Oxygen Activation Research Articles

Metal-support interaction in supported Pt single-atom catalyst promotes lattice oxygen activation to achieve complete oxidation of acetone at low concentrations

A precious metal catalyst with loaded Pt single atoms was prepared and used for the complete oxidation of C3H6O. Detailed results show that the T100 of the 1.5Pt SA/γ-Al2O3 catalyst in the oxidation process of acetone is 250 °C, the TOF of Pt is 1.09 × 10−2 s−1, and the catalyst exhibits good stability. Characterization reveals that the high dispersion of Pt single atoms and strong interaction with the carrier improve the redox properties of the catalyst, enhancing the adsorption and dissociation capability of gaseous oxygen. DFT calculations show that after the introduction of Pt, the oxygen vacancy formation energy on the catalyst surface is reduced to 1.2 eV, and PDOS calculations prove that electrons on Pt atoms can be quickly transferred to O atoms, increasing the number of electrons on the σp * bond and promoting the escape of lattice oxygen. In addition, in situ DRIFTS and adsorption experiments indicate that the C3H6O oxidation process follows the Mars-van Krevelen reaction mechanism, and CH2 =C(CH3)=O(ads), O* (O2-), formate, acetate, and carbonate are considered as the main intermediate species and/or transients in the reaction process. Particularly, the activation rate of O2 and the cleavage of the -C-C- bond are the main rate-determining steps in the oxidation of C3H6O. This work will further enhance the study of the oxidation mechanism of oxygenated volatile organic pollutants over loaded noble metal catalysts.

Visible light assisted periodate activation with porous C3N5 for tetracycline degradation: Enhanced electron-hole separation and reactive oxygen species formation

In this study, porous C3N5 (p-C3N5) was synthesized to activate periodate (PI) for tetracycline (TC) degradation under visible light condition. Experimental results confirmed that the porous structure in C3N5 created abundant defects as active sites, which not only increased the photoelectricity and electron-hole separation efficiency, but also promoted PI activation and reactive oxygen species formation, achieving significantly improved PI-assisted photocatalytic performance. In detail, p-C3N5 exhibited high photocurrent density which was 12.7 and 28.9 times as much as those of g-C3N5 and g-C3N4 respectively. Moreover, the p-C3N5/PI/vis system can achieve 80% TC removal rate within 10 min via ∙O2-, 1O2, IO3∙, ∙OH, h+ and electron transfer pathways. Furthermore, this system could maintain stable degradation capacity under a wide pH range, with less interference by inorganic anions, demonstrating its high reusability, robustness and environmental friendliness. Six possible degradation pathways of TC were proposed based on the detection of intermediate products and density functional theory calculation. Finally, the toxicity assessment showed a significantly reduction of TC bio-toxicity after treatment by p-C3N5/PI/vis system, and no formation of iodine by-products. It provides a deep insight into designing high efficiency and environmentally photocatalysts for activating PI to treat the antibiotic wastewater.

Modulating Copper Ladder Spacing in Copper Phenylacetylide for Enhanced Photocatalysis via Substituent Control.

Copper phenylacetylide (PACu) is a promising photocatalyst due to its unique copper ladder (CL) electron transport channel, which facilitates efficient charge transfer. However, the structure-activity relationship between the CL spacing and its catalytic performance has yet to be revealed. In this study, we skillfully selected multiple substituents to regulate the CL spacing of the PACu photocatalyst. Our findings indicate that reducing the CL spacing significantly enhances carrier separation and transport efficiency, leading to improved oxygen adsorption and activation. Specifically, PACu-F demonstrated superior photocatalytic activity, achieving a 99% conversion rate in benzylamine oxidation and maintaining an excellent stability over multiple cycles. This study confirms the feasibility of tuning the CL spacing in PACu using donor/acceptor substituents to achieve a high-efficiency photocatalytic performance, offering crucial insights into the rational design of advanced photocatalysts.

