the Li@Co@HNC anode exhibited outstanding cycling stability and rate capability under low negative/positive capacity ratio, demonstrating its great potential in practical applications of high-energy-density lithium metal batteries.

High performance of N-doped cobalt oxide (N-CoOx) for peroxymonosulfate activation: Unraveling the functional mechanism of Co-Nx sites at molecular level

Nitrogen (N)-doping has been reported effective to reinforce catalysis in advanced oxidation processes (AOPs) due to the formation of N-related active sites. Although several documents have reported that transition metal-nitrogen (metal-Nx) sites could work as reactive centers, the catalytic mechanism was hardly elucidated. In this study, N-doped cobalt oxide (N-CoOx) was initiatively prepared via calcination in ammonia atmosphere to construct cobalt-nitrogen (Co-Nx) sites. The emergence of Co-Nx sites effectively improved peroxymonosulfate (PMS) activation efficiency (above 5.8 times), leading to higher pollutant decomposition rate (95.8 % at 30 min) and kinetics constant (above 4.1 times). N introduction changed main facets of material and elevated adsorption energy (Eads) (from −1.81 eV to −3.71 eV) between catalyst and PMS. Co atoms at Co-Nx sites could donate larger quantity of electrons (from 1.088 e to 1.583 e) to PMS, therefore, contributed to stretching and breaking O–O bonds of PMS molecules to form reactive species. As a result, both radical and electron transfer pathway (ETP) were enhanced in the oxidation processes. Ultimately, the catalytic membrane coated with N-CoOx maintained 100 % treatment towards continuous antibiotic wastewater at environmentally relevant concentration (μg/L), realizing purification as well as separation of catalyst. This work systematically elaborates the superiority of Co-Nx sites and unravels the underlying mechanism to inspire further study to metal-Nx tailored catalysis.

High-density Co-Nx sites anchored on biomass-based carbon nanotubes for efficient removal of plant viruses in water

In this study, we selected rice straw, wheat straw and corn cob as raw materials to successfully prepare cobalt-nitrogen co-doped biomass-based carbon nanotubes composites (BM@CoNCNTs) with Co-Nx sites highly dispersed on porous biochar carrier, which could effectively activate peroxymonosulfate (PMS) to remove tobacco mosaic virus (TMV) in water. Particularly, BM@CoNCNTs-CC, with its confined carbon nanotubes and high-density Co-Nx sites, enhanced the Co2+/Co3+ cycle and direct adsorption of PMS to generate Co(IV)=O and 1O2, playing a dominant role. This led to the effective disruption of TMV coat protein and degradation of its genome within 5 min, achieving up to 6 log10 removal efficiency. Additionally, BM@CoNCNTs-CC/PMS system maintained efficient catalytic removal performance even in complex water matrices (river water and tap water). Overall, our research not only elucidates the production of efficient biomass-based catalysts for environmental remediation, but also highlights the application potential of biomass-based carbon nanotubes composites enriched with Co-Nx sites.

A novel flexible electrochemical sensor with multi-level carbon nano-array for in-situ real-time monitoring of H2O2 secreted by cells

Developing ultra-sensitive sensors for in-situ real-time monitoring of low-level cell secretions is of paramount importance in understanding various biological processes, and it is still a challenge. Herein, for the first time, we constructed a novel flexible Au-Co@C-CNT/CC sensing electrode with nano-array structures by in-situ synthesis, catalytic pyrolysis and electrochemical deposition, and successfully realized the real-time monitoring of H2O2 released by cells. The 3D leaf-like structure of the electrode not only provided a large electroactive surface area (7.66 cm2) but also exhibited a microvilli structure of carbon nanotubes (CNT) on the surface, which further enhanced the presence of active sites. Moreover, the Co-Nx sites generated by catalytic pyrolysis can promote the adsorption and catalysis of H2O2 on the surface of sensing electrode. The introduction of Au NPs facilitated the transfer of electrons, thereby enhancing the electrical conductivity and electrocatalytic performance of Au-Co@C-CNT/CC. Benefiting from these unique superiorities, this sensing platform displayed excellent performance for H2O2 determination with a wide linear range (10–27080 μM) and low detection limit (0.13 μM). Notably, the good biocompatibility and flexibility of this sensing platform allowed direct culture of human lung cancer cells (A549 cells) on the electrodes, which can realize dynamic in-situ real-time detection of H2O2 released by cells, showing great potential in the diagnosis of related diseases.

