Integrating Photoactive Ligands into Crystalline Ultrathin 2D Metal-Organic Framework Nanosheets for Efficient Photoinduced Energy Transfer.

Autor: Lin H; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Yang Y; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Diamond BG; Department of Chemistry, University of Oregon, Eugene, Oregon 97403, United States., Yan TH; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Bakhmutov VI; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Festus KW; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Cai P; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Xiao Z; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Leng M; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Afolabi I; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Day GS; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Fang L; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States., Hendon CH; Department of Chemistry, University of Oregon, Eugene, Oregon 97403, United States., Zhou HC; Department of Chemistry, Texas A&M University, College Station, Texas 77843, United States.
Jazyk: angličtina
Zdroj: Journal of the American Chemical Society [J Am Chem Soc] 2024 Jan 17; Vol. 146 (2), pp. 1491-1500. Date of Electronic Publication: 2024 Jan 03.
DOI: 10.1021/jacs.3c10917
Abstrakt: 3D metal-organic frameworks (MOFs) have gained attention as heterogeneous photocatalysts due to their porosity and unique host-guest interactions. Despite their potential, MOFs face challenges, such as inefficient mass transport and limited light penetration in photoinduced energy transfer processes. Recent advancements in organic photocatalysis have uncovered a variety of photoactive cores, while their heterogenization remains an underexplored area with great potential to build MOFs. This gap is bridged by incorporating photoactive cores into 2D MOF nanosheets, a process that merges the realms of small-molecule photochemistry and MOF chemistry. This approach results in recyclable heterogeneous photocatalysts that exhibit an improved mass transfer efficiency. This research demonstrates a bottom-up synthetic method for embedding photoactive cores into 2D MOF nanosheets, successfully producing variants such as PCN-641-NS, PCN-643-NS, and PCN-644-NS. The synthetic conditions were systematically studied to optimize the crystallinity and morphology of these 2D MOF nanosheets. Enhanced host-guest interactions in these 2D structures were confirmed through various techniques, particularly solid-state NMR studies. Additionally, the efficiency of photoinduced energy transfer in these nanosheets was evidenced through photoborylation reactions and the generation of reactive oxygen species (ROS).
Databáze: MEDLINE