Ir doping improved oxygen activation of WO3 for boosting acetone sensing performance at low working temperature

Thermally excited oxygen activation is the key to realize gas sensing by semiconductor. However, the relevant strategies and mechanisms are rarely studied. Herewith, the model material of highly oxygen catalytic active Ir doped WO3 (Ir-WO3) is prepared to elucidate the impact of enhanced oxygen activation on sensing performance. Interestingly, the 0.5 wt% Ir doped WO3 successfully reduced the working temperature of WO3 from 370 to 260 ℃ and significantly enhanced the response from 25.1 to 127.9 (at 50 ppm) for acetone. Meanwhile, the sensor also has fast response/recovery times (∼8.3/3.8 s), long-term stability, low detection limit (19 ppb) and high selectivity. Gas sensitive performance tests, in situ-DRIFTS and DFT calculations reveal that the Ir doping facilitates the oxygen adsorption and activation, which can significantly weaken the activation energy of acetone at low temperatures and contribute to enhance sensing performance. Our work paves a new pathway to improving metal oxide-based gas sensors at lower operating temperatures.

The effect of supported metal Species on soot oxidation over PGM/CeO2-ZrO2

Abstract Herein is studied the soot oxidation over platinum group metal oxide/CeO2–ZrO2 (PGM/CZ) catalysts. The ability to capture gas-phase oxygen was in sequence of Ru/CZ > Rh/CZ > Ir/CZ > Pt/CZ > Pd/CZ. A soot oxidation test by TG-DTA showed that Ru/CZ, Rh/CZ, and Ir/CZ are highly active catalysts. It was found that there is a good correlation between the ability to capture gas-phase oxygen and soot oxidation activity. TEM observation revealed that soot oxidation mainly occurs at the interface between soot and CZ surfaces. The Ea values and soot oxidation test using labelled oxygen suggest that highly active catalysts oxidize soot by CZ lattice oxygen. For Ir/CZ, soot oxidation at 270 °C occurred due to the reduction by soot. Ru/CZ and Rh/CZ captured gas-phase oxygen spontaneously below 250 °C, resulting in soot oxidation at 270 °C. H2-TPR results suggest that the reactivity of lattice oxygen in the CZ surface, improved by PGM, is also related to soot oxidation activity. This suggests that the ability to capture gas-phase oxygen and the reactivity of lattice oxygen in the CZ surface determine the soot oxidation activity, and that Ru, Rh, and Ir have the effect of enhancing these properties.

Efficient generation of singlet oxygen (1O2) by CoP/Ni2P@NF for degradation of sulfamerazine through a heterogeneous electro-Fenton process at circumneutral pH

In electro-Fenton (EF), the development of a catalytic material with wide pH application range and high interference resistance is more suitable for practical wastewater treatment. In this study, the nanoneedle-shaped CoP/Ni2P heterostructure loaded onto a nickel foam substrate (CoP/Ni2P@NF) was successfully fabricated, which was used as a cathode material for heterogeneous electro-Fenton (Hetero-EF) to degrade sulfamerazine (SMR) at circumneutral pH. The SMR degradation efficiency within 90 min went to 100% and 87% at initial pH of 6.8 and 11, respectively. Experiments and theoretical calculations demonstrated that the heterostructure of CoP/Ni2P redistributed the interfacial charge and accelerated the electron transfer, resulting in different two-electron oxygen reduction (2e−ORR) selectivity and activity than CoP and Ni2P. The ion interference and complex water quality experiment exhibited that the degradation performance remained almost unchanged, showing better anti-interference ability and complex water quality applications. Through quenching experiments and EPR tests, it is confirmed that singlet oxygen (1O2) was the major reactive oxygen species (ROS) and 1O2 was converted from hydroxyl radical (·OH) adsorbed on the catalyst surface. This study provides an efficient catalyst for the application of Hetero-EF to remove organic compounds in complex water at circumneutral pH.

Ultrafine copper oxide nanoparticles immobilized on poly (4-vinylpyridine)-grafted UiO-66-NH2 as heterogeneous catalyst for oxidative homocoupling of terminal alkynes

Terminal alkyne homocoupling is an effective route to synthesize 1,3-diynes, which are crucial components of many fine chemicals and natural products. However, the reaction often faces challenges of catalyst recovery and typically necessitates the introduction of basic additives, which limits its practical applicability. Here, we have developed a green and efficient Cu2O@UiO-66-g-P4VP nanocatalyst that exhibits outstanding activity for homocoupling terminal alkynes under mild, base- or ligand-free conditions. The characterization results indicate that the nitrogen atoms in P4VP interfere with the electronic structure of Cu in Cu2O nanoparticles, causing the N electrons to shift onto Cu. Density functional theory (DFT) calculations suggest that this catalytic system facilitates the activation of oxygen on the copper surface, promoting the coupling reaction. This work provides a feasible strategy for the rational fabrication of MOF-supported polybase and Cu2O nanocrystals as heterogeneous nanocatalysts in the oxidative homocoupling of alkynes.