Hollow carbon sphere featuring highly dispersed Co-Nx sites for efficient and controllable syngas electrosynthesis from CO2

Electrochemical reduction of CO2 and H2O powered by green electricity provides a sustainable way to produce syngas. However, this reaction still suffers from insufficient syngas selectivity, slow charge kinetic process, and poor controllability of the CO/H2 ratio. In this work, we report a hollow carbon sphere electrocatalyst featuring highly dispersed Co-Nx sites (Co-NHCS-x) for efficient and controllable syngas electrosynthesis. The Co-NHCS-400 sample exhibits a high syngas production rate with a steady CO/H2 ratio (≈1:2) over a wide range of operating potential from −0.6 V to −1.1 V vs. RHE. The variation in synthesis temperature can finely tune the coordination environment of Co-Nx in the catalyst. Consequently, the adsorption behaviors of the CO and hydrogen atoms can be manipulated, allowing for the precise adjustment of CO and H2 proportions in the product gas. The findings are potentially applicable to the exploitation of promising carbon-based electrocatalysts for electrochemical CO2 conversion into syngas.

Bifunctional ligand Co metal-organic framework derived heterostructured Co-based nanocomposites as oxygen electrocatalysts toward rechargeable zinc-air batteries

Rational construction of efficient and robust bifunctional oxygen electrocatalysts is key but challenging for the widespread application of rechargeable zinc-air batteries (ZABs). Herein, bifunctional ligand Co metal–organic frameworks were first explored to fabricate a hybrid of heterostructured CoOx/Co nanoparticles anchored on a carbon substrate rich in CoNx sites (CoOx/Co@CoNC) via a one-step pyrolysis method. Such a unique heterostructure provides abundant CoNx and CoOx/Co active sites to drive oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), respectively. Besides, their positive synergies facilitate electron transfer and optimize charge/mass transportation. Consequently, the obtained CoOx/Co@CoNC exhibits a superior ORR activity with a higher half-wave potential of 0.88 V than Pt/C (0.83 V vs. RHE), and a comparable OER performance with an overpotential of 346 mV at 10 mA cm−2 to the commercial RuO2. The assembled ZAB using CoOx/Co@CoNC as a cathode catalyst displays a maximum power density of 168.4 mW cm−2, and excellent charge–discharge cyclability over 250 h at 5 mA cm−2. This work highlights the great potential of heterostructures in oxygen electrocatalysis and provides a new pathway for designing efficient bifunctional oxygen catalysts toward rechargeable ZABs.

Synergistic catalysis: cobalt-catalyzed cascade reaction for the oxidative cleavage of olefins to access esters.

An efficient strategy for the oxidative cleavage of CC bonds in olefins to form esters with one or multiple carbon atoms less over heterogeneous cobalt/nitrogen-doped carbon catalyst with dioxygen as the oxidant was described. The protocol features a wide substrate range including the challenging inactive aliphatic and long-chain alkyl aryl olefins. The reactivity of the catalyst did not decrease after reused for seven times. Characterization and control experiments reveal that synergistic effects between the metallic Co nanoparticles and Co-Nx sites provide access to the excellent catalytic activity.

Structural and Reactivity Effects of Secondary Metal Doping into Iron-Nitrogen-Carbon Catalysts for Oxygen Electroreduction.

While improved activity was recently reported for bimetallic iron-metal-nitrogen-carbon (FeMNC) catalysts for the oxygen reduction reaction (ORR) in acid medium, the nature of active sites and interactions between the two metals are poorly understood. Here, FeSnNC and FeCoNC catalysts were structurally and catalytically compared to their parent FeNC and SnNC catalysts. While CO cryo-chemisorption revealed a twice lower site density of M-Nx sites for FeSnNC and FeCoNC relative to FeNC and SnNC, the mass activity of both bimetallic catalysts is 50-100% higher than that of FeNC due to a larger turnover frequency in the bimetallic catalysts. Electron microscopy and X-ray absorption spectroscopy identified the coexistence of Fe-Nx and Sn-Nx or Co-Nx sites, while no evidence was found for binuclear Fe-M-Nx sites. 57Fe Mössbauer spectroscopy revealed that the bimetallic catalysts feature a higher D1/D2 ratio of the spectral signatures assigned to two distinct Fe-Nx sites, relative to the FeNC parent catalyst. Thus, the addition of the secondary metal favored the formation of D1 sites, associated with the higher turnover frequency.

