Cation Substitution Induced d‐Band Center Modulation on Cobalt‐Based Spinel Oxides for Catalytic Ozonation
Co 3 O 4 spinel is a promising transition metal oxide (TMO) catalyst for the catalytic ozonation of volatile organic compounds (VOCs). Herein, metal–organic frameworks (MOFs)‐derived Ni‐ and Mg‐ substituted Co 3 O 4 catalysts retain similar spinel structures, but display improved and reduced ozonati...
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| Published in | Advanced functional materials Vol. 33; no. 44 |
|---|---|
| Main Authors | , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Hoboken
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25.10.2023
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| Subjects | |
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| Abstract | Co
3
O
4
spinel is a promising transition metal oxide (TMO) catalyst for the catalytic ozonation of volatile organic compounds (VOCs). Herein, metal–organic frameworks (MOFs)‐derived Ni‐ and Mg‐ substituted Co
3
O
4
catalysts retain similar spinel structures, but display improved and reduced ozonation performance of methyl mercaptan (CH
3
SH), respectively. Remarkably, the NiCo
2
O
4
catalyst can still ≈90% removal of CH
3
SH after running for 20 h at room temperature under an initial concentration of 50 ppm CH
3
SH and 40 ppm O
3
, relative humidity of 60%, and space velocity of 300 000 mL h
−1
g
−1
, exceeding the reported values. Experimental characterizations have unveiled that the substitution of Ni and Mg into the Co
3
O
4
spinel altered surface acidity, oxygen species mobility, and Co
2+
/Co
3+
ratio. The in situ Raman spectra reveal the dynamic formation Co(III)‐O
ad
* via the transformation of O
3
into surface atomic oxygen (O
ad
*) and peroxide species (O
2
*). Theoretical calculations verify that Ni‐substitution increases nonuniform charges and Fermi density, leading to a moderate increase in d‐band center energy levels, thereby promoting O
3
specific adsorption/activation to convert O
ad
*/O
2
* and •OH/
1
O
2
/•O
2
−
, which contributes to eliminate CH
3
SH and prevent poisoning. The concept of tuning the d‐band center can provide valuable insights for the design of other catalysts for catalytic ozonation. |
|---|---|
| AbstractList | Co3O4 spinel is a promising transition metal oxide (TMO) catalyst for the catalytic ozonation of volatile organic compounds (VOCs). Herein, metal–organic frameworks (MOFs)‐derived Ni‐ and Mg‐ substituted Co3O4 catalysts retain similar spinel structures, but display improved and reduced ozonation performance of methyl mercaptan (CH3SH), respectively. Remarkably, the NiCo2O4 catalyst can still ≈90% removal of CH3SH after running for 20 h at room temperature under an initial concentration of 50 ppm CH3SH and 40 ppm O3, relative humidity of 60%, and space velocity of 300 000 mL h−1 g−1, exceeding the reported values. Experimental characterizations have unveiled that the substitution of Ni and Mg into the Co3O4 spinel altered surface acidity, oxygen species mobility, and Co2+/Co3+ ratio. The in situ Raman spectra reveal the dynamic formation Co(III)‐Oad* via the transformation of O3 into surface atomic oxygen (Oad*) and peroxide species (O2*). Theoretical calculations verify that Ni‐substitution increases nonuniform charges and Fermi density, leading to a moderate increase in d‐band center energy levels, thereby promoting O3 specific adsorption/activation to convert Oad*/O2* and •OH/1O2/•O2−, which contributes to eliminate CH3SH and prevent poisoning. The concept of tuning the d‐band center can provide valuable insights for the design of other catalysts for catalytic ozonation. Co 3 O 4 spinel is a promising transition metal oxide (TMO) catalyst for the catalytic ozonation of volatile organic compounds (VOCs). Herein, metal–organic frameworks (MOFs)‐derived Ni‐ and Mg‐ substituted Co 3 O 4 catalysts retain similar spinel structures, but display improved and reduced ozonation performance of methyl mercaptan (CH 3 SH), respectively. Remarkably, the NiCo 2 O 4 catalyst can still ≈90% removal of CH 3 SH after running for 20 h at room temperature under an initial concentration of 50 ppm CH 3 SH and 40 ppm O 3 , relative humidity of 60%, and space velocity of 300 000 mL h −1 g −1 , exceeding the reported values. Experimental characterizations have unveiled that the substitution of Ni and Mg into the Co 3 O 4 spinel altered surface acidity, oxygen species mobility, and Co 2+ /Co 3+ ratio. The in situ Raman spectra reveal the dynamic formation Co(III)‐O ad * via the transformation of O 3 into surface atomic oxygen (O ad *) and peroxide species (O 2 *). Theoretical calculations verify that Ni‐substitution increases nonuniform charges and Fermi density, leading to a moderate increase in d‐band center energy levels, thereby promoting O 3 specific adsorption/activation to convert O ad */O 2 * and •OH/ 1 O 2 /•O 2 − , which contributes to eliminate CH 3 SH and prevent poisoning. The concept of tuning the d‐band center can provide valuable insights for the design of other catalysts for catalytic ozonation. |
| Author | Fang, Jingyun Shu, Dong Tang, Zhuoyun Qu, Wei Tang, Su He, Chun Wen, Hailin Lian, Qiyu |
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spinel is a promising transition metal oxide (TMO) catalyst for the catalytic ozonation of volatile organic compounds (VOCs). Herein, metal–organic... Co3O4 spinel is a promising transition metal oxide (TMO) catalyst for the catalytic ozonation of volatile organic compounds (VOCs). Herein, metal–organic... |
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| SubjectTerms | Atomic oxygen Catalysts Cobalt oxides Energy levels Materials science Metal-organic frameworks Nickel Poisoning (reaction inhibition) Raman spectra Relative humidity Room temperature Spinel Substitutes Transition metal oxides VOCs Volatile organic compounds |
| Title | Cation Substitution Induced d‐Band Center Modulation on Cobalt‐Based Spinel Oxides for Catalytic Ozonation |
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