Mesoporosity‐Enabled Selectivity of Mesoporous Palladium‐Based Nanocrystals Catalysts in Semihydrogenation of Alkynes
We reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)‐based nanobundles catalysts. The best mesoporous PdP displayed full conversion, remarkable activity, excellent selectivity, and high stability in semihydrogenation of 1‐phenyl‐1‐prop...
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Published in | Angewandte Chemie International Edition Vol. 61; no. 8; pp. e202114539 - n/a |
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Main Authors | , , , , , |
Format | Journal Article |
Language | English |
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14.02.2022
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Abstract | We reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)‐based nanobundles catalysts. The best mesoporous PdP displayed full conversion, remarkable activity, excellent selectivity, and high stability in semihydrogenation of 1‐phenyl‐1‐propyne, all of which are remarkably better than commercial Lindlar catalysts. Mechanistic investigations ascribed high semihydrogenation selectivity to the continuous crystalline framework and penetrated mesoporous channel of catalysts that weakened the adsorption and interaction capacity of alkenes and thus inhibited over‐hydrogenation of alkenes to industrially unfavorable alkanes. Density functional theory calculations further demonstrated that convex crystalline mesoporosity of nanobundles catalysts electronically optimized the coordination environment of Pd active sites and energetically changed hydrogenation trends, resulting in a superior semihydrogenation selectivity to targeted alkenes.
Mesoporosity engineering is demonstrated as an efficient route for boosting catalytic selectivity of Pd‐based nanobundle catalysts in the semihydrogenation of alkynes. Mechanistic studies reveal that the continuous crystalline framework and penetrated mesoporous channel of mesoporous Pd‐based catalysts synergistically weaken the adsorption and binding strength of alkenes and energetically disable further over‐hydrogenation of alkenes to alkanes. |
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AbstractList | We reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)‐based nanobundles catalysts. The best mesoporous PdP displayed full conversion, remarkable activity, excellent selectivity, and high stability in semihydrogenation of 1‐phenyl‐1‐propyne, all of which are remarkably better than commercial Lindlar catalysts. Mechanistic investigations ascribed high semihydrogenation selectivity to the continuous crystalline framework and penetrated mesoporous channel of catalysts that weakened the adsorption and interaction capacity of alkenes and thus inhibited over‐hydrogenation of alkenes to industrially unfavorable alkanes. Density functional theory calculations further demonstrated that convex crystalline mesoporosity of nanobundles catalysts electronically optimized the coordination environment of Pd active sites and energetically changed hydrogenation trends, resulting in a superior semihydrogenation selectivity to targeted alkenes.
Mesoporosity engineering is demonstrated as an efficient route for boosting catalytic selectivity of Pd‐based nanobundle catalysts in the semihydrogenation of alkynes. Mechanistic studies reveal that the continuous crystalline framework and penetrated mesoporous channel of mesoporous Pd‐based catalysts synergistically weaken the adsorption and binding strength of alkenes and energetically disable further over‐hydrogenation of alkenes to alkanes. We reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)‐based nanobundles catalysts. The best mesoporous PdP displayed full conversion, remarkable activity, excellent selectivity, and high stability in semihydrogenation of 1‐phenyl‐1‐propyne, all of which are remarkably better than commercial Lindlar catalysts. Mechanistic investigations ascribed high semihydrogenation selectivity to the continuous crystalline framework and penetrated mesoporous channel of catalysts that weakened the adsorption and interaction capacity of alkenes and thus inhibited over‐hydrogenation of alkenes to industrially unfavorable alkanes. Density functional theory calculations further demonstrated that convex crystalline mesoporosity of nanobundles catalysts electronically optimized the coordination environment of Pd active sites and energetically changed hydrogenation trends, resulting in a superior semihydrogenation selectivity to targeted alkenes. Abstract We reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)‐based nanobundles catalysts. The best mesoporous PdP displayed full conversion, remarkable activity, excellent selectivity, and high stability in semihydrogenation of 1‐phenyl‐1‐propyne, all of which are remarkably better than commercial Lindlar catalysts. Mechanistic investigations ascribed high semihydrogenation selectivity to the continuous crystalline framework and penetrated mesoporous channel of catalysts that weakened the adsorption and interaction capacity of alkenes and thus inhibited over‐hydrogenation of alkenes to industrially unfavorable alkanes. Density functional theory calculations further demonstrated that convex crystalline mesoporosity of nanobundles catalysts electronically optimized the coordination environment of Pd active sites and energetically changed hydrogenation trends, resulting in a superior semihydrogenation selectivity to targeted alkenes. |
Author | Qin, Huaiyu Lv, Hao Huang, Bolong Liu, Ben Sun, Mingzi Jia, Fengrui |
Author_xml | – sequence: 1 givenname: Hao surname: Lv fullname: Lv, Hao organization: Sichuan University – sequence: 2 givenname: Huaiyu surname: Qin fullname: Qin, Huaiyu organization: Sichuan University – sequence: 3 givenname: Mingzi surname: Sun fullname: Sun, Mingzi organization: The Hong Kong Polytechnic University, Hung Hom – sequence: 4 givenname: Fengrui surname: Jia fullname: Jia, Fengrui organization: Sichuan University – sequence: 5 givenname: Bolong surname: Huang fullname: Huang, Bolong email: bhuang@polyu.edu.hk organization: The Hong Kong Polytechnic University, Hung Hom – sequence: 6 givenname: Ben orcidid: 0000-0003-1305-5900 surname: Liu fullname: Liu, Ben email: ben.liu@scu.edu.cn organization: Sichuan University |
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Keywords | Semihydrogenation Catalytic Mechanism Crystalline Framework Mesoporosity Mesoporous Metal |
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Snippet | We reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)‐based nanobundles catalysts. The best... We reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)-based nanobundles catalysts. The best... Abstract We reported mesoporosity engineering as a general strategy to promote semihydrogenation selectivity of palladium (Pd)‐based nanobundles catalysts. The... |
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SubjectTerms | Alkanes Alkenes Alkynes Catalysts Catalytic Mechanism Crystal structure Crystalline Framework Crystallinity Density functional theory Hydrogenation Mesoporosity Mesoporous Metal Nanocrystals Palladium Selectivity Semihydrogenation |
Title | Mesoporosity‐Enabled Selectivity of Mesoporous Palladium‐Based Nanocrystals Catalysts in Semihydrogenation of Alkynes |
URI | https://onlinelibrary.wiley.com/doi/abs/10.1002%2Fanie.202114539 https://www.ncbi.nlm.nih.gov/pubmed/34913234 https://www.proquest.com/docview/2625968246/abstract/ https://search.proquest.com/docview/2610910591 |
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