Joule heating-assisted tailoring Co-MOC derived chainmail catalyst to regulate peroxymonosulfate activation for tetracycline destruction: Singlet oxygen integrated direct electron transfer pathways

Rational design of stable and high-efficiency non-precious catalysts to activate peroxymonosulfate (PMS) is crucially important for recalcitrant pollutant elimination. In this study, we present a microwave-assisted combustion heat method to fabricate stable Co-MOC-800 as a highly efficient peroxymonosulfate (PMS) activator for tetracycline hydrochloride (TCH) degradation. Joule heating from short-time microwave irradiation enables the expeditious fabrication of Co-based metal–organic-complex (Co-MOC) precursor, which is carbonized to form the representative Co-MOC-800 chainmail catalyst with a maximum degradation rate of 97% in 10 min. This catalyst still possesses an excellent stability with highly remained activity of the initial cycle after five consecutive runs. The N-doped amorphous carbon encapsulated Co nanoparticles integrated Co-Nx sites play an essential role in activating PMS for TCH degradation through non-radial dominant pathways including singlet oxygen and direct electron transfer. Attributing to the non-radical pathways, the Co-MOC-800-catalyzed PMS activation exhibits relatively high anti-interference ability under different solution pH, inorganic anions and humic acid. Three reaction pathways for TCH degradation are proposed by recording the degradation intermediates, and the toxicity of the detected intermediates was evaluated. The present work provides a vivid example for simply fabricating efficient Co-based catalysts for recalcitrant pollutant elimination via activating PMS.

Oxidative cleavage and ammoxidation of organosulfur compounds via synergistic Co-Nx sites and Co nanoparticles catalysis

The cleavage and functionalization of C–S bonds have become a rapidly growing field for the design or discovery of new transformations. However, it is usually difficult to achieve in a direct and selective fashion due to the intrinsic inertness and catalyst-poisonous character. Herein, for the first time, we report a novel and efficient protocol that enables direct oxidative cleavage and cyanation of organosulfur compounds by heterogeneous nonprecious-metal Co-N-C catalyst comprising graphene encapsulated Co nanoparticles and Co-Nx sites using oxygen as environmentally benign oxidant and ammonia as nitrogen source. A wide variety of thiols, sulfides, sulfoxides, sulfones, sulfonamides, and sulfonyl chlorides are viable in this reaction, enabling access to diverse nitriles under cyanide-free conditions. Moreover, modifying the reaction conditions also allows for the cleavage and amidation of organosulfur compounds to deliver amides. This protocol features excellent functional group tolerance, facile scalability, cost-effective and recyclable catalyst, and broad substrate scope. Characterization and mechanistic studies reveal that the remarkable effectiveness of the synergistic catalysis of Co nanoparticles and Co-Nx sites is crucial for achieving outstanding catalytic performance.

Enhanced electron transfer-based nonradical activation of peroxymonosulfate by CoNx sites anchored on carbon nitride nanotubes for the removal of organic pollutants

The nonradical pathway selectively oxidizes pollutants with less interference from environmental factors, which can effectively improve the environmental suitability of peroxymonosulfate (PMS) activation. Herein, a Co-doped nanotubular carbon nitride catalyst (Co-CNNT) based on CoNx sites was constructed for stable and efficient PMS activation with a better specific surface area, number of CoNx sites, and electron transfer capability than Co-doped lamellar carbon nitride catalyst (Co-CN). Co-CNNT improved PMS utilization efficiency (∼50%) and enhanced the contribution of the electron transfer pathway to tetracycline (TET) degradation. The enhanced ability of Co-CNNT to adsorb PMS leads to Co-CNNT–PMS* generated by PMS at the CoNx site, which raises the Co-CNNT surface potential and allows PMS to be activated in a manner that captured electrons. Thus, the Co-CNNT/PMS system could effectively destroy electron-rich or low-potential pollutants within 24 min. The stronger environmental adaptability allows it to maintain catalytic activity in complex aqueous matrices, achieving effective oxidation of diluted tetracycline-based pharmaceutical wastewater. This paper reveals the effects of carbon nitride morphology control strategies on the properties of CoNx active sites and PMS activation mechanisms, providing new insights into the induction of nonradical PMS activation pathways.

