TY - JOUR
T1 - Cage-Confined CuO Nanoparticles
T2 - Unlocking Site-Selective Catalysis for Borylation of α,β-Unsaturated Conjugated Compounds
AU - Li, Zexu
AU - Ao, Ranxiao
AU - Zhai, Yizhuang
AU - Li, Shuozi
AU - Liu, Yuzhou
N1 - Publisher Copyright:
© 2025 Wiley-VCH GmbH.
PY - 2025/8/20
Y1 - 2025/8/20
N2 - The borylation of α,β-unsaturated carbonyl compounds is pivotal for constructing multifunctional organoboron intermediates in pharmaceuticals and materials. Here, the study reports CuO@COP1-T, a novel catalyst integrating CuO nanoparticles (NPs) within a covalent organic porous cage (COP1-T), which achieves unprecedented site-selectivity in the borylation of α,β-unsaturated conjugated compounds. Experimental results demonstrate CuO@COP1-T exhibits 100% monoboration selectivity for trans-dibenzylideneacetone, surpassing unsupported CuO@NPs (8%). Molecular dynamics (MD) simulations reveal the 1.2 nm triangular cage pores enforce selectivity via geometric matching with reaction intermediates. Optimization of reaction conditions clarifies the impacts of methanol amount, solvent type, and base addition. The catalyst retains >95% activity over five cycles, showcasing robust stability. This work establishes a synergistic platform where COP1-T stabilizes CuO NPs while creating a confined microenvironment to enforce spatial confinement effects, providing a rational design strategy for confined-metal catalysts in organoboron chemistry.
AB - The borylation of α,β-unsaturated carbonyl compounds is pivotal for constructing multifunctional organoboron intermediates in pharmaceuticals and materials. Here, the study reports CuO@COP1-T, a novel catalyst integrating CuO nanoparticles (NPs) within a covalent organic porous cage (COP1-T), which achieves unprecedented site-selectivity in the borylation of α,β-unsaturated conjugated compounds. Experimental results demonstrate CuO@COP1-T exhibits 100% monoboration selectivity for trans-dibenzylideneacetone, surpassing unsupported CuO@NPs (8%). Molecular dynamics (MD) simulations reveal the 1.2 nm triangular cage pores enforce selectivity via geometric matching with reaction intermediates. Optimization of reaction conditions clarifies the impacts of methanol amount, solvent type, and base addition. The catalyst retains >95% activity over five cycles, showcasing robust stability. This work establishes a synergistic platform where COP1-T stabilizes CuO NPs while creating a confined microenvironment to enforce spatial confinement effects, providing a rational design strategy for confined-metal catalysts in organoboron chemistry.
KW - borylation reaction
KW - copper nanoparticles
KW - covalent organic porous cage
KW - molecular dynamics simulation
KW - α,β-unsaturated conjugated compounds
UR - https://www.scopus.com/pages/publications/105002620533
U2 - 10.1002/smtd.202402178
DO - 10.1002/smtd.202402178
M3 - 文章
C2 - 40231597
AN - SCOPUS:105002620533
SN - 2366-9608
VL - 9
JO - Small Methods
JF - Small Methods
IS - 8
M1 - 2402178
ER -