Water-Driven Surface Lattice Oxygen Activation in MnO2 for Promoted Low-Temperature NH3-SCR.

Water is ubiquitous in various heterogeneous catalytic reactions, where it can be easily adsorbed, chemically dissociated, and diffused on catalyst surfaces, inevitably influencing the catalytic process. However, the specific role of water in these reactions remains unclear. In this study, we innovatively propose that H2O-driven surface lattice oxygen activation in γ-MnO2 significantly enhances low-temperature NH3-SCR. The proton from water dissociation activates the surface lattice oxygen in γ-MnO2, giving rise to a doubling of catalytic activity (achieving 90% NO conversion at 100 °C) and remarkable stability. Comprehensive in situ characterizations and calculations reveal that spontaneous proton diffusion to the surface lattice oxygen reduces the orbital overlap between the protonated oxygen atom and its neighboring Mn atom. Consequently, the Mn-O bond is weakened and the surface lattice oxygen is effectively activated to provide excess oxygen vacancies available for converting O2 into O2-. Therefore, the redox property of Mn-H is improved, leading to enhanced NH3 oxidation-dehydrogenation and NO oxidation processes, which are crucial for low-temperature NH3-SCR. This work provides a deeper understanding and fresh perspectives on the water promotion mechanism in low-temperature NOx elimination.

Actinidia chinensis Planch Ameliorates Photoaging in UVB-Irradiated NIH-3T3 Cells and SKH-1 Hairless Mice by Controlling the Reactive Oxygen Species/AKT Pathway.

In this study, we evaluated the antiphotoaging properties of Actinidia chinensis Planch (ACP) and the molecular mechanisms underlying its ability to prevent UVB-mediated photoaging. Administration of the ethanolic extract of ACP (EEACP) to the dorsal area of hairless mice effectively ameliorated UVB-mediated wrinkle formation, epidermal thickening, and loss of lipid droplets in the epidermis. Additionally, the UVB-induced loss of collagen content in the epidermis was significantly attenuated in mouse skin treated with EEACP. The expression of procollagen type 1 and metalloproteinase-1a, which are related to collagen content in the epidermis, was restored by EEACP treatment in UVB-irradiated mice and NIH-3T3 mouse skin fibroblast cells. Interestingly, EEACP effectively ameliorated UVB-induced reactive oxygen species overproduction. Furthermore, the activation/phosphorylation of AKT, rather than mitogen-activated protein kinases, has been identified as a major target of EEACP in preventing UVB-mediated photoaging. Additionally, N-(1 deoxy-1-fructosyl) valine and phenethylamine glucuronide were identified as analytical indicators of EEACP using high-performance liquid chromatography/mass spectrometry. These results suggest that EEACP can be developed as a functional natural agent capable of preventing photoaging by attenuating UVB-induced activation of the reactive oxygen species/AKT pathway.

Periodic Trends and Fluxionality Effects on Transition Metal Catalyzed Sulfoxidation.

Despite the extended interest in d0 metal complexes as catalysts for peroxide activation and eventual oxygen transfer processes, there are still gaps in the understanding of how they proceed at the microscopic level. Herein, we have considered sulfide oxidation with cumyl hydroperoxide as a test system, performing the reaction with a series of eight different aminotriphenolate d0 metal complexes: Ti(IV), Zr(IV), Hf(IV), V(V), Nb(V), Ta(V), Mo(VI), and W(VI). The reactivity and selectivity of the catalytic systems, as well as the effect of a strong Lewis base (dimethylhexyl-N-oxide), have been determined experimentally, correlating kinetic values with Sanderson electronegativity values. Theoretical calculations of the catalytic cycles have been performed to have a clearer description of the role of the reactive peroxo species. Combining experimental results and DFT predictions, we propose suitable mechanisms for all eight metal aminotriphenolates, rationalizing the expected periodic trends, while also unveiling the unique reaction pathways available to highly flexible vanadium complexes.