String of ZIF-derived hollow beaded nanocage embedded into carbon nanofiber with intensified exposed Co-Nx sites for efficient oxygen catalysis in various fuel cell devices

The rational control of Co-Nx active sites dispersion in nanomaterials is significant to construct efficient oxygen reduction reaction (ORR) electrocatalysts in fuel cells. Herein, a novel strategy for the scalable synthesis of carbon nanofiber supported hollow beaded nanocage with accessible Co-Nx sites in cavity wall (PAN-Co-ZIF-8-C-A and PAN-Co/ZIF-8-C-A) originated from zeolitic imidazolate frameworks (ZIFs) and polyacrylonitrile (PAN) is reported. Remarkably, the formed samples modified with Co-Nx sites exhibit superior ORR activity, which makes it promising ORR catalysts for microbial fuel cell (MFC) and direct methanol fuel cell (DMFC). Accordingly, the maximum power densities of MFC decorated with PAN-Co-ZIF-8-C-A and PAN-Co/ZIF-8-C-A achieve 869.6 and 888.3 mW cm−2, which are 1.17 and 1.19 times higher than that of Pt/C. In addition, the PAN-Co/ZIF-8-C-A modified DMFC exhibits comparable power density of 23.27 mW cm−2 close to Pt/C electrode (25.63 mW cm−2). Such commendable catalytic performances can be primarily attributed to the synergistic effect of hierarchical porosity for fast mass transport, high conductivity for electron migration, and well-tuned Co-Nx sites for oxygen reduction. This facile-effective optimization strategy may open a new avenue for exposing the catalytic centers of one-dimensional (1D) nanofiber and ZIFs-derived oxygen catalyst in fuel cells.

Bifunctional carbon nanofibrous interlayer embedded with cobalt single atoms for polysulfides trapping and catalysis in lithium-sulfur batteries

Lithium-sulfur (Li-S) batteries are in the spotlight as one of the most promising energy storage systems, specifically suitable for electric vehicles and intelligent electronic devices. However, Li-S batteries still suffer from the shuttle effect of intermediate polysulfides, inducing the loss of active materials and slow redox reaction kinetics. Herein, a freestanding functional nanofibrous membrane with cobalt single atoms supported by porous carbon nanofiber skeletons is fabricated using a one-step carbonization process. The flexible nanofiber structure can provide the characteristics of good conductivity and lightweight, helping the polysulfides trapped in the porous structure of the fibrous skeleton. Moreover, the results of electrocatalytic characterization and theoretical calculation demonstrate the existence of the metal coordinate center Co-Nx sites, and their functions of reducing polarization voltage and accelerating polysulfide conversion. Using this functional nanofiber membrane as an interlayer with the Co-Nx coordination structure (Co@N-PCNFs), the assembled Li-S batteries exhibit a high initial specific capacity (1522 mAh·g−1 at 0.1C) and outstanding rate performance (905 mAh·g−1 at 2C). Especially, the specific capacity of the Li-S batteries can achieve 786 mAh·g−1 at 0.5C with a sulfur loading of 4 mg·cm−2 after 100 cycles. This effective method of fabricating nanofibrous interlayers can effectively promote the development of advanced Li-S batteries and the application of electrospun materials in energy storage fields.

Ultrafine particles of zeolitic imidazolate frameworks induced by efficient nucleation facilitated conversion of microalgal lipids

In order to improve property and utilization of active sites on catalyst surfaces, novel ultrafine particles of zeolitic imidazolate framework (ZIF-67) were synthesized for microalgal biodiesel production. The synergy of N,N-dimethylformamide (DMF) and ethanol promoted deprotonation of imidazole and efficient nucleation of ZIF-67, which reduced crystal size from ∼300 nm (using methanol as solvent) to ∼20 nm. Meanwhile, the ratio of unsaturated coordinated Co-Nx (x = 1,2,3) to saturated CoN4 increased from 0.40 to 0.57, and pyridinic N content on catalyst surface increased from 16.59% to 32.25%, which enhanced the acidity and basicity of catalyst. The total acidity of optimal ZIF-67 increased from 0.125 to 0.691 mmol/g, while total basicity increased from 0.078 to 0.137 mmol/g. Density functional theory (DFT) calculations clarified that unsaturated Co-Nx sites and pyridinic N exhibited excellent catalytic activity. Therefore, ZIF-67-DE catalyst (using DMF and ethanol as solvents) effectively converted microalgal lipids into biodiesel with a catalytic efficiency of 97.8%.

