Efficient adsorptive separation of propylene/propane (C 3 H 6 /C 3 H 8 )i sh ighly desired and challenging.K nown strategies focus on either the thermodynamic or the kinetic mechanism. Here,w er eport an interesting reactivity of am etal-organic framework that improves thermodynamic and kinetic adsorption selectivity simultaneously.W hen the metal-organic framework is heated under oxygen flow, half of the soft methylene bridges of the organic ligands are selectively oxidized to form the more polar and rigid carbonyl bridges. Mixture breakthrough experiments showed drastic increase of C 3 H 6 /C 3 H 8 selectivity from 1.5 to 15. Forc omparison, the C 3 H 6 /C 3 H 8 selectivities of the best-performing metal-organic frameworks Co-MOF-74 and KAUST-7 were experimentally determined to be 6.5 and 12, respectively.G as adsorption isotherms/kinetics,s ingle-crystal X-ray diffraction, and computational simulations revealed that the oxidation gives additional guest recognition sites,w hich improve thermodynamic selectivity,a nd reduces the