Excellent Performance and Feasible Mechanism of ErOx-Boosted MnOx-Modified Biochars Derived from Sewage Sludge and Rice Straw for Formaldehyde Elimination: In Situ DRIFTS and DFT
To avoid resource waste and environmental pollution, a chain of ErO<sub>x</sub>-boosted MnO<sub>x</sub>-modified biochars derived from rice straw and sewage sludge (Er<sub>y</sub>Mn<sub>1-y</sub>/BACs, where biochars derived from rice straw and sewage...
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MDPI AG
2023-08-01
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| Online Access: | https://www.mdpi.com/2073-4344/13/8/1222 |
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| author | Jiajie Wang Lei Gao Dong Xie Caiting Li Liping Xiang Yun Jiang Qing Xu Huiyu Xiong Lei Yi Jie Liu Jiajun Wu |
| author_facet | Jiajie Wang Lei Gao Dong Xie Caiting Li Liping Xiang Yun Jiang Qing Xu Huiyu Xiong Lei Yi Jie Liu Jiajun Wu |
| author_sort | Jiajie Wang |
| collection | DOAJ |
| description | To avoid resource waste and environmental pollution, a chain of ErO<sub>x</sub>-boosted MnO<sub>x</sub>-modified biochars derived from rice straw and sewage sludge (Er<sub>y</sub>Mn<sub>1-y</sub>/BACs, where biochars derived from rice straw and sewage sludge were defined as BACs) were manufactured for formaldehyde (HCHO) elimination. The optimal 15%Er<sub>0.5</sub>Mn<sub>0.5</sub>/BAC achieved a 97.2% HCHO removal efficiency at 220 °C and exhibited favorable E<sub>HCHO</sub> and thermal stability in a wide temperature window between 180 and 380 °C. The curbed influences of H<sub>2</sub>O and SO<sub>2</sub> offset the boosting effect of O<sub>2</sub> in a certain range. Er–Mn bimetallic-modified BACs offered a superior HCHO removal performance compared with that of BACs boosted using Er or Mn separately, owing to the synergistic effect of ErO<sub>x</sub> and MnO<sub>x</sub> conducive to improving the samples’ total pore volume and surface area, surface active oxygen species, promoting redox ability, and inhibiting the crystallization of MnO<sub>x</sub>. Moreover, the support’s hierarchical porous structure not only expedited the diffusion and mass transfer of reactants and their products but also elevated the approachability of adsorption and catalytic sites. Notably, these prominent features were partly responsible for the outstanding performance and excellent tolerance to H<sub>2</sub>O and SO<sub>2</sub>. Using in situ DRIFTS characterization analysis, it could be inferred that the removal process of HCHO was HCHO<sub>ad</sub> → dioxymethylene (DOM) → formate species → CO<sub>2</sub> + H<sub>2</sub>O, further enhanced with reactive oxygen species. The DFT calculation once again proved the removal process of HCHO and the strengthening effect of Er doping. Furthermore, the optimal catalytic performance of 15%Er<sub>0.5</sub>Mn<sub>0.5</sub>/BAC demonstrated its vast potential for practical applications. |
| first_indexed | 2024-03-11T00:03:11Z |
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| institution | Directory Open Access Journal |
| issn | 2073-4344 |
| language | English |
| last_indexed | 2024-03-11T00:03:11Z |
| publishDate | 2023-08-01 |
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| spelling | doaj.art-42065b57f33c4e1f958cbdd91ead80122023-11-19T00:36:01ZengMDPI AGCatalysts2073-43442023-08-01138122210.3390/catal13081222Excellent Performance and Feasible Mechanism of ErOx-Boosted MnOx-Modified Biochars Derived from Sewage Sludge and Rice Straw for Formaldehyde Elimination: In Situ DRIFTS and DFTJiajie Wang0Lei Gao1Dong Xie2Caiting Li3Liping Xiang4Yun Jiang5Qing Xu6Huiyu Xiong7Lei Yi8Jie Liu9Jiajun Wu10School of Reces Environment and Safety Engineering, University of South China, Hengyang 421001, ChinaSchool of Reces Environment and Safety Engineering, University of South China, Hengyang 421001, ChinaNational & Local Joint Engineering Research Center for Airborne Pollutants Control and Radioactivity Protection in Buildings, Hengyang 421001, ChinaCollege of Environmental Science and Engineering, Hunan University, Changsha 410082, ChinaNational & Local Joint Engineering Research Center for Airborne Pollutants Control and Radioactivity Protection in Buildings, Hengyang 421001, ChinaSchool of Reces Environment and Safety Engineering, University of South China, Hengyang 421001, ChinaSchool of