Constructing a novel strategy for one-step colorimetric glucose biosensing based on Co-Nx sites on porous carbon as oxidase mimetics

Nanozyme-based sensing strategy for glucose generally involves a two-step H2O2-bridged cascade reaction. However, this two-step cascade reaction always shows a limited detection efficiency for glucose, which hardly makes simply operation, rapid detection, and sensitivity all promised. Herein, a novel strategy for one-step glucose detection was proposed based on the efficiently competitive relationship between glucose oxidase catalyzed glucose oxidation and oxidase nanozyme catalyzed 3,3′,5,5′-tetramethylbenzidine (TMB) colorimetric oxidation. As a proof of concept, Co-Nx sites on porous carbon (Co-Nx/PC) derived from ZIF-67 was selected as the oxidase nanozyme with O2-sensitive nature, which can activate O2 to produce 1O2 for TMB colorimetric oxidation. In the presence of glucose, the competitive reaction of glucose oxidase catalyzed glucose oxidation occurs, which will obviously inhibit the Co-Nx/PC catalyzed TMB colorimetric oxidation to construct method for glucose detection. The usage of the same reactant O2 and the production of suppressive H2O2 cause a dual effect to this inhibition. In addition, the available pH range of Co-Nx/PC overlaps with that of glucose oxidase, promising a one pot reaction. The proposed method with Co-Nx/PC as oxidase nanozyme based on one-step competitive strategy for glucose detection possesses high detection efficiency with convenience (one-pot), rapidness (total reaction time of 10 min) and sensitivity (LOD of 0.31 μM) all promised, which is superior among the methods based on two-step one-pot or two-pot cascade strategy. The strategy can be successfully applied into the blood glucose detection in human serums with satisfactory results. Also, the strategy can be scalable to other oxidase nanozyme like Mn3O4.

Coupling PtZn intermetallic and atomically dispersed cobalt towards efficient and stable oxygen reduction reaction catalysts

A strong metal–support interaction between PtZn intermetallic and CoNx sites is developed to boost the overall oxygen reduction performance.

Enhanced activation of peroxymonosulfate by abundant Co-Nx sites onto hollow N-doped carbon polyhedron for bisphenol A degradation via a nonradical mechanism

In this study, novel Co-embedded hollow N-doped carbon polyhedrons, derived from ZIF-8@ZIF-67 core–shell structure, were synthesized and used for activating peroxymonosulfate (PMS) towards efficient bisphenol A (BPA) degradation. The contents of different N species, especially Co-Nx and graphitic N sites, were tuned by different calcination temperatures (800, 900, and 1000 °C). Characterization results demonstrated that hollow polyhedron with high graphitization degree and abundant porosity anchored numerous Co nanoparticles, which could enhance the catalytic performance. Compared to other as-prepared catalysts, Co/HNCP-900 (pyrolyzed at 900 °C) showed a more outstanding performance of PMS activation towards BPA degradation, and 95.1 % of BPA (20 mg/L) could be removed within 3 min. Abundant Co-Nx sites were a critical factor to induce the reaction process. Based on trapping, radical scavenger, and electrochemical analysis experiments, a nonradical process (singlet oxygen and direct electron transfer) was proposed to play the dominant role in BPA degradation. Benefiting from the nonradical process, BPA degradation efficiency almost remained stable either in a wide pH range (2.5–8.0) or in the presence of coexisting ions and natural organic matter. The findings of this study will elucidate a new opportunity for improving environmental remediation.

