Crystallographic Dependence of CO Activation on Cobalt Catalysts: HCP versus FCC
Identifying the structure sensitivity of catalysts in reactions, such as Fischer–Tropsch synthesis from CO and H2 over cobalt catalysts, is an important yet challenging issue in heterogeneous catalysis. Based on a first-principles kinetic study, we find for the first time that CO activation on hexag...
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| Published in | Journal of the American Chemical Society Vol. 135; no. 44; pp. 16284 - 16287 |
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| Main Authors | , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
06.11.2013
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0002-7863 1520-5126 1520-5126 |
| DOI | 10.1021/ja408521w |
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| Abstract | Identifying the structure sensitivity of catalysts in reactions, such as Fischer–Tropsch synthesis from CO and H2 over cobalt catalysts, is an important yet challenging issue in heterogeneous catalysis. Based on a first-principles kinetic study, we find for the first time that CO activation on hexagonal close-packed (HCP) Co not only has much higher intrinsic activity than that of face centered-cubic (FCC) Co but also prefers a different reaction route, i.e., direct dissociation with HCP Co but H-assisted dissociation on the FCC Co. The origin is identified from the formation of various denser yet favorable active sites on HCP Co not available for FCC Co, due to their distinct crystallographic structure and morphology. The great dependence of the activity on the crystallographic structure and morphology of the catalysts revealed here may open a new avenue for better, stable catalysts with maximum mass-specific reactivity. |
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| AbstractList | Identifying the structure sensitivity of catalysts in reactions, such as Fischer–Tropsch synthesis from CO and H₂ over cobalt catalysts, is an important yet challenging issue in heterogeneous catalysis. Based on a first-principles kinetic study, we find for the first time that CO activation on hexagonal close-packed (HCP) Co not only has much higher intrinsic activity than that of face centered-cubic (FCC) Co but also prefers a different reaction route, i.e., direct dissociation with HCP Co but H-assisted dissociation on the FCC Co. The origin is identified from the formation of various denser yet favorable active sites on HCP Co not available for FCC Co, due to their distinct crystallographic structure and morphology. The great dependence of the activity on the crystallographic structure and morphology of the catalysts revealed here may open a new avenue for better, stable catalysts with maximum mass-specific reactivity. Identifying the structure sensitivity of catalysts in reactions, such as Fischer-Tropsch synthesis from CO and H2 over cobalt catalysts, is an important yet challenging issue in heterogeneous catalysis. Based on a first-principles kinetic study, we find for the first time that CO activation on hexagonal close-packed (HCP) Co not only has much higher intrinsic activity than that of face centered-cubic (FCC) Co but also prefers a different reaction route, i.e., direct dissociation with HCP Co but H-assisted dissociation on the FCC Co. The origin is identified from the formation of various denser yet favorable active sites on HCP Co not available for FCC Co, due to their distinct crystallographic structure and morphology. The great dependence of the activity on the crystallographic structure and morphology of the catalysts revealed here may open a new avenue for better, stable catalysts with maximum mass-specific reactivity. Identifying the structure sensitivity of catalysts in reactions, such as Fischer-Tropsch synthesis from CO and H2 over cobalt catalysts, is an important yet challenging issue in heterogeneous catalysis. Based on a first-principles kinetic study, we find for the first time that CO activation on hexagonal close-packed (HCP) Co not only has much higher intrinsic activity than that of face centered-cubic (FCC) Co but also prefers a different reaction route, i.e., direct dissociation with HCP Co but H-assisted dissociation on the FCC Co. The origin is identified from the formation of various denser yet favorable active sites on HCP Co not available for FCC Co, due to their distinct crystallographic structure and morphology. The great dependence of the activity on the crystallographic structure and morphology of the catalysts revealed here may open a new avenue for better, stable catalysts with maximum mass-specific reactivity.Identifying the structure sensitivity of catalysts in reactions, such as Fischer-Tropsch synthesis from CO and H2 over cobalt catalysts, is an important yet challenging issue in heterogeneous catalysis. Based on a first-principles kinetic study, we find for the first time that CO activation on hexagonal close-packed (HCP) Co not only has much higher intrinsic activity than that of face centered-cubic (FCC) Co but also prefers a different reaction route, i.e., direct dissociation with HCP Co but H-assisted dissociation on the FCC Co. The origin is identified from the formation of various denser yet favorable active sites on HCP Co not available for FCC Co, due to their distinct crystallographic structure and morphology. The great dependence of the activity on the crystallographic structure and morphology of the catalysts revealed here may open a new avenue for better, stable catalysts with maximum mass-specific reactivity. |
| Author | Su, Hai-Yan Zhang, Bing-Yan Sun, Da-Peng Liu, Jin-Xun Li, Wei-Xue |
| AuthorAffiliation | State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academic of Sciences |
| AuthorAffiliation_xml | – name: State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics – name: Chinese Academic of Sciences |
| Author_xml | – sequence: 1 givenname: Jin-Xun surname: Liu fullname: Liu, Jin-Xun – sequence: 2 givenname: Hai-Yan surname: Su fullname: Su, Hai-Yan – sequence: 3 givenname: Da-Peng surname: Sun fullname: Sun, Da-Peng – sequence: 4 givenname: Bing-Yan surname: Zhang fullname: Zhang, Bing-Yan – sequence: 5 givenname: Wei-Xue surname: Li fullname: Li, Wei-Xue email: wxli@dicp.ac.cn |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/24147726$$D View this record in MEDLINE/PubMed |
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| Snippet | Identifying the structure sensitivity of catalysts in reactions, such as Fischer–Tropsch synthesis from CO and H2 over cobalt catalysts, is an important yet... Identifying the structure sensitivity of catalysts in reactions, such as Fischer-Tropsch synthesis from CO and H2 over cobalt catalysts, is an important yet... Identifying the structure sensitivity of catalysts in reactions, such as Fischer–Tropsch synthesis from CO and H₂ over cobalt catalysts, is an important yet... |
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| Title | Crystallographic Dependence of CO Activation on Cobalt Catalysts: HCP versus FCC |
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