Engineering oxygen vacancies and localized amorphous regions in CuO-ZnO separately boost catalytic reactivity and selectivity

Ji, Yongjun; Chen, Xiaoli; Liu, Shaomian; Xing, Liwen; Jiang, Xingyu; Zhang, Bin; Li, Huifang; Zhong, Ziyi; Wang, Ligen; Xu, Guangwen; Su, Fabing

doi:10.1007/s12274-022-4940-3

Cited by 9 publications

(3 citation statements)

References 48 publications

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“…Furthermore, the EPR spectra presented, in both qualitative and quantitative manners, that ball-milling treatment with sulfur powder addition significantly increased the concentration of vacancies, but only the ball-milling treatment accidentally suppressed the generation of vacancies (Figure k and Table S7). Previous studies illustrated that the high-speed ball milling treatment with the heteroatom addition could cause the generation of lattice distortion and vacancies, resulting in the coordinated unsaturated and unstable valence states. , It is still unavailable to directly distinguish between sulfur and oxygen vacancies, because their signals were both at g = 2.006 around via the EPR test. Hence, S–CuFe 2 O 4 /BC was prepared by using H 2 O 2 to fill the O V but reserve S V , , named SQ S–CuFe 2 O 4 /BC.…”

Section: Resultsmentioning

confidence: 99%

“…Previous studies illustrated that the high-speed ball milling treatment with the heteroatom addition could cause the generation of lattice distortion and vacancies, resulting in the coordinated unsaturated and unstable valence states. 22,23 It is still unavailable to directly distinguish between sulfur and oxygen vacancies, because their signals were both at g = 2.006 around via the EPR test. Hence, S−CuFe 2 O 4 /BC was prepared by using H 2 O 2 to fill the O V but reserve S V , 24,25 named SQ S−CuFe 2 O 4 /BC.…”

Section: Morphologies Of Prepared Catalyst Materials To Characterize ...mentioning

confidence: 99%

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Defect Engineering Boosted Peroxydisulfate Activation of Dual-Vacancy Cu–Fe Spinel Oxides for Soil Organics Decontamination

Zhao,

Zhang,

Xia

et al. 2024

ACS EST Eng.

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Oxygen-limited environments in a compact soil medium significantly restrict the charge transfer of catalysts to degrade organics, considerably reducing the catalytic performance. Defect engineering has been proposed to modulate electronic structures and enrich active sites of catalysts, but single vacancy defects are still insufficient to overcome the slow redox cycling between different valence states of metals. Herein, sulfur-doped CuFe2O4/biochar (S–CuFe2O4/BC) with oxygen and sulfur dual vacancies was synthesized for peroxydisulfate (PDS) activation. Experimental and theoretical analysis reveals that the S-doping treatment significantly raises the electron delocalization to enlarge FeOh–O covalency, thereby lowering the charge transfer energy to favor FeOh–PDS interaction with higher oxidants’ utilization efficiency. Consequently, more than 2-fold increase in the pseudo-first-order rate constant and longevity for organics degradation was demonstrated. The stronger capability of the selective adsorption-oxidation toward hydrophobic organic contaminants was also achieved. This work offers an insightful understanding for collaboratively stimulating the intrinsic activity of the catalyst for soil organics decontamination.

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Section: Resultsmentioning

confidence: 99%

Section: Morphologies Of Prepared Catalyst Materials To Characterize ...mentioning

confidence: 99%

Defect Engineering Boosted Peroxydisulfate Activation of Dual-Vacancy Cu–Fe Spinel Oxides for Soil Organics Decontamination

Zhao,

Zhang,

Xia

et al. 2024

ACS EST Eng.

View full text Add to dashboard Cite

show abstract

“…2k and Table S2). Previous studies illustrated that the high-speed ball milling treatment with the heteroatom addition could cause the generation of lattice distortion and vacancies, resulting in the coordinated unsaturated and unstable valence states 24,25 . It is still unavailable to directly distinguish between sulfur and oxygen vacancies, because their signals were both at g=2.006 around via the EPR test.…”

Section: Identification Of Coordination Structuresmentioning

confidence: 99%

Tuning Anion Defects in Cu-Fe Spinel Oxides by Sulfur Doping for Boosted Peroxydisulfate Activation

Zhao

Song²,

Liu³

et al. 2023

Preprint

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The bimetallic spinel oxides have broad application prospects in pollution control by advanced oxidation processes. However, despite extensive efforts, the available commercial catalysts for soil contaminant degradation still suffer from inferior activity, low selectivity and poor longevity. Herein, we proposed an efficient strategy for boosting the intrinsic activities of sulfur-doped CuFe2O4/BC by defect engineering of dual vacancies. It is experimentally demonstrated that both the pseudo first-order rate constant and longevity of the sulfur-doped CuFe2O4/BC+PDS system for organics degradation have been promoted twice. Moreover, this system exhibits strong selective adsorption-oxidation capability towards hydrophobic organic contaminants. Theoretical calculations revealed that the incorporation of S-doping into the system plays a substantial role in the regulation of interface energetics and the enhancement of Fe-O covalency. This effectively facilitates electron transfer between metal redox pairs, culminating in high PDS utilization efficiency. This work offers an insightful understanding for collaboratively stimulating the intrinsic activity of the catalyst for soil remediation.

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Synthesis of Oxygen Vacancy‐Enriched POM Heterostructure with Enhanced Metal–Support Interactions via Supercritical Anti‐Solvent Method for Ultratrace Cysteine Analysis

Xiong,

Li,

Chen

et al. 2024

Adv Funct Materials

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This study introduces a novel polyoxometalate (POM) heterostructure designed to address challenges in ultratrace analysis and sensor stability. Supercritical anti‐solvent and hydrothermal methods are employed to fabricate a composite that enhances stability, sensitivity, and selectivity for cysteine (Cys) detection. The optimization of inter‐component interactions and improved dispersibility contributes to superior stability and longevity. These preparation techniques increase the total oxygen vacancy density, which facilitates the migration of surface oxygen vacancies and promotes the electrocatalytic process. Additionally, tuning the band structure effectively suppresses electron–hole recombination, thereby enhancing catalytic capability. The integration of potassium phosphotungstate (KPW) as an electron transport mediator results in a stable “point‐surface” loading structure, increasing active sites and improving the material's specific surface area and catalytic efficiency. The Cu/Zr nanoparticle‐grafted KPW composite (CZPW) demonstrates excellent performance, achieving an ultratrace detection limit of 30.6 pM and a broad linear detection range from 50 pM to 1 mM. Overall, this study elucidates the mechanisms of supercritical preparation and its impact on electrocatalytic Cys reactions, providing valuable insights into the development of highly effective and stable biosensors.

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Engineering oxygen vacancies and localized amorphous regions in CuO-ZnO separately boost catalytic reactivity and selectivity

Cited by 9 publications

References 48 publications

Defect Engineering Boosted Peroxydisulfate Activation of Dual-Vacancy Cu–Fe Spinel Oxides for Soil Organics Decontamination

Defect Engineering Boosted Peroxydisulfate Activation of Dual-Vacancy Cu–Fe Spinel Oxides for Soil Organics Decontamination

Tuning Anion Defects in Cu-Fe Spinel Oxides by Sulfur Doping for Boosted Peroxydisulfate Activation

Synthesis of Oxygen Vacancy‐Enriched POM Heterostructure with Enhanced Metal–Support Interactions via Supercritical Anti‐Solvent Method for Ultratrace Cysteine Analysis

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