“…Pd 3d and P 2p high-resolution XPS spectra of BP1-Pd(BU) and BP1-Pd(PS) COFs are shown in Figure 4, while the C 1s, B 1s, and O 1s HR-XPS spectra regions and analogous spectra for BP2-derived hybrid materials are placed in the SI (Figures S33-S36). [49] As indicated by the analysis of Pd 3d region, two different Pd species can be distinguished. The doublet at binding energies (B.E) of 341.5 eV (Pd 3d 3/2 ) and 336.3 eV (Pd 3d 5/2 ) can be assigned to bulk palladium nanoparticles-(Pd(bulk), Table 1).…”
We have demonstrated that the general approach to phosphine coordination materials, mostly developed for MOF families, can be successfully extended to Covalent Organic Frameworks. Consequently,w eh ave obtained as eries of COFs comprising both Lewis acid boron and Lewis base P III /P=Os ites. These bifunctional COFs showed significant gas sorption ability and can be easily functionalized with metal atoms using both post-synthetic and bottom-up approaches. The DFT calculations on framework-guest interactions revealed that the behavior of adjacent boron and P III /P=Oc enters is reminiscent of that found in Frustrated Lewis Pairs.
“…Pd 3d and P 2p high-resolution XPS spectra of BP1-Pd(BU) and BP1-Pd(PS) COFs are shown in Figure 4, while the C 1s, B 1s, and O 1s HR-XPS spectra regions and analogous spectra for BP2-derived hybrid materials are placed in the SI (Figures S33-S36). [49] As indicated by the analysis of Pd 3d region, two different Pd species can be distinguished. The doublet at binding energies (B.E) of 341.5 eV (Pd 3d 3/2 ) and 336.3 eV (Pd 3d 5/2 ) can be assigned to bulk palladium nanoparticles-(Pd(bulk), Table 1).…”
We have demonstrated that the general approach to phosphine coordination materials, mostly developed for MOF families, can be successfully extended to Covalent Organic Frameworks. Consequently,w eh ave obtained as eries of COFs comprising both Lewis acid boron and Lewis base P III /P=Os ites. These bifunctional COFs showed significant gas sorption ability and can be easily functionalized with metal atoms using both post-synthetic and bottom-up approaches. The DFT calculations on framework-guest interactions revealed that the behavior of adjacent boron and P III /P=Oc enters is reminiscent of that found in Frustrated Lewis Pairs.
Two covalent organic frameworks comprising Lewis basic P III centers and Lewis acidic boron atoms were prepared by poly-condensation reactions of newly obtained tris(4-diisopropoxyborylphenyl)phosphine with 2,3,6,7,10,11hexahydroxytriphenylene and 2,3,6,7-tetrahydroxy-9,10-dimethylanthracene. Obtained materials exhibit significant sorption of dihydrogen (100 cm 3 g À1 at 1 bar at 77 K), methane (20 cm 3 g À1 at 1 bar at 273 K) and carbon dioxide (50 cm 3 g À1 at 1 bar at 273 K). They were exploited as solidstate ligands for coordination of Pd 0 centers. Alternatively, in a bottom-up approach, boronated phosphine was treated with Pd 2 dba 3 and poly-condensated, yielding hybrid materials where the polymer networks are formed by means of covalent boronate linkages and coordination PÀPd bonds. In addition, the analogous materials based on phosphine oxide were synthesized. The DFT calculations on framework-guest interactions revealed that the behavior of adjacent boron and phosphorus/phosphine oxide centers is reminiscent of that found in Frustrated Lewis Pairs and may improve sorption of selected molecules.
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