Polymer surfaces adorning ligand-coordinated palladium for hydrogenation reactions

Nasrollahzadeh, Mahmoud; Shafiei, Nasrin; Maham, Mehdi; Issaabadi, Zahra; Nezafat, Zahra; Varma, Rajender S.

doi:10.1016/j.mcat.2020.111129

Cited by 2 publications

(2 citation statements)

References 143 publications

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“…In one strategy, the Pd nanoparticles were modified with other metal-to-alloy nanoparticles for isolating the Pd active sites. , These alloy catalysts can improve the selectivity of alkenes at the expense of conversion. Another strategy is modulating Pd nanoparticles with organic capping ligands . Capping ligands (thiols, phosphine, amine, etc.)…”

Section: Introductionmentioning

confidence: 99%

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Selective Hydrogenation of Alkyne by Atomically Precise Pd₆ Nanocluster Catalysts: Accurate Construction of the Coplanar and Specific Active Sites

Tang,

Jia,

Zhang

et al. 2024

ACS Catal.

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Atomically precise nanoclusters are promising model catalysts to understand the relationship between structure and catalytic activity. However, designing efficient active sites remains challenging because the highly covered ligands obscure the metal sites. Herein, we reported a Pd 6 (S-Adm) 6 (PPh 3 )(PPh) nanocluster, which shows high selectivity in the semihydrogenation of aromatic alkyne. The Pd 6 nanocluster has a unique chair structure, where the pan is composed of the coplanar Pd atoms, the back is composed of two S-Adm ligands, and the legs are composed of four S-Adm, one PPh 3 , and one PPh ligands. Experiments reveal that the high selectivity of intact Pd 6 nanocluster is attributed to the synergistic effect of thiols and phosphines, modulating the electron properties and benefiting the proper hydrogen dissociation ability and desorption of product. Interestingly, it was found that the exposed coplanar Pd atoms could provide specific active sites for the adsorption of C�C and benzene ring. DFT calculations show that phenylacetylene and styrene adsorb on the coplanar Pd 6 much weaker than on the Pd(111) surface, allowing the styrene to be desorbed before further hydrogenation. The phenyl adsorption constrains that the hydrogenation can occur only on the coplanar Pd 6 , which is more facile for phenylacetylene than for styrene, and results in semihydrogenation.

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Section: Introductionmentioning

confidence: 99%

“…Another strategy is modulating Pd nanoparticles with organic capping ligands. 41 Capping ligands (thiols, phosphine, amine, etc.) could alter the electronic state of Pd nanoparticles, adsorption mode (intensity) of alkynes and alkenes, and further effectively enhance the selectivity to alkene.…”

Section: ■ Introductionmentioning

confidence: 99%

Selective Hydrogenation of Alkyne by Atomically Precise Pd₆ Nanocluster Catalysts: Accurate Construction of the Coplanar and Specific Active Sites

Tang,

Jia,

Zhang

et al. 2024

ACS Catal.

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Metal-free nanostructured catalysts: sustainable driving forces for organic transformations

et al. 2021

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Polymer surfaces adorning ligand-coordinated palladium for hydrogenation reactions

Cited by 2 publications

References 143 publications

Selective Hydrogenation of Alkyne by Atomically Precise Pd₆ Nanocluster Catalysts: Accurate Construction of the Coplanar and Specific Active Sites

Selective Hydrogenation of Alkyne by Atomically Precise Pd₆ Nanocluster Catalysts: Accurate Construction of the Coplanar and Specific Active Sites

Metal-free nanostructured catalysts: sustainable driving forces for organic transformations

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Polymer surfaces adorning ligand-coordinated palladium for hydrogenation reactions

Cited by 2 publications

References 143 publications

Selective Hydrogenation of Alkyne by Atomically Precise Pd6 Nanocluster Catalysts: Accurate Construction of the Coplanar and Specific Active Sites

Selective Hydrogenation of Alkyne by Atomically Precise Pd6 Nanocluster Catalysts: Accurate Construction of the Coplanar and Specific Active Sites

Metal-free nanostructured catalysts: sustainable driving forces for organic transformations

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Selective Hydrogenation of Alkyne by Atomically Precise Pd₆ Nanocluster Catalysts: Accurate Construction of the Coplanar and Specific Active Sites

Selective Hydrogenation of Alkyne by Atomically Precise Pd₆ Nanocluster Catalysts: Accurate Construction of the Coplanar and Specific Active Sites