Understanding the catalytic ozonation process on ceria nanorods: Efficacy, Frenkel-type oxygen vacancy as a key descriptor and mechanism insight

Lei, Wu; Wang, Jiaren; Yang, Chenyu; Gao, Xingmin; Fang, Yan; Wang, Xiaoning; Wu, Wenjun; Wu, Zhangxiong

doi:10.1016/j.apcatb.2022.122152

Cited by 23 publications

(10 citation statements)

References 65 publications

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“…26 Additionally, CuBO 2 featured two types of −OH groups: bridged (−OH) in the range of 3625−3662 cm −1 and multicoordinated (−OH) in the range of 3300−3500 cm −1 . 27 N 2 adsorption/desorption isotherms of CuBO 2 (B = Cr, Co, Mn, and Fe) were all type IV curves (Figure 1e), and the Brunauer−Emmett−Teller (BET) specific surface area were 47.41, 6.01, 11.96, and 0.97 m 2 •g −1 , respectively (Table S2). When P/P 0 is in the range of 0.4−1.0, a hysteresis loop similar to H3 type could be observed.…”

Section: Resultsmentioning

confidence: 99%

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Regulating B-Site Metals in Delafossite to Reach Efficient and Selective Peroxymonosulfate Activation for Water Remediation

Zhao,

Song,

Zhang

et al. 2023

ACS EST Eng.

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Transition metals (TMs) are excellent active sites to activate peroxymonosulfate (PMS) for water remediation; however, the factors determining the efficiency and selectivity of PMS activation over different TMs remain blurred. Herein, delafossite with different B-site metals (denoted as CuBO 2 , B = Mn, Fe, Co, Cr) was synthesized to activate PMS for Orange I (OI) degradation. Their catalytic activity order followed CuCrO 2 (91.5%) ≈ CuCoO 2 (91.2%) > CuMnO 2 (46.9%) > CuFeO 2 (27.9%); especially the degradation rate (k) of CuCrO 2 (CuCoO 2 ) was 14.0 (12.6)-fold and 30.0 (27.1)-fold higher than that of CuMnO 2 > CuFeO 2 , respectively. Mechanism analysis showed that sulfate radical (SO 4•− ) was the main oxidant responsible for OI degradation in the CuCoO 2 /PMS system, while CuCrO 2 interacted with PMS to execute an electron transfer pathway (ETP) for degrading OI. Experimental and density functional theory calculation results deciphered that the d-band centers of CuCoO 2 (E d = −1.22 eV) and CuCrO 2 (E d = 0.62 eV) were closest to the Fermi level (E F ), thereby facilitating the interfacial electron transfer process and enhancing the PMS activation efficiency. Moreover, it was important to note that the E d value of CuCoO 2 was located below the E F , which led CuCoO 2 to easily lose electrons to PMS, thereby generating sulfate radicals SO 4•− . On the other hand, the E d value of CuCrO 2 was situated above the E F , which facilitated the catalyst to obtain electrons, acting as electron shuttles and driving a nonradical ETP. Finally, the established CuBO 2 -activated PMS systems also exhibited excellent stability and robust resistance against coexisting substances. These findings provided an alternative perspective to understanding the inherent nature of TM-based catalysts for regulating the efficiency and selectivity of PMS activation in water remediation.

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Section: Resultsmentioning

confidence: 99%

“…Furthermore, bands at approximately 725 cm –1 were identified as Mn–O wagging vibrations . Additionally, CuBO 2 featured two types of –OH groups: bridged (−OH) in the range of 3625–3662 cm –1 and multicoordinated (−OH) in the range of 3300–3500 cm –1 …”

Section: Resultsmentioning

confidence: 99%

Regulating B-Site Metals in Delafossite to Reach Efficient and Selective Peroxymonosulfate Activation for Water Remediation

Zhao,

Song,

Zhang

et al. 2023

ACS EST Eng.