Data-driven designed low Pt loading PtFeCoNiMnGa nano high entropy alloy with high catalytic activity for Zn-air batteries

Developing low Pt loading and high-activity oxygen electrocatalysts is necessary to promote large-scale fuel cell applications. By data-driven and density functional theory calculations, PtFeCoNiMnGa nano high entropy alloy (HEA) was synthesized through liquid-phase reduction and H2 calcination method and loaded on carbon nano-tube (CNT). Due to high entropy, electronic modulation, and cocktail effects, PtFeCoNiMnGa HEA catalyst shows great catalytic activity in oxygen evolution/reduction reaction (OER/ORR). The PtFeCoNiMnGa/CNT showed a low overpotential of 243 mV for OER, and for ORR a mass activity of 1.12 A mgPt−1 (5.3 times than Pt/C). Moreover, the PtFeCoNiMnGa/CNT showed high durability by maintaining 95 % of its initial performance for up to 50 h. In addition, the zinc-air battery assembled with PtFeCoNiMnGa/CNT as the cathode catalyst had an open-circuit potential of 1.52 V and an energy density of 130.6 mW cm−2, and was able to operate stably for 120 h without any significant degradation.

Synergistic enhancement of ion/electron transport by ultrafine nanoparticles and graphene in Li2FeTiO4/C/G nanofibers for symmetric Li-ion batteries

Low-cost Fe-based disordered rock salt (DRX) Li2FeTiO4 is capable of providing high capacity (295 mA h g−1) by redox activity of cations (Fe2+/Fe4+ and Ti3+/Ti4+) and anionic oxygen. However, DRX structures lack transport channels for ions and electrons, resulting in sluggish kinetics, poor electrochemical activity, and cyclability. Herein, graphene conductive carbon network permeated Li2FeTiO4 (LFT/C/G) nanofibers are successfully prepared by a facile sol-gel assisted electrospinning method. Ultrafine Li2FeTiO4 nanoparticles (2 nm) and one-dimensional (1D) structure provide abundant active sites and unobstructed diffusion channels, accelerating ion diffusion. In addition, introducing graphene reduces the band gap and Li+ diffusion barrier and improves the dynamic properties of Li2FeTiO4, thus achieving a relatively mild interfacial reaction and reversible redox reaction. As expected, the LFT/C/1.0G cathode delivers a remarkable discharge capacity (238.5 mA h g−1), high energy density (508.8 Wh kg−1), and excellent rate capability (51.2 mA h g−1 at 1.0 A g−1). Besides, the LFT/C/1.0G anode also displays a high capacity (514.5 mA h g−1 at 500 mA g−1) and a remarkable rate capability (243.9 mA h g−1 at 8 A g−1). Moreover, the full batteries based on the LFT/C/1.0G symmetric electrode demonstrate a reversible capacity of 117.0 mA h g−1 after 100 cycles at 50 mA g−1. This study presents useful insights into developing cost-effective DRX cathodes with durable and fast lithium storage.

Novel reduced heteropolyacid nanoparticles for effective treatment of drug-induced liver injury by manipulating reactive oxygen and nitrogen species and inflammatory signals

With the rapid advancements in biomedicine, the use of clinical drugs has surged sharply. However, potential hepatotoxicity limits drug exploitation and widespread usage, posing serious threats to patient health. Hepatotoxic drugs disrupt liver enzyme levels and cause refractory pathological damage, creating a challenge in the application of diverse first-line drugs. The activation and deterioration of reactive oxygen and nitrogen species (RONS) and inflammatory signals are key pathological mechanisms of drug-induced liver injury (DILI). Herein, a novel reduced heteropolyacid nanoparticle (RNP) has been developed, possessing high RONS-scavenging ability, strong anti-inflammatory activity, and excellent biosafety. These features enable it to swiftly restore the redox and immune balance of the liver. Intravenous administration of RNP effectively scavenged RONS storm, reversing liver oxidative stress and restoring normal mitochondrial membrane potential and function. Furthermore, by inhibiting c-Jun-N-terminal kinase phosphorylation, RNP facilitated the restoration of nuclear factor erythroid 2-related factor 2-mediated endogenous antioxidant signaling, ultimately rescuing the liver function and tissue morphology in acetaminophen-induced DILI mice. Crucially, the high biocompatible RNP exhibited superior efficacy in the DILI mouse model compared to the clinical antioxidant N-acetylcysteine. This targeted therapeutic approach, tailored to address the onset and progression of DILI, offers valuable new insights into controlling the condition and restoring liver structure and function.

