Boosting catalytic efficiency of nanostructured CuO-supported doped-CeO2 in oxidative coupling of benzyl amines to N-benzylidenebenzyl amines and benzimidazoles: impact of acidic and defect sites
This study presents the rational synthesis of Cu-supported doped-CeO2 catalysts designed for the oxidation of benzylamine, both in the absence and presence of 1,2-diaminobenzene. The catalysts were prepared using a two-step method and characterized by various techniques, including XRD, Raman spectro...
Saved in:
| Main Authors: | , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Frontiers Media S.A.
2025-01-01
|
| Series: | Frontiers in Nanotechnology |
| Subjects: | |
| Online Access: | https://www.frontiersin.org/articles/10.3389/fnano.2024.1513783/full |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1841527809359478784 |
|---|---|
| author | Sailatha Sakinala Naga Pranava Sree Kothoori Suman Jeedi Mohan Varkolu Mallesham Baithy |
| author_facet | Sailatha Sakinala Naga Pranava Sree Kothoori Suman Jeedi Mohan Varkolu Mallesham Baithy |
| author_sort | Sailatha Sakinala |
| collection | DOAJ |
| description | This study presents the rational synthesis of Cu-supported doped-CeO2 catalysts designed for the oxidation of benzylamine, both in the absence and presence of 1,2-diaminobenzene. The catalysts were prepared using a two-step method and characterized by various techniques, including XRD, Raman spectroscopy, BET surface area analysis, NH3-TPD, pyridine-FTIR, H2-TPR, XPS, SEM, and TEM. Raman and XPS analyses confirmed the presence of oxygen vacancy sites, with CuO/CeO2-ZrO2 displaying the highest concentration of these sites. H2-TPR revealed strong metal-support interactions, while NH3-TPD indicated that CuO/CeO2-ZrO2 possessed the greatest number of acidic sites. The pyridine-FTIR results indicates both the acidic sites present on the catalyst surface. The Cu/CeZr sample exhibits the lowest Iu////ITotal ratio (0.0567) compared to the Cu/Ce (0.0843) and Cu/CeSi (0.0672) samples, indicating a higher number of Ce3+ species or a greater number of oxygen defect sites in the sample. The catalyst demonstrated excellent performance in converting benzylamine to imines and was also highly effective in the synthesis of benzimidazole from benzylamine and 1,2-diaminobenzene, broadening its application potential. The superior catalytic activity is attributed to the abundant oxygen vacancies, redox properties, strong metal-support interactions, and acidic sites. Furthermore, the CuO/CeO2-ZrO2 catalyst maintained its efficiency over five consecutive cycles, exhibiting robustness, high functional group tolerance, and reduced reaction times, making it a promising system for diverse catalytic applications. |
| format | Article |
| id | doaj-art-2b23977038444f8e80538b21288d7dd2 |
| institution | Kabale University |
| issn | 2673-3013 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Frontiers Media S.A. |
| record_format | Article |
| series | Frontiers in Nanotechnology |
| spelling | doaj-art-2b23977038444f8e80538b21288d7dd22025-01-15T06:10:36ZengFrontiers Media S.A.Frontiers in Nanotechnology2673-30132025-01-01610.3389/fnano.2024.15137831513783Boosting catalytic efficiency of nanostructured CuO-supported doped-CeO2 in oxidative coupling of benzyl amines to N-benzylidenebenzyl amines and benzimidazoles: impact of acidic and defect sitesSailatha Sakinala0Naga Pranava Sree Kothoori1Suman Jeedi2Mohan Varkolu3Mallesham Baithy4Department of Chemistry, School of Science, Gandhi Institute of Technology and Management (GITAM), Hyderabad, IndiaDepartment of Chemistry, School of Science, Gandhi Institute of Technology and Management (GITAM), Hyderabad, IndiaDepartment of Chemistry, School of Science, Gandhi Institute of Technology and Management (GITAM), Hyderabad, IndiaDepartment of Chemistry, Koneru Lakshmaiah Education Foundation, Hyderabad, Telangana, IndiaDepartment of Chemistry, School of Science, Gandhi Institute of Technology and Management (GITAM), Hyderabad, IndiaThis study presents the rational synthesis of Cu-supported doped-CeO2 catalysts designed for the oxidation of benzylamine, both in the absence and presence of 1,2-diaminobenzene. The catalysts were prepared using a two-step method and characterized by various techniques, including XRD, Raman spectroscopy, BET surface area analysis, NH3-TPD, pyridine-FTIR, H2-TPR, XPS, SEM, and