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“…[28] After the reaction with PMS, the peak of Ce 3 + shifted to the direction of higher binding energy (about 0.8 eV), and the content of Ce 3 + /Ce 4 + was slightly lower (Figure 3c), indicating that the increase of Ce oxidation state was caused by electron loss during the reaction. [29] Moreover, the XPS spectrum of Co 2p determined that Co exists in CoÀ CVO in the form of Co 2 + and Co 3 + , and the content of Co is low. After reacting with PMS, the content of Co 3 + in CoÀ CVO decreases, while the content of Co 2 + increases (Figure 3d), indicating that Co may have obtained electrons during the reaction process.…”

Section: Methodsmentioning

confidence: 99%

Efficient Removal of Antibiotic Resistance Genes through 4f‐2p‐3d Gradient Orbital Coupling Mediated Fenton‐Like Redox Processes

Li,

Wang,

Zhang

et al. 2023

Angew Chem Int Ed

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Peroxymonosulfate (PMS) mediated radical and nonradical active substances can synergistically achieve the efficient elimination of antibiotic resistance genes (ARGs). However, enhancing interface electron cycling and optimizing the coupling of the oxygen‐containing intermediates to improve PMS activation kinetics remains a major challenge. Here, Co doped CeVO4 catalyst (Co‐CVO) with asymmetric sites was constructed based on Ce 4f‐O 2p‐Co 3d gradient orbital coupling. The catalyst achieved approximately 2.51×105 copies/mL of extracellular ARGs (eARGs) removal within 15 minutes, exhibited ultrahigh degradation rate (k = 1.24 min‐1). The effective gradient 4f‐2p‐3d orbital coupling precisely regulates the electron distribution of Ce‐O‐Co active center microenvironment, while optimizing the electronic structure of Co 3d states (especially the occupancy of eg), promoting the adsorption of oxygen‐containing intermediates. The generated radical and nonradical generated by interfacial electron cycling enhanced by the reduction reaction of PMS at the Ce site and the oxidation reaction at the Co site achieved a significant mineralization rate of ARGs (83.4%). The efficient removal of ARGs by a continuous flow reactor for 10 hours significantly reduces the ecological risk of ARGs in actual wastewater treatment.

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“…Furthermore, it possesses abundant oxygen vacancies (OV), which often favor the formation of ROS. L. Wu et al 26 showed that the formation of two neighboring Ce 3+ is possible due to the absence of an oxygen atom from the CeO 2 lattice, generating Frenkel-type OV (movement of the oxygen atom from the lattice site to an interstitial site), and this was the critical descriptor of ozone decomposition. Therefore, it is expected that NiO and CeO 2 films can provide excellent catalytic activity towards pollutant removal in the presence of ozone.…”

Section: Introductionmentioning

confidence: 99%

Efficient catalytic activity of NiO and CeO₂ films in benzoic acid removal using ozone

Franco Peláez,

Rodríguez S.,

Poznyak

et al. 2024

RSC Adv.

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Understanding the catalytic ozonation process on ceria nanorods: Efficacy, Frenkel-type oxygen vacancy as a key descriptor and mechanism insight

Cited by 23 publications

References 65 publications

Regulating B-Site Metals in Delafossite to Reach Efficient and Selective Peroxymonosulfate Activation for Water Remediation

Regulating B-Site Metals in Delafossite to Reach Efficient and Selective Peroxymonosulfate Activation for Water Remediation

Efficient Removal of Antibiotic Resistance Genes through 4f‐2p‐3d Gradient Orbital Coupling Mediated Fenton‐Like Redox Processes

Efficient catalytic activity of NiO and CeO₂ films in benzoic acid removal using ozone

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Understanding the catalytic ozonation process on ceria nanorods: Efficacy, Frenkel-type oxygen vacancy as a key descriptor and mechanism insight

Cited by 23 publications

References 65 publications

Regulating B-Site Metals in Delafossite to Reach Efficient and Selective Peroxymonosulfate Activation for Water Remediation

Regulating B-Site Metals in Delafossite to Reach Efficient and Selective Peroxymonosulfate Activation for Water Remediation

Efficient Removal of Antibiotic Resistance Genes through 4f‐2p‐3d Gradient Orbital Coupling Mediated Fenton‐Like Redox Processes

Efficient catalytic activity of NiO and CeO2 films in benzoic acid removal using ozone

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Efficient catalytic activity of NiO and CeO₂ films in benzoic acid removal using ozone