First-Principles Investigation of CO Adsorption on h-Fe<sub>7</sub>C<sub>3</sub> Catalyst
h-Fe<sub>7</sub>C<sub>3</sub> is considered as the main active phase of medium-temperature Fe-based Fischer–Tropsch catalysts. Basic theoretical guidance for the design and preparation of Fe-based Fischer–Tropsch catalysts can be obtained by studying the adsorption and activa...
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| Format: | Article |
| Language: | English |
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MDPI AG
2020-07-01
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| Series: | Crystals |
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| Online Access: | https://www.mdpi.com/2073-4352/10/8/635 |
| _version_ | 1827712521336782848 |
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| author | Jinzhe Fu Deshuai Sun Zhaojun Chen Jian Zhang Hui Du |
| author_facet | Jinzhe Fu Deshuai Sun Zhaojun Chen Jian Zhang Hui Du |
| author_sort | Jinzhe Fu |
| collection | DOAJ |
| description | h-Fe<sub>7</sub>C<sub>3</sub> is considered as the main active phase of medium-temperature Fe-based Fischer–Tropsch catalysts. Basic theoretical guidance for the design and preparation of Fe-based Fischer–Tropsch catalysts can be obtained by studying the adsorption and activation behavior of CO on h-Fe<sub>7</sub>C<sub>3</sub>. In this paper, the first-principles method based on density functional theory is used to study the crystal structure properties of h-Fe<sub>7</sub>C<sub>3</sub> and the adsorption and activation CO on its low Miller index surfaces <inline-formula> <math display="inline"> <semantics> <mrow> <mrow> <mo>(</mo> <mrow> <mn>1</mn> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> <mn>0</mn> </mrow> <mo>)</mo> </mrow> <mo>,</mo> <mrow> <mo>(</mo> <mrow> <mn>1</mn> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> <mn>1</mn> </mrow> <mo>)</mo> </mrow> <mo>,</mo> <mrow> <mo>(</mo> <mrow> <mn>101</mn> </mrow> <mo>)</mo> </mrow> <mo>,</mo> <mrow> <mo>(</mo> <mrow> <mn>1</mn> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> </mrow> <mo>)</mo> </mrow> </mrow> </semantics> </math> </inline-formula> and <inline-formula> <math display="inline"> <semantics> <mrow> <mrow> <mo>(</mo> <mrow> <mn>001</mn> </mrow> <mo>)</mo> </mrow> </mrow> </semantics> </math> </inline-formula>. It was found that the low Miller index crystal plane of h-Fe<sub>7</sub>C<sub>3</sub> crystal has multiple equivalent crystal planes and that the maximum adsorption energy of CO at the 3F2 point of the <inline-formula> <math display="inline"> <semantics> <mrow> <mrow> <mo>(</mo> <mrow> <mn>1</mn> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> <mn>1</mn> </mrow> <mo>)</mo> </mrow> </mrow> </semantics> </math> </inline-formula> plane is −2.50 eV, indicating that h-Fe<sub>7</sub>C<sub>3</sub> has a better CO adsorption performance. In addition, the defects generated at the truncated position of the h-Fe<sub>7</sub>C<sub>3</sub> crystal plane have a great impact on the adsorption energy of CO on its surface, that is, the adsorption energy of CO on Fe atoms with C vacancies is higher. The activity of CO after adsorption is greatly affected by the adsorption configuration and less affected by the adsorption energy. The higher the coordination number of Fe atoms after adsorption, the higher the CO activity. At the same time, it was found that the bonding of O and Fe atoms is conducive to the activation of CO. |
| first_indexed | 2024-03-10T18:16:55Z |
| format | Article |
| id | doaj.art-6800fd9e14d6405baf6e15ad9cc2d19c |
| institution | Directory Open Access Journal |
| issn | 2073-4352 |
| language | English |
| last_indexed | 2024-03-10T18:16:55Z |
| publishDate | 2020-07-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Crystals |
| spelling | doaj.art-6800fd9e14d6405baf6e15ad9cc2d19c2023-11-20T07:39:18ZengMDPI AGCrystals2073-43522020-07-0110863510.3390/cryst10080635First-Principles Investigation of CO Adsorption on h-Fe<sub>7</sub>C<sub>3</sub> CatalystJinzhe Fu0Deshuai Sun1Zhaojun Chen2Jian Zhang3Hui Du4College of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, ChinaCollege of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, ChinaCollege of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, ChinaSoda ash plant of Shandong Haihua Co., Ltd., Weifang 262737, ChinaCollege of Chemistry and Chemical Engineering, Qingdao University, Qingdao 266071, Chinah-Fe<sub>7</sub>C<sub>3</sub> is considered as the main active phase of medium-temperature Fe-based Fischer–Tropsch catalysts. Basic theoretical guidance for the design and preparation of Fe-based Fischer–Tropsch catalysts can be obtained by studying the adsorption and activation behavior of CO on h-Fe<sub>7</sub>C<sub>3</sub>. In this paper, the first-principles method based on density functional theory is used to study the crystal structure properties of h-Fe<sub>7</sub>C<sub>3</sub> and the adsorption and activation CO on its low Miller index surfaces <inline-formula> <math display="inline"> <semantics> <mrow> <mrow> <mo>(</mo> <mrow> <mn>1</mn> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> <mn>0</mn> </mrow> <mo>)</mo> </mrow> <mo>,</mo> <mrow> <mo>(</mo> <mrow> <mn>1</mn> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> <mn>1</mn> </mrow> <mo>)</mo> </mrow> <mo>,</mo> <mrow> <mo>(</mo> <mrow> <mn>101</mn> </mrow> <mo>)</mo> </mrow> <mo>,</mo> <mrow> <mo>(</mo> <mrow> <mn>1</mn> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> </mrow> <mo>)</mo> </mrow> </mrow> </semantics> </math> </inline-formula> and <inline-formula> <math display="inline"> <semantics> <mrow> <mrow> <mo>(</mo> <mrow> <mn>001</mn> </mrow> <mo>)</mo> </mrow> </mrow> </semantics> </math> </inline-formula>. It was found that the low Miller index crystal plane of h-Fe<sub>7</sub>C<sub>3</sub> crystal has multiple equivalent crystal planes and that the maximum adsorption energy of CO at the 3F2 point of the <inline-formula> <math display="inline"> <semantics> <mrow> <mrow> <mo>(</mo> <mrow> <mn>1</mn> <mover accent="true"> <mn>1</mn> <mo>¯</mo> </mover> <mn>1</mn> </mrow> <mo>)</mo> </mrow> </mrow> </semantics> </math> </inline-formula> plane is −2.50 eV, indicating that h-Fe<sub>7</sub>C<sub>3</sub> has a better CO adsorption performance. In addition, the defects generated at the truncated position of the h-Fe<sub>7</sub>C<sub>3</sub> crystal plane have a great impact on the adsorption energy of CO on its surface, that is, the adsorption energy of CO on Fe atoms with C vacancies is higher. The activity of CO after adsorption is greatly affected by the adsorption configuration and less affected by the adsorption energy. The higher the coordination number of Fe atoms after adsorption, the higher the CO activity. At the same time, it was found that the bonding of O and Fe atoms is conducive to the activation of CO.https://www.mdpi.com/2073-4352/10/8/635Fischer–Tropsch synthesish-Fe<sub>7</sub>C<sub>3</sub>quantum chemistryadsorption activation |
| spellingShingle | Jinzhe Fu Deshuai Sun Zhaojun Chen Jian Zhang Hui Du First-Principles Investigation of CO Adsorption on h-Fe<sub>7</sub>C<sub>3</sub> Catalyst Crystals Fischer–Tropsch synthesis h-Fe<sub>7</sub>C<sub>3</sub> quantum chemistry adsorption activation |
| title | First-Principles Investigation of CO Adsorption on h-Fe<sub>7</sub>C<sub>3</sub> Catalyst |
| title_full | First-Principles Investigation of CO Adsorption on h-Fe<sub>7</sub>C<sub>3</sub> Catalyst |
| title_fullStr | First-Principles Investigation of CO Adsorption on h-Fe<sub>7</sub>C<sub>3</sub> Catalyst |
| title_full_unstemmed | First-Principles Investigation of CO Adsorption on h-Fe<sub>7</sub>C<sub>3</sub> Catalyst |
| title_short | First-Principles Investigation of CO Adsorption on h-Fe<sub>7</sub>C<sub>3</sub> Catalyst |
| title_sort | first principles investigation of co adsorption on h fe sub 7 sub c sub 3 sub catalyst |
| topic | Fischer–Tropsch synthesis h-Fe<sub>7</sub>C<sub>3</sub> quantum chemistry adsorption activation |
| url | https://www.mdpi.com/2073-4352/10/8/635 |
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