2022
DOI: 10.1021/acscatal.2c02674
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A Stable Zn-MOF for Photocatalytic Csp3–H Oxidation: Vinyl Double Bonds Boosting Electron Transfer and Enhanced Oxygen Activation

Abstract: Molecular oxygen activation has always been a difficult issue and challenge in heterogeneous photocatalytic aerobic oxidations due to the kinetically persistent or spin-forbidden nature of O 2 . In this work, a highly delocalized interpenetrated 3D MOF photocatalyst with high stability, Zn-TACPA (H 3 TACPA = tris(3carboxybiphenyl)amine), based on vinyl-functionalized triphenylamine and bipyridine ligands has been fabricated and employed as a reactive oxygen species (ROS) generator to catalyze the photooxidativ… Show more

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Cited by 23 publications
(17 citation statements)
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“…Therefore, this synergistic catalytic strategy offers great opportunities for achieving C–H bond selective oxidation with molecular oxygen as an oxidant. Of the reported synergistic activation approaches, metal – organic frameworks (MOFs), also known as porous coordination polymers (PCPs), can provide a fine-tunable catalytic platform by judiciously introducing different functional unit blocks into the structures for realizing multiple catalytic processes synergistically in tandem. , Moreover, taking the advantage of interpenetration in the structures of metal – organic frameworks, not only the rigidity and stability of the catalyst structures would simultaneously be enhanced, but also the distances between different catalytic active sites could be adjusted appropriately, possibly boosting the synergistic catalytic process. , …”
Section: Introductionmentioning
confidence: 99%
See 1 more Smart Citation
“…Therefore, this synergistic catalytic strategy offers great opportunities for achieving C–H bond selective oxidation with molecular oxygen as an oxidant. Of the reported synergistic activation approaches, metal – organic frameworks (MOFs), also known as porous coordination polymers (PCPs), can provide a fine-tunable catalytic platform by judiciously introducing different functional unit blocks into the structures for realizing multiple catalytic processes synergistically in tandem. , Moreover, taking the advantage of interpenetration in the structures of metal – organic frameworks, not only the rigidity and stability of the catalyst structures would simultaneously be enhanced, but also the distances between different catalytic active sites could be adjusted appropriately, possibly boosting the synergistic catalytic process. , …”
Section: Introductionmentioning
confidence: 99%
“…22,23 Moreover, taking the advantage of interpenetration in the structures of metal−organic frameworks, not only the rigidity and stability of the catalyst structures would simultaneously be enhanced, but also the distances between different catalytic active sites could be adjusted appropriately, possibly boosting the synergistic catalytic process. 24,25 In cytochrome c oxidase, the iron−porphyrin motif serves as a catalytic site for the activation of molecular oxygen, while the adjacent Cu site could activate C−H bonds of substrates, realizing dual-site synergistic catalytic C−H bond oxidation with high efficiency and high selectivity. 26−28 Inspired by the synergistic catalysis of cytochrome c oxidase, combining oxygen activation sites and C(sp 3 )−H bond activation sites into one catalytic platform would be an ideal strategy for synergistic catalytic inert C(sp 3 )−H bond oxidation under mild conditions.…”
Section: ■ Introductionmentioning
confidence: 99%
“…The photoresponsive organic ligands are properly introduced into the MOFs to give rise to chemical modifications to become efficient and heterogeneous catalysts for the construction of various photocatalytic reactions. 15,16 On the other hand, MOFs have promising applications in gas adsorption and separation, 17−19 drug delivery and release, 20 fluorescence sensing, 21,22 supercapacitors, 23 and other fields.…”
Section: ■ Introductionmentioning
confidence: 99%
“…For example, Wu et al reported a case of DUT-67­(Zr), which exposed unsaturated metal sites through surface coordination to activate substrate molecules, so it has great application potential in the field of photocatalysis. The photoresponsive organic ligands are properly introduced into the MOFs to give rise to chemical modifications to become efficient and heterogeneous catalysts for the construction of various photocatalytic reactions. , On the other hand, MOFs have promising applications in gas adsorption and separation, drug delivery and release, fluorescence sensing, , supercapacitors, and other fields.…”
Section: Introductionmentioning
confidence: 99%
“…21 On the other hand, rationally modifying the interpenetration degree of frameworks could provide abundant hierarchically porous reaction channels to accelerate hole-electron separation and facilitate the adsorption and activation of molecular oxygen. 22,23 Nevertheless, many existing large-pore networks constructed from interpenetrated frameworks lose a signicant number of accessible reaction channels during MOF activation and visible light excitation. 24,25 Thus, we envisioned that the ne modulation of interpenetration between frameworks would precisely regulate the generation and proportion of O 2 c − and 1 O 2 species, balancing the framework stability and photocatalytic performance during photocatalytic aerobic oxidation reactions.…”
Section: Introductionmentioning
confidence: 99%