Intensify Mass Transfer and Molecular Oxygen Activation by Defect‐Bridged Asymmetric Catalytic Sites Toward Efficient Membrane‐Based Nanoconfined Catalysis (Adv. Funct. Mater. 37/2024)

Intensify Mass Transfer and Molecular Oxygen Activation by Defect‐Bridged Asymmetric Catalytic Sites Toward Efficient Membrane‐Based Nanoconfined Catalysis (Adv. Funct. Mater. 37/2024)

Constructing novel metal-free HCOF-Ph@g-C3N4 heterojunctions through molecular expansion to enhance photogenerated carrier involved molecular oxygen activation and photocatalytic hydrogen evolution

Modification of covalent organic frameworks (COFs) have exceptional stability as well as tunable structures is the key to efficient photocatalysts. In this study, hyper-crosslinked COF-Ph was constructed with g-C3N4 to obtain a novel HCOF-Ph@g-C3N4 heterojunction, and the lamellar mesoporous of g-C3N4 was successfully embedded into the pores of 3D HCOF-Ph. The synthetic strategy greatly enhanced the photocatalytic properties and molecular oxygen activation capability of the catalyst. 10 mg of HCOF-Ph@g-C3N4 heterojunction could completely degrade 30 mg/L of tetracycline (TC) within 14 min, and the rate of hydrogen generation reached 9214.69 μmol g−1 h−1. The active species in this process of photocatalysis were verified through tests with free radical trapping and ESR spectra. In addition, the molecular oxygen activation capacity of heterojunction interface and the yield of superoxide radicals were examined by 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation and degradation of nitrotetrazolium nlue chloride (NBT) experiments, respectively. We found that the molecular expansion strategy can change molecule energy band structure to improve absorption of sunlight, and the efficient segregation of the photogenerated charge were ensured by the complementary energy band structure between g-C3N4 and HCOF-Ph. This study created an efficient molecular expansion method for the synthesis of COF-based catalysts with potential uses in the energy and environmental fields.

Selective oxidation of methane to C2+ products over Au-CeO2 by photon-phonon co-driven catalysis

Direct methane conversion to high-value chemicals under mild conditions is attractive yet challenging due to the inertness of methane and the high reactivity of valuable products. This work presents an efficient and selective strategy to achieve direct methane conversion through the oxidative coupling of methane over a visible-responsive Au-loaded CeO2 by photon-phonon co-driven catalysis. A record-high ethane yield of 755 μmol h−1 (15,100 μmol g−1 h−1) and selectivity of 93% are achieved under optimised reaction conditions, corresponding to an apparent quantum efficiency of 12% at 365 nm. Moreover, the high activity of the photocatalyst can be maintained for at least 120 h without noticeable decay. The pre-treatment of the catalyst at relatively high temperatures introduces oxygen vacancies, which improves oxygen adsorption and activation. Furthermore, Au, serving as a hole acceptor, facilitates charge separation, inhibits overoxidation and promotes the C-C coupling reaction. All these enhance photon efficiency and product yield.

Effect of modified Ca-Al adsorbents on heavy metal fixation during co-combustion of coal and coconut shells: Experiments and simulations

As an alternative fuel, bio-waste coconut shells have shown promise in reducing pollution during the co-combustion process. In this study, a novel metal-mineral adsorbent, Ca-Al (Ca5Al6O14), was prepared and physically (ultrasonic) and chemically (ethylene glycol) modified to enhance its adsorption properties. Thermal adsorption experiments investigated the effect of the adsorbents on the fixation of six heavy metals (HMs): Cr, Cu, Mn, Ni, Pb, and Zn. XRD, SEM, BET, and XPS were used to analyze the adsorbents and the adsorption mechanism was investigated by combining lattice oxygen concentration and Factsage simulation calculations. The ecological risk assessment of heavy metals was used to comprehensively evaluate the fixation effects of the three Ca-Al adsorbents at different additive levels. The results showed that the modification significantly changed the morphological characteristics and oxygen activity of the Ca-Al adsorbents, increased the lattice oxygen and chemisorbed oxygen concentration, and laid the foundation for promoting the chemisorption process in the fixation of heavy metals. In combination with the Er (environmental risk factors), adding all three adsorbents reduced Ri (Risk index). Among them, Ca-Al (EG) at 3% had the best effect on Ri. 3% Ca–Al (EG) reduced the Er value of Ni by 49.02%. 5% Ca–Al (EG) reduced the Er value of Cr by 86.01%. 5% Ca–Al (UM) had the best effect on Mn, with a reduction of 46.13%. The addition of 10% Ca–Al (UM) reduced Er of Ni by 50.43%. Considering the practical application in coal-fired power plants, Ca-Al(EG), which exhibits a higher fixation rate at small additions, is more suitable.