TEM. Raman and XPS analyses confirmed the presence of oxygen vacancy sites, with CuO/CeO2-ZrO2 displaying the highest concentration of these sites. H2-TPR revealed strong metal-support interactions, while NH3-TPD indicated that CuO/CeO2-ZrO2 possessed the greatest number of acidic sites. The pyridine-FTIR results indicates both the acidic sites present on the catalyst surface. The Cu/CeZr sample exhibits the lowest Iu////ITotal ratio (0.0567) compared to the Cu/Ce (0.0843) and Cu/CeSi (0.0672) samples, indicating a higher number of Ce3+ species or a greater number of oxygen defect sites in the sample. The catalyst demonstrated excellent performance in converting benzylamine to imines and was also highly effective in the synthesis of benzimidazole from benzylamine and 1,2-diaminobenzene, broadening its application potential. The superior catalytic activity is attributed to the abundant oxygen vacancies, redox properties, strong metal-support interactions, and acidic sites. Furthermore, the CuO/CeO2-ZrO2 catalyst maintained its efficiency over five consecutive cycles, exhibiting robustness, high functional group tolerance, and reduced reaction times, making it a promising system for diverse catalytic applications.https://www.frontiersin.org/articles/10.3389/fnano.2024.1513783/fullCu-supported catalystsdoped-CeO2benzylamine oxidationoxygen vacanciesbenzimidazole synthesisacidic sites and redox behavior |
| spellingShingle | Sailatha Sakinala Naga Pranava Sree Kothoori Suman Jeedi Mohan Varkolu Mallesham Baithy Boosting catalytic efficiency of nanostructured CuO-supported doped-CeO2 in oxidative coupling of benzyl amines to N-benzylidenebenzyl amines and benzimidazoles: impact of acidic and defect sites Frontiers in Nanotechnology Cu-supported catalysts doped-CeO2 benzylamine oxidation oxygen vacancies benzimidazole synthesis acidic sites and redox behavior |
| title | Boosting catalytic efficiency of nanostructured CuO-supported doped-CeO2 in oxidative coupling of benzyl amines to N-benzylidenebenzyl amines and benzimidazoles: impact of acidic and defect sites |
| title_full | Boosting catalytic efficiency of nanostructured CuO-supported doped-CeO2 in oxidative coupling of benzyl amines to N-benzylidenebenzyl amines and benzimidazoles: impact of acidic and defect sites |
| title_fullStr | Boosting catalytic efficiency of nanostructured CuO-supported doped-CeO2 in oxidative coupling of benzyl amines to N-benzylidenebenzyl amines and benzimidazoles: impact of acidic and defect sites |
| title_full_unstemmed | Boosting catalytic efficiency of nanostructured CuO-supported doped-CeO2 in oxidative coupling of benzyl amines to N-benzylidenebenzyl amines and benzimidazoles: impact of acidic and defect sites |
| title_short | Boosting catalytic efficiency of nanostructured CuO-supported doped-CeO2 in oxidative coupling of benzyl amines to N-benzylidenebenzyl amines and benzimidazoles: impact of acidic and defect sites |
| title_sort | boosting catalytic efficiency of nanostructured cuo supported doped ceo2 in oxidative coupling of benzyl amines to n benzylidenebenzyl amines and benzimidazoles impact of acidic and defect sites |
| topic | Cu-supported catalysts doped-CeO2 benzylamine oxidation oxygen vacancies benzimidazole synthesis acidic sites and redox behavior |
| url | https://www.frontiersin.org/articles/10.3389/fnano.2024.1513783/full |
| work_keys_str_mv | AT sailathasakinala boostingcatalyticefficiencyofnanostructuredcuosupporteddopedceo2inoxidativecouplingofbenzylaminestonbenzylidenebenzylaminesandbenzimidazolesimpactofacidicanddefectsites AT nagapranavasreekothoori boostingcatalyticefficiencyofnanostructuredcuosupporteddopedceo2inoxidativecouplingofbenzylaminestonbenzylidenebenzylaminesandbenzimidazolesimpactofacidicanddefectsites AT sumanjeedi boostingcatalyticefficiencyofnanostructuredcuosupporteddopedceo2inoxidativecouplingofbenzylaminestonbenzylidenebenzylaminesandbenzimidazolesimpactofacidicanddefectsites AT mohanvarkolu boostingcatalyticefficiencyofnanostructuredcuosupporteddopedceo2inoxidativecouplingofbenzylaminestonbenzylidenebenzylaminesandbenzimidazolesimpactofacidicanddefectsites AT malleshambaithy boostingcatalyticefficiencyofnanostructuredcuosupporteddopedceo2inoxidativecouplingofbenzylaminestonbenzylidenebenzylaminesandbenzimidazolesimpactofacidicanddefectsites |