Selective oxidation of β-keto ester modulated by the d-band centers in D-A conjugated microporous metallaphotoredox catalysts containing M-salen (MZn, Cu and Co) and triazine monomers
Copyright © 2024 Elsevier Inc. All rights reserved..
Photocatalytic selective oxidation plays an important role in developing green chemistry. However, it is challenging to design an efficient photocatalyst for controlling the selectivity of photocatalytic oxidation reaction and exploring its detailed mechanism. Here, we synthesized three conjugated microporous polymers (CMPs) with D-A structures, named M-SATE-CMPs (MZn, Cu and Co), with different d-band centers based on different metal centers, resulting in the discrepancy in adsorption and activation capacities for the reactants, which produces the selectivity of β-keto esters being catalyzed into α-hydroperoxide β-keto esters (ROOH) or to α-hydroxyl β-keto esters (ROH). Density functional theory (DFT) calculations also demonstrate that the adsorption and activation capacities of the metal active centers in M-SATE-CMPs (MZn, Cu and Co) for ROOH are the key factors to influence the photocatalytic selective oxidation of β-keto ester. This study provides a promising strategy for designing a metallaphotoredox catalyst whose photocatalytic selectivity depends on the d-band center of metal site in the catalyst.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:665 |
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| Enthalten in: |
Journal of colloid and interface science - 665(2024) vom: 15. Apr., Seite 399-412 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Xie, Lin-Fu [VerfasserIn] |
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| Links: |
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| Themen: |
Conjugated microporous polymer |
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| Anmerkungen: |
Date Revised 16.04.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1016/j.jcis.2024.03.153 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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NLM370271300 |
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| 245 | 1 | 0 | |a Selective oxidation of β-keto ester modulated by the d-band centers in D-A conjugated microporous metallaphotoredox catalysts containing M-salen (MZn, Cu and Co) and triazine monomers |
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| 500 | |a Date Revised 16.04.2024 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Copyright © 2024 Elsevier Inc. All rights reserved. | ||
| 520 | |a Photocatalytic selective oxidation plays an important role in developing green chemistry. However, it is challenging to design an efficient photocatalyst for controlling the selectivity of photocatalytic oxidation reaction and exploring its detailed mechanism. Here, we synthesized three conjugated microporous polymers (CMPs) with D-A structures, named M-SATE-CMPs (MZn, Cu and Co), with different d-band centers based on different metal centers, resulting in the discrepancy in adsorption and activation capacities for the reactants, which produces the selectivity of β-keto esters being catalyzed into α-hydroperoxide β-keto esters (ROOH) or to α-hydroxyl β-keto esters (ROH). Density functional theory (DFT) calculations also demonstrate that the adsorption and activation capacities of the metal active centers in M-SATE-CMPs (MZn, Cu and Co) for ROOH are the key factors to influence the photocatalytic selective oxidation of β-keto ester. This study provides a promising strategy for designing a metallaphotoredox catalyst whose photocatalytic selectivity depends on the d-band center of metal site in the catalyst | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Conjugated microporous polymer | |
| 650 | 4 | |a D-band center | |
| 650 | 4 | |a Metallaphotoredox catalyst | |
| 650 | 4 | |a Oxide intermediate | |
| 650 | 4 | |a Photocatalytic selective oxidation | |
| 700 | 1 | |a Huang, Wan-Hong |e verfasserin |4 aut | |
| 700 | 1 | |a Chen, Jian-Ping |e verfasserin |4 aut | |
| 700 | 1 | |a Chen, Hai-Lin |e verfasserin |4 aut | |
| 700 | 1 | |a Hou, Cheng |e verfasserin |4 aut | |
| 700 | 1 | |a Ni, Qing-Ling |e verfasserin |4 aut | |
| 700 | 1 | |a Huang, Ting-Hong |e verfasserin |4 aut | |
| 700 | 1 | |a Gui, Liu-Cheng |e verfasserin |4 aut | |
| 700 | 1 | |a Wang, Xiu-Jian |e verfasserin |4 aut | |
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