Oxidation of 2,5-bis(hydroxymethyl)furan to 2,5-furandicarboxylic acid with morphology-dependent Au/CeO2 catalysts

2,5-Furandicarboxylic acid (FDCA), a bio-based diacid with a rigid ring, has a similar structure to petroleum-based terephthalic acid. Its co-polyester with ethylene glycol has excellent performance in terms of thermal and mechanical properties. Herein, an Au/CeO2-rod catalyst with rich oxygen vacancies was developed to achieve the efficient oxidation of 2,5-bis(hydroxymethyl)furan (BHMF) to FDCA with a 92 % yield under mild conditions, with the addition of 4 equivalents of Na2CO3 at 80℃ under 2 MPa O2 for 6 h. The large specific surface area of CeO2-rod is beneficial for better dispersion of Au nanoparticles. Meanwhile, the high activity of Au/CeO2-rod can be attributed to that the rod-shaped CeO2 exposed more active (100) facets, resulting in strong metal-support interaction between Au nanoparticles and CeO2-rod. This could generate more Au species with oxidized state and more oxygen vacancies, thus promoting the reactant adsorption and oxygen activation and enhancing the final oxidation activity. The oxidation of 5-hydroxymethyl-2-furancarboxylic acid to FDCA was determined as the rate-determining step in the oxidation of BHMF over the Au/CeO2 catalyst.

Synergistic enhancement of singlet oxygen generation in Au and oxygen vacancy co-modified Bi2MoO6 ultrathin nanosheets for efficient ciprofloxacin degradation

Solar-driven molecular oxygen activation (MOA) is crucial for generating reactive oxygen species (ROS) for pollutant degradation, while the low activation efficiency greatly weakens the degradation efficiency. Herein, oxygen vacancies (OVs) and Au nanoparticles are co-introduced into Bi2MoO6 (ABMOH) to enhance the photocatalytic activity of Bi2MoO6 (BMO), thereby promoting MOA efficiency. Density functional theory demonstrates that the introduction of OVs not only improves the molecular oxygen adsorption on BMO, and but also strengthens the O-O bond dissociation of molecular oxygen, which is beneficial to MOA. Meanwhile, the unique localized surface plasmon resonance effect of Au nanoparticles immensely increases the photo-absorption capacity. Crucially, both OVs and Au nanoparticles work as “electron traps” to capture photogenerated electrons, thereby accelerating charge transfer. Based on the advantage of OVs and Au nanoparticles, ABMOH displays excellent MOA efficiency, and the degradation rate constant of ciprofloxacin (CIPF) by ABMOH-4 is 3.62-fold higher than BMO. Free radical trapping experiment and electron spin resonance suggest that singlet oxygen (1O2) can be selectively formed in the ABMOH system for CIPF degradation, and superoxide radical (•O2–) conversion and energy transfer are two pathways for 1O2 formation. This investigation serves as a beacon for the strategic design of high-performance and stable photocatalysts for MOA activation, paving the way for advancements in environmental remediation.

Rigid covalent organic frameworks with thiazole linkage to boost oxygen activation for photocatalytic water purification

Owing to their capability to produce reactive oxygen species (ROS) under solar irradiation, covalent organic frameworks (COFs) with pre-designable structure and unique architectures show great potentials for water purification. However, the sluggish charge separation, inefficient oxygen activation and poor structure stability in COFs restrict their practical applications to decontaminate water. Herein, via a facile one-pot synthetic strategy, we show the direct conversion of reversible imine linkage into rigid thiazole linkage can adjust the π-conjugation and local charge polarization of skeleton to boost the exciton dissociation on COFs. The rigid linkage can also improve the robustness of skeleton and the stability of COFs during the consecutive utilization process. More importantly, the thiazole linkage in COFs with optimal C 2p states (COF-S) effectively increases the activities of neighboring benzene unit to directly modulate the O2-adsorption energy barrier and improve the ROS production efficiency, resulting in the excellent photocatalytic degradation efficiency of seven toxic emerging contaminants (e.g. degrading ~99% of 5 mg L−1 paracetamol in only 7 min) and effective bacterial/algal inactivation performance. Besides, COF-S can be immobilized in continuous-flow reactor and in enlarged reactor to efficiently eliminate pollutants under natural sunlight irradiation, demonstrating the feasibility for practical application.