TY - JOUR
T1 - Poly(heptazine imide) ligand exchange enables remarkable low catalyst loadings in heterogeneous metallaphotocatalysis
AU - Xing, Liuzhuang
AU - Yang, Qian
AU - Zhu, Chen
AU - Bai, Yilian
AU - Tang, Yurong
AU - Rueping, Magnus
AU - Cai, Yunfei
N1 - Funding Information:
This work is supported by funding from the Natural Science Foundation of Chongqing (CSTB2022NSCQ-MSX1105 to Y.C., CSTB2022NSCQ-MSX1032 to Y.T.), the National Natural Science Foundation of China (Grant no. 21801030 to Y.C.), the King Abdullah University of Science and Technology (KAUST), Saudi Arabia, Office of Sponsored Research (URF/1/4025 to C.Z. and M.R.). We thank the Analytical and Testing Center of Chongqing University for assistance with NMR spectrum analysis.
Funding Information:
This work is supported by funding from the Natural Science Foundation of Chongqing (CSTB2022NSCQ-MSX1105 to Y.C., CSTB2022NSCQ-MSX1032 to Y.T.), the National Natural Science Foundation of China (Grant no. 21801030 to Y.C.), the King Abdullah University of Science and Technology (KAUST), Saudi Arabia, Office of Sponsored Research (URF/1/4025 to C.Z. and M.R.). We thank the Analytical and Testing Center of Chongqing University for assistance with NMR spectrum analysis.
Publisher Copyright:
© 2023, The Author(s).
PY - 2023/12
Y1 - 2023/12
N2 - The development of heterogeneous metallaphotocatalysis is of great interest for sustainable organic synthesis. The rational design and controllable preparation of well-defined (site-isolated) metal/photo bifunctional solid catalysts to meet such goal remains a critical challenge. Herein, we demonstrate the incorporation of privileged homogeneous bipyridyl-based Ni-catalysts into highly ordered and crystalline potassium poly(heptazine imide) (K-PHI). A variety of PHI-supported cationic bipyridyl-based Ni-catalysts (LnNi-PHI) have been prepared and fully characterized by various techniques including NMR, ICP-OES, XPS, HAADF-STEM and XAS. The LnNi-PHI catalysts exhibit exceptional chemical stability and recyclability in diverse C−P, C−S, C−O and C−N cross-coupling reactions. The proximity and cooperativity effects in LnNi-PHI significantly enhances the photo/Ni dual catalytic activity, thus resulting in low catalyst loadings and high turnover numbers.
AB - The development of heterogeneous metallaphotocatalysis is of great interest for sustainable organic synthesis. The rational design and controllable preparation of well-defined (site-isolated) metal/photo bifunctional solid catalysts to meet such goal remains a critical challenge. Herein, we demonstrate the incorporation of privileged homogeneous bipyridyl-based Ni-catalysts into highly ordered and crystalline potassium poly(heptazine imide) (K-PHI). A variety of PHI-supported cationic bipyridyl-based Ni-catalysts (LnNi-PHI) have been prepared and fully characterized by various techniques including NMR, ICP-OES, XPS, HAADF-STEM and XAS. The LnNi-PHI catalysts exhibit exceptional chemical stability and recyclability in diverse C−P, C−S, C−O and C−N cross-coupling reactions. The proximity and cooperativity effects in LnNi-PHI significantly enhances the photo/Ni dual catalytic activity, thus resulting in low catalyst loadings and high turnover numbers.
UR - http://www.scopus.com/inward/record.url?scp=85150416042&partnerID=8YFLogxK
U2 - 10.1038/s41467-023-37113-8
DO - 10.1038/s41467-023-37113-8
M3 - Article
C2 - 36932064
AN - SCOPUS:85150416042
SN - 2041-1723
VL - 14
JO - Nature Communications
JF - Nature Communications
IS - 1
M1 - 1501
ER -