Reces Environment and Safety Engineering, University of South China, Hengyang 421001, ChinaSchool of Reces Environment and Safety Engineering, University of South China, Hengyang 421001, ChinaSchool of Reces Environment and Safety Engineering, University of South China, Hengyang 421001, ChinaSchool of Reces Environment and Safety Engineering, University of South China, Hengyang 421001, ChinaSchool of Reces Environment and Safety Engineering, University of South China, Hengyang 421001, ChinaTo avoid resource waste and environmental pollution, a chain of ErO<sub>x</sub>-boosted MnO<sub>x</sub>-modified biochars derived from rice straw and sewage sludge (Er<sub>y</sub>Mn<sub>1-y</sub>/BACs, where biochars derived from rice straw and sewage sludge were defined as BACs) were manufactured for formaldehyde (HCHO) elimination. The optimal 15%Er<sub>0.5</sub>Mn<sub>0.5</sub>/BAC achieved a 97.2% HCHO removal efficiency at 220 °C and exhibited favorable E<sub>HCHO</sub> and thermal stability in a wide temperature window between 180 and 380 °C. The curbed influences of H<sub>2</sub>O and SO<sub>2</sub> offset the boosting effect of O<sub>2</sub> in a certain range. Er–Mn bimetallic-modified BACs offered a superior HCHO removal performance compared with that of BACs boosted using Er or Mn separately, owing to the synergistic effect of ErO<sub>x</sub> and MnO<sub>x</sub> conducive to improving the samples’ total pore volume and surface area, surface active oxygen species, promoting redox ability, and inhibiting the crystallization of MnO<sub>x</sub>. Moreover, the support’s hierarchical porous structure not only expedited the diffusion and mass transfer of reactants and their products but also elevated the approachability of adsorption and catalytic sites. Notably, these prominent features were partly responsible for the outstanding performance and excellent tolerance to H<sub>2</sub>O and SO<sub>2</sub>. Using in situ DRIFTS characterization analysis, it could be inferred that the removal process of HCHO was HCHO<sub>ad</sub> → dioxymethylene (DOM) → formate species → CO<sub>2</sub> + H<sub>2</sub>O, further enhanced with reactive oxygen species. The DFT calculation once again proved the removal process of HCHO and the strengthening effect of Er doping. Furthermore, the optimal catalytic performance of 15%Er<sub>0.5</sub>Mn<sub>0.5</sub>/BAC demonstrated its vast potential for practical applications.https://www.mdpi.com/2073-4344/13/8/1222HCHOcatalytic oxidationEr–Mn oxidesdensity-functional theoryhierarchical porous biochar |
| spellingShingle | Jiajie Wang Lei Gao Dong Xie Caiting Li Liping Xiang Yun Jiang Qing Xu Huiyu Xiong Lei Yi Jie Liu Jiajun Wu Excellent Performance and Feasible Mechanism of ErOx-Boosted MnOx-Modified Biochars Derived from Sewage Sludge and Rice Straw for Formaldehyde Elimination: In Situ DRIFTS and DFT Catalysts HCHO catalytic oxidation Er–Mn oxides density-functional theory hierarchical porous biochar |
| title | Excellent Performance and Feasible Mechanism of ErOx-Boosted MnOx-Modified Biochars Derived from Sewage Sludge and Rice Straw for Formaldehyde Elimination: In Situ DRIFTS and DFT |
| title_full | Excellent Performance and Feasible Mechanism of ErOx-Boosted MnOx-Modified Biochars Derived from Sewage Sludge and Rice Straw for Formaldehyde Elimination: In Situ DRIFTS and DFT |
| title_fullStr | Excellent Performance and Feasible Mechanism of ErOx-Boosted MnOx-Modified Biochars Derived from Sewage Sludge and Rice Straw for Formaldehyde Elimination: In Situ DRIFTS and DFT |
| title_full_unstemmed | Excellent Performance and Feasible Mechanism of ErOx-Boosted MnOx-Modified Biochars Derived from Sewage Sludge and Rice Straw for Formaldehyde Elimination: In Situ DRIFTS and DFT |
| title_short | Excellent Performance and Feasible Mechanism of ErOx-Boosted MnOx-Modified Biochars Derived from Sewage Sludge and Rice Straw for Formaldehyde Elimination: In Situ DRIFTS and DFT |
| title_sort | excellent performance and feasible mechanism of erox boosted mnox modified biochars derived from sewage sludge and rice straw for formaldehyde elimination in situ drifts and dft |
| topic | HCHO catalytic oxidation Er–Mn oxides density-functional theory hierarchical porous biochar |
| url | https://www.mdpi.com/2073-4344/13/8/1222 |
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