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• The Fenton-like Cu-PAN 3 catalysts is first synthesized by co-precipitation and carbon thermal reduction method. • Dual reaction centers are constructed around graphene-like carbon and Cu species. • The pollutants as electron donors inhibit the ineffective decomposition of H 2 O 2 at the electron-poor centers. • The pollutant removal mainly relies on the surface cleavage at the electron-poor centers. High energy consumption has seriously hindered the development of Fenton-like reactions for the removal of refractory organic pollutants in water. To solve this problem, we designed a novel Fenton-like catalyst (Cu-PAN 3) by coprecipitation and carbon thermal reduction. The catalyst exhibits excellent Fenton-like catalytic activity and stability for the degradation of various pollutants with low H 2 O 2 consumption. The experimental results indicate that the dual reaction centers (DRCs) are composed of Cu-N-C and Cu-O-C bridges between copper and graphene-like carbon, which form electron-poor/rich centers on the catalyst surface. H 2 O 2 is mainly reduced at electron-rich Cu centers to free radicals for pollutant degradation. Meanwhile, pollutants can be oxidized by donating electrons to the electron-poor C centers of the catalyst, which inhibits the ineffective decomposition of H 2 O 2 at the electron-poor centers. This therefore significantly reduces the consumption of H 2 O 2 and reduces energy consumption. [Display omitted] [ABSTRACT FROM AUTHOR]

Excessive consumption of energy and resources is a major challenge in wastewater treatment. Here, a novel heterogeneous Fenton-like catalyst consisting of Cu-doped graphene-like catalysts (Cu-GCD NSs) was first synthesized by an enhanced carbothermal reduction of β-cyclodextrin (β-CD). The catalyst exhibits excellent Fenton-like catalytic activity for the degradation of various pollutants under neutral conditions, accompanied by low H 2 O 2 consumption. The results of structural characterization and theoretical calculations confirmed that the dual reaction centers (DRCs) were constructed on Cu-GCD NSs surface through C-O-Cu bonds supported on zero-valent copper species, which play a significant role in the high-performance Fenton-like reaction. The pollutants that served as electron donors were decomposed in the electron-poor carbon centers, whereas H 2 O 2 and dissolved oxygen obtained these electrons in the electron-rich Cu centers through C-O-Cu bonds, thereby producing more active species. This study demonstrates that the electrons of pollutants can be efficiently utilized in Fenton-like reactions by DRCs on the catalyst surface, which provides an effective strategy to improve Fenton-like reactivity and reduce H 2 O 2 consumption. [Display omitted] [ABSTRACT FROM AUTHOR]

• Mesoporous reduction state cobalt species-doped silica nanospheres are first prepared. • Excellent activity is realized in mp -RSCo-SiO 2 NSs/H 2 O 2 system. • Efficient dual-pathway degradation of pollutant is achieved in Fenton-like process. • Pollutants replace H 2 O 2 as electron donors for the mp -RSCo-SiO 2 NSs system. • A new interfacial Fenton-like reaction mechanism involving pollutants is proposed. A novel heterogeneous Co-containing Fenton-like catalyst consisting of mesoporous reduction state cobalt (RSCo)-doped silica (SiO 2) nanospheres (mp -RSCo-SiO 2 NSs) was prepared by an enhanced hydrothermal process. The catalyst exhibited very high activity and stability for a series of refractory pollutant degradation in a very wide pH range of 3.1–10.9. The Fenton-like reaction rate constant of this Co-containing catalyst was approximately 290 times higher than that of Co 3 O 4 for pollutant degradation under the neutral and mild conditions. Based on the characterization, the catalyst possessed a porous nanosphere morphology, and the reduction state cobalt species, including nano-zero-valent cobalt (nZVCo) and Co2+, were found to be generated in the SiO 2 framework through forming Co O Si bonds. During the Fenton-like reaction, the electron donation effect of organic pollutants was successfully realized through the interaction of "Pollutants → Co2+/0-SiO 2 ". The obtained electrons from pollutants were transferred to the catalyst surface and captured by H 2 O 2 , resulting in the generation of hydroxyl radicals (OH). Therefore, a dual-pathway degradation of the pollutants was realized: (I) oxidation and degradation as the electron donors for the system and (II) attacking and destruction by OH radicals. This work provided a new perspective on the effective utilization of the electrons of pollutants and the improvement of Fenton reaction efficiency. [ABSTRACT FROM AUTHOR]

Single-atom Fe catalysis has exhibited remarkable potentials in water treatment applications. However, rational design of single-atom Fe catalysts with controlled catalytic performance is still challenging, due to the lack of the fundamental understanding on the corelated factors of structure, property, and catalytic behavior. Herein, PMS activation performance of the single-atom Fe sites is successfully boosted by molecular-engineering on the polymeric carbon nitride (CN) framework. Benzene-1,4-diamine regulates the polymerization process, and rises the ratio of carbon/nitrogen; the valence of the single-atom Fe is thereby positively shifted, leading to favorable thermal dynamics of the high-valent Fe(IV)=O involved oxidation reaction. The carbon-rich CN supported single-atom Fe catalyst thus exhibits remarkable performance in selective degradation of a series of organic pollutants via high-valent Fe(IV)=O oxidation pathway. The findings in this work implicate the significance of electronic properties of the support as one of the essential descriptors for a robust single-atom catalyst for pollutants abatement. [Display omitted] • Benzene diamine in precursor for synthesis of single-atom Fe catalyst could positively shift the valence of Fe center. • A 5.1 times of performance improvement in bisphenol A degradation reaction was realized. • The single atom Fe catalyst with optimized valence is durable in a fixed-bed reactor. • Theoretical simulation states that positive valence of Fe center lowered the energy barrier of the catalytic reaction. [ABSTRACT FROM AUTHOR]

• Heterogeneous Fenton-like reaction was studied using a pilot scale test. • TCM, DCAA and TCAA were the main compositions of DBPs in drinking water. • C1-C5 and F1-F5 of NOM were the main precursors of different DBPs. • This treatment improved removal efficiency of DBPs and NOM without adjusting pH. • This treatment process also controlled the genotoxicity of drinking water. This paper explores the removal of natural organic matter (NOM) and disinfection by-products (DBPs) in drinking water by heterogeneous Fenton-like oxidation and granular activated carbon (GAC) filtration in a pilot scale test without adjusting pH of the water. pH of the used water in this study was from 7.5 to 8.7. Comparing with conventional water treatment processes, heterogeneous Fenton-like reaction and GAC filtration increased the removal rate of dissolved organic carbon (DOC), NOM with different apparent molecular weight (AMW) (F1-F7) and with different compositions (C1-C5) to 75.11%, 88.65% and 58.73%, respectively. Moreover, heterogeneous Fenton-like reaction and GAC filtration increased the removal rate of DBPs to 88.18%. The multivariate statistical analysis indicated that haloacetic acids (HAAs) and haloketones (HKs) mainly came from fulvic-like and humic-like NOM with AMW lower than 1.5 K Da. These substances with AMW between 1.5 K Da and 3.5 K Da were the main precursors of trihalomethanes (THMs). The main precursors of halonitriles (HANs) were soluble microbial byproduct-like (SMP-like), tyrosine-like and tryptophan-like substance with the AMW between 3.5 K Da and 4.5 K Da. Overall, without adjusting pH of water, heterogeneous Fenton-like reaction and GAC filtration improved the removal efficiency of NOM and DBPs, and controlled the genotoxicity of drinking water. [ABSTRACT FROM AUTHOR]