Nitrogen-doped carbon fibers loaded with Co/Co2Mn3O8 alloy nanoparticles as bifunctional oxygen electrocatalysts for rechargeable zinc-air batteries

The lack of low-cost and high-activity bifunctional electrocatalysts for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is an important factor restricting the massive application of rechargeable zinc-air batteries (ZABs). Herein, nitrogen-doped carbon fibers (NCFs) loaded with Co/Co2Mn3O8 alloy nanoparticles (Co/Co2Mn3O8@NCFs) were reported as a bifunctional oxygen electrocatalyst for rechargeable ZABs. The hierarchical porous structure of NCFs and strong synergetic coupling between Co/Co2Mn3O8 alloys and Co-Nx sites accelerated the kinetics of ORR reaction. The abundant lattice oxygen and N-doped sites promoted the efficient OER process. Benefiting from the above advantages, a rechargeable ZAB assembled with Co/Co2Mn3O8@NCFs delivered an excellent energy density of 968.10 Wh kg−1 (normalized to the mass of consumed zinc) and outstanding stable cyclability (steady cycle charge and discharge at 10 mA cm−2 for 120 h), surpassing state-of-the-art Pt/C catalyst (830.86 Wh kg−1/75 h). This study demonstrated the potential value of Co/Co2Mn3O8 alloys in energy conversion and storage.

Highly Dispersed Ru-Co Nanoparticles Interfaced With Nitrogen-Doped Carbon Polyhedron for High Efficiency Reversible Li-O2 Battery.

The lithium-oxygen (Li-O2 ) battery with high energy density of 3860Wh kg-1 represents one of the most promising new secondary batteries for future electric vehicles and mobile electronic devices. However, slow oxygen reduction/oxygen evolution (ORR/OER) reaction efficiency and unstable cycling performance restrain the practical applications of the Li-O2 battery. Herein, Ru-modified nitrogen-doped porous carbon-encapsulated Co nanoparticles (Ru/Co@CoNx -C) are synthesized through reduction of Ru on metal-organic framework (MOFs) pyrolyzed derivatives strategies. Porous carbon polyhedra provide channels for reactive species and stable structure ensures the cyclic stability of the catalyst; abundant Co-Nx sites and high specific surface area (353 m2 g-1 ) provide more catalytically active sites and deposition sites for reaction products. Theoretical calculations further verify that Ru/Co@CoNx -C can regulate the growth of Li2 O2 to improve reversibility of Li-O2 batteries. Li-O2 batteries with Ru/Co@CoNx -C as cathode catalyst achieve small voltage gaps of 1.08V, exhibit excellent cycle stability (205 cycles), and deliver high discharge specific capacity (17050 mAh g-1 ). Furthermore, pouch-type Li-O2 batteries that maintain stable electrochemical performance output even under conditions of bending deformation and corner cutting are successfully assembled. This study demonstrates Ru/Co@CoNx -C catalyst's great application potential in Li-O2 batteries.

Co-doped carbon nitride nanosheets supported on SMFs for peroxymonosulfate activation to degrade tetracycline

For the treatment of antibiotics contained wastewater, developing a highly efficient catalyst is key to peroxymonosulfate (PMS) activation and antibiotics degradation. In this work, nitrogen-doped carbon nanosheets (NCS) coated sintered metal fibers (SMFs) catalyst was designed and developed, which could positively promote the contacting efficiency between PMS, TC and catalysts. In specific, by the dip-coating of SMFs in the cobalt-contained dicyandiamide formaldehyde resin and the following pyrolyzing coordinated polymer procedure, it was possible to create a Co-doped NCS catalyst supported on SMFs. NCS with abundant exposed surface active sites could result in a relatively higher catalytic activity. Microscopy studies confirmed the presence of stacked NCS with high Co active sites loading, which was anchored on the surface of SMFs. The developed Co NCS/SMFs catalyst exhibited a highly degradation efficiency of 96% in 240 min. Effects of operating parameters (including PMS concentration and solution pH) on the TC elimination efficicency were also investigated. Additionally, Co NCS/SMFs exhibited good PMS activation activity in the wide pH range of 2.0–9.0, and acceptable recyclability with over 86% TC removal efficiency after five cycles test. According to SEM, XRD and XPS results, highly exposed active metal sites, O defects, Co-Nx sites and reactivity of Co0 in Co NCS/SMFs played an important role in the enhancement of degradation efficiency. Finally, radical inhibition experiment and corresponding EPR test revealedthe presence of SO4∙−, ∙OH, O2∙− and 1O2 in the TC degradation system, in which singlet oxygen (1O2) was demonstrated to be the dominating reactive species for PMS activation and TC degradation. This work provided an efficient strategy for developing robust monolithic lamellar catalyst for the continuous PMS activated degradation of TC.