Importance of the dipole of interstitial H induced by Pauli - repulsion for the catalysis
Recently we mentioned that the surface of solids often exerts Pauli repulsion on the interstitial/substitutional hydrogen, which markedly changes the properties of H, and increases its chemical activity, which is referred to as ‘Pauli activation of interstitial H’ for short. The purpose of this pape...
| Main Authors: | , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Elsevier
2022-12-01
|
| Series: | Chemical Physics Impact |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S266702242200024X |
| _version_ | 1818194618893729792 |
|---|---|
| author | You Jun-han Ding Wen-jiang Liu Dang-bo Gao Hai-xiang Cong Lina Gu Xiao-kun Hu Song |
| author_facet | You Jun-han Ding Wen-jiang Liu Dang-bo Gao Hai-xiang Cong Lina Gu Xiao-kun Hu Song |
| author_sort | You Jun-han |
| collection | DOAJ |
| description | Recently we mentioned that the surface of solids often exerts Pauli repulsion on the interstitial/substitutional hydrogen, which markedly changes the properties of H, and increases its chemical activity, which is referred to as ‘Pauli activation of interstitial H’ for short. The purpose of this paper is to further confirm the reality of this activation mechanism at a quantitative level. We particularly mention the importance of the H-dipole of the interstitial hydrogen induced by Pauli activation for this catalysis, which is the key to understand the principle of this catalysis mechanism. Taking a simple diatomic molecule as an example, we first illustrate what are the prerequisites for forming a molecular covalent bond, when the two atoms are in close contact. Then we argue that, the Pauli-activated H at solid surface just meets these prerequisites due to the dual modulation effect of the induced H-dipole on both the energy and the spatial orientation of a foreign atom/molecule in the bonding process with H, thus accelerates the hydrogenation. Moreover, we emphasize that the size of the depression/hole at solid surface, where the interstitial H sited(simply referred to as ‘Pauli hole’), must match the radius of H to ensure the effectiveness of Pauli activation of H. Accordingly it provides a criteria for selecting a suitable catalysts for the specific chemical reaction, which would be useful in practical applications. Taking a common chemical reaction as an example, we make a calculation and quantitative analysis of the synthesis of MgH2, using Ni as the heterogeneous catalyst. Details of how to select a suitable catalyst are given in this reaction. And why and how the dual modulation effect of the induced H-dipole of interstitial H promotes the realization of the prerequisites, thus facilitates the formation of the covalent bond Mg-H. Therefore the rationality of the Pauli activation-catalysis is confirmed theoretically. |
| first_indexed | 2024-12-12T01:05:10Z |
| format | Article |
| id | doaj.art-3ad6968cd4884524aa5b30c7c7af1142 |
| institution | Directory Open Access Journal |
| issn | 2667-0224 |
| language | English |
| last_indexed | 2024-12-12T01:05:10Z |
| publishDate | 2022-12-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Chemical Physics Impact |
| spelling | doaj.art-3ad6968cd4884524aa5b30c7c7af11422022-12-22T00:43:36ZengElsevierChemical Physics Impact2667-02242022-12-015100085Importance of the dipole of interstitial H induced by Pauli - repulsion for the catalysisYou Jun-han0Ding Wen-jiang1Liu Dang-bo2Gao Hai-xiang3Cong Lina4Gu Xiao-kun5Hu Song6Department of Astronomy, School of Physics and Astronomy, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, ChinaCenter of Hydrogen Science, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240 ChinaDepartment of Astronomy, School of Physics and Astronomy, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China; Shanghai Key Laboratory for Particle Physics and Cosmology, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China; Corresponding author at: Department of Astronomy, School of Physics and Astronomy, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, China.Zhiyuan College, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, ChinaCenter of Hydrogen Science, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240 ChinaInstitute of Engineering Thermophysics, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, ChinaInstitute of Engineering Thermophysics, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, ChinaRecently we mentioned that the surface of solids often exerts Pauli repulsion on the interstitial/substitutional hydrogen, which markedly changes the properties of H, and increases its chemical activity, which is referred to as ‘Pauli activation of interstitial H’ for short. The purpose of this paper is to further confirm the reality of this activation mechanism at a quantitative level. We particularly mention the importance of the H-dipole of the interstitial hydrogen induced by Pauli activation for this catalysis, which is the key to understand the principle of this catalysis mechanism. Taking a simple diatomic molecule as an example, we first illustrate what are the prerequisites for forming a molecular covalent bond, when the two atoms are in close contact. Then we argue that, the Pauli-activated H at solid surface just meets these prerequisites due to the dual modulation effect of the induced H-dipole on both the energy and the spatial orientation of a foreign atom/molecule in the bonding process with H, thus accelerates the hydrogenation. Moreover, we emphasize that the size of the depression/hole at solid surface, where the interstitial H sited(simply referred to as ‘Pauli hole’), must match the radius of H to ensure the effectiveness of Pauli activation of H. Accordingly it provides a criteria for selecting a suitable catalysts for the specific chemical reaction, which would be useful in practical applications. Taking a common chemical reaction as an example, we make a calculation and quantitative analysis of the synthesis of MgH2, using Ni as the heterogeneous catalyst. Details of how to select a suitable catalyst are given in this reaction. And why and how the dual modulation effect of the induced H-dipole of interstitial H promotes the realization of the prerequisites, thus facilitates the formation of the covalent bond Mg-H. Therefore the rationality of the Pauli activation-catalysis is confirmed theoretically.http://www.sciencedirect.com/science/article/pii/S266702242200024XHeterogeneous catalysis‘Pauli activation’Surface/Subsurface interstitial hydrogenInduced H-dipoleHydrogenation |
| spellingShingle | You Jun-han Ding Wen-jiang Liu Dang-bo Gao Hai-xiang Cong Lina Gu Xiao-kun Hu Song Importance of the dipole of interstitial H induced by Pauli - repulsion for the catalysis Chemical Physics Impact Heterogeneous catalysis ‘Pauli activation’ Surface/Subsurface interstitial hydrogen Induced H-dipole Hydrogenation |
| title | Importance of the dipole of interstitial H induced by Pauli - repulsion for the catalysis |
| title_full | Importance of the dipole of interstitial H induced by Pauli - repulsion for the catalysis |
| title_fullStr | Importance of the dipole of interstitial H induced by Pauli - repulsion for the catalysis |
| title_full_unstemmed | Importance of the dipole of interstitial H induced by Pauli - repulsion for the catalysis |
| title_short | Importance of the dipole of interstitial H induced by Pauli - repulsion for the catalysis |
| title_sort | importance of the dipole of interstitial h induced by pauli repulsion for the catalysis |
| topic | Heterogeneous catalysis ‘Pauli activation’ Surface/Subsurface interstitial hydrogen Induced H-dipole Hydrogenation |
| url | http://www.sciencedirect.com/science/article/pii/S266702242200024X |
| work_keys_str_mv | AT youjunhan importanceofthedipoleofinterstitialhinducedbypaulirepulsionforthecatalysis AT dingwenjiang importanceofthedipoleofinterstitialhinducedbypaulirepulsionforthecatalysis AT liudangbo importanceofthedipoleofinterstitialhinducedbypaulirepulsionforthecatalysis AT gaohaixiang importanceofthedipoleofinterstitialhinducedbypaulirepulsionforthecatalysis AT conglina importanceofthedipoleofinterstitialhinducedbypaulirepulsionforthecatalysis AT guxiaokun importanceofthedipoleofinterstitialhinducedbypaulirepulsionforthecatalysis AT husong importanceofthedipoleofinterstitialhinducedbypaulirepulsionforthecatalysis |