First row transition metal catalyzed small molecule activation for sustainable organic transformation: Synergy between nature and chemist’s toolbox

Maurya, Yashdeep; Singh, Arya; Kumar, Vishal; Ul Nisa, Mehar; Chatterjee, Sayanti

doi:10.1016/j.tetlet.2024.155066

Tetrahedron Letters

2024

DOI: 10.1016/j.tetlet.2024.155066

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First row transition metal catalyzed small molecule activation for sustainable organic transformation: Synergy between nature and chemist’s toolbox

Yashdeep Maurya,

Arya Singh,

Vishal Kumar

et al.

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2024

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Cited by 4 publications

References 126 publications

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Novel Lewis Acid‐Base Interactions in Polymer‐Derived Sodium‐Doped Amorphous Si−B−N Ceramic: Towards Main‐Group‐Mediated Hydrogen Activation

Tada,

Terashima,

Shimizu

et al. 2024

Angewandte Chemie

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Interest is growing in transition metal‐free compounds for small molecule activation and catalysis. We discuss the opportunities arising from synthesizing sodium‐doped amorphous silicon‐boron‐nitride (Na‐doped a‐SiBN). Na+ cations and 3‐fold coordinated BIII moieties were incorporated into an amorphous silicon nitride network via chemical modification of a polysilazane followed by pyrolysis in ammonia at 1000 °C. Emphasis is placed on the mechanisms of hydrogen (H2) activation within Na‐doped a‐SiBN structure. This material design approach allows the homogeneous distribution of Na+ and BIII moieties surrounded by SiN4 units contributing to the transformation of the BIII moieties into 4‐fold coordinated geometry upon encountering H2, potentially serving as frustrated Lewis acid (FLA) sites. Exposure to H2 induced formation of frustrated Lewis base (FLB) N–= sites with Na+ as a charge‐compensating cation, resulting in the in situ formation of a frustrated Lewis pair (FLP) motif (≡BFLA···Hδ–···Hδ+···:N–(Na+)=). Reversible H2 adsorption‐desorption behavior with high activation energy for H2 desorption (124 kJ mol–1) suggested the H2 chemisorption on Na‐doped a‐SiBN. These findings highlight a future landscape full of possibilities within our reach, where we anticipate main‐group‐mediated small molecule activation will have an important impact on the design of more efficient catalytic processes and the discovery of new catalytic transformations.

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Novel Lewis Acid‐Base Interactions in Polymer‐Derived Sodium‐Doped Amorphous Si−B−N Ceramic: Towards Main‐Group‐Mediated Hydrogen Activation

Tada,

Terashima,

Shimizu

et al. 2024

Angewandte Chemie

View full text Add to dashboard Cite

show abstract

Novel Lewis Acid‐Base Interactions in Polymer‐Derived Sodium‐Doped Amorphous Si−B−N Ceramic: Towards Main‐Group‐Mediated Hydrogen Activation

Tada,

Terashima,

Shimizu

et al. 2024

Angew Chem Int Ed

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Synthesis and Structural Characterization of 2,2’-Bipyridine Zinc Formate: Analysis of Formate Bonding and Hydrosilylation of CO2 and Carbonyl Compounds

de la Mora,

Loo,

Yan

et al. 2024

Journal of Organometallic Chemistry

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First row transition metal catalyzed small molecule activation for sustainable organic transformation: Synergy between nature and chemist’s toolbox

Cited by 4 publications

References 126 publications

Novel Lewis Acid‐Base Interactions in Polymer‐Derived Sodium‐Doped Amorphous Si−B−N Ceramic: Towards Main‐Group‐Mediated Hydrogen Activation

Novel Lewis Acid‐Base Interactions in Polymer‐Derived Sodium‐Doped Amorphous Si−B−N Ceramic: Towards Main‐Group‐Mediated Hydrogen Activation

Novel Lewis Acid‐Base Interactions in Polymer‐Derived Sodium‐Doped Amorphous Si−B−N Ceramic: Towards Main‐Group‐Mediated Hydrogen Activation

Synthesis and Structural Characterization of 2,2’-Bipyridine Zinc Formate: Analysis of Formate Bonding and Hydrosilylation of CO2 and Carbonyl Compounds

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