An Adaptive Palladium Single-Atom Catalyst Enabling Reactivity Switching between Borylation and C-C Coupling

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989592%3A15640%2F25%3A73631060" target="_blank" >RIV/61989592:15640/25:73631060 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61989100:27640/25:10258198

Výsledek na webu

<a href="https://pubs.acs.org/doi/10.1021/jacs.4c17943" target="_blank" >https://pubs.acs.org/doi/10.1021/jacs.4c17943</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/jacs.4c17943" target="_blank" >10.1021/jacs.4c17943</a>

Jazyk výsledku

angličtina

Název v původním jazyce

An Adaptive Palladium Single-Atom Catalyst Enabling Reactivity Switching between Borylation and C-C Coupling

Popis výsledku v původním jazyce

The development of single-atom catalysts (SACs) with site-specific and tunable catalytic functionalities remains a highly desirable yet challenging goal in catalysis. In this study, we report a SAC featuring anisotropic coordination cavities synthesized via a one-step polymerization of 2,6-diaminopyridine and cyanuric chloride. These cavities provide a robust framework for anchoring isolated Pd single atoms with exceptional stability. The unique broken symmetry of the catalyst&apos;s local structure enables precise control over reaction pathways, allowing reactivity to be switched between distinct catalytic outcomes. Specifically, under tailored reaction conditions, the catalyst can either halt at the borylation step or proceed seamlessly to Suzuki coupling in a self-cascade process. Mechanistic studies unveil the pivotal role of Pd single atoms in driving key steps, including oxidative addition, base exchange, and reductive elimination. Furthermore, green metrics demonstrate the process&apos;s sustainability, with minimized waste generation and reduced reliance on hazardous reagents in the self-cascade transformation. This work establishes an innovative benchmark in the field of single-atom catalysis: by enabling complex, multistep transformations via strategic activation of multiple functional groups, this catalyst exemplifies the potential of self-cascade processes to revolutionize synthetic chemistry via catalysis engineering.

Název v anglickém jazyce

An Adaptive Palladium Single-Atom Catalyst Enabling Reactivity Switching between Borylation and C-C Coupling

Popis výsledku anglicky

The development of single-atom catalysts (SACs) with site-specific and tunable catalytic functionalities remains a highly desirable yet challenging goal in catalysis. In this study, we report a SAC featuring anisotropic coordination cavities synthesized via a one-step polymerization of 2,6-diaminopyridine and cyanuric chloride. These cavities provide a robust framework for anchoring isolated Pd single atoms with exceptional stability. The unique broken symmetry of the catalyst&apos;s local structure enables precise control over reaction pathways, allowing reactivity to be switched between distinct catalytic outcomes. Specifically, under tailored reaction conditions, the catalyst can either halt at the borylation step or proceed seamlessly to Suzuki coupling in a self-cascade process. Mechanistic studies unveil the pivotal role of Pd single atoms in driving key steps, including oxidative addition, base exchange, and reductive elimination. Furthermore, green metrics demonstrate the process&apos;s sustainability, with minimized waste generation and reduced reliance on hazardous reagents in the self-cascade transformation. This work establishes an innovative benchmark in the field of single-atom catalysis: by enabling complex, multistep transformations via strategic activation of multiple functional groups, this catalyst exemplifies the potential of self-cascade processes to revolutionize synthetic chemistry via catalysis engineering.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10402 - Inorganic and nuclear chemistry

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

ISSN

0002-7863

e-ISSN

1520-5126

Svazek periodika

147

Číslo periodika v rámci svazku

22

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

17

Strana od-do

"18524 "- 18540

Kód UT WoS článku

001494642700001

EID výsledku v databázi Scopus

2-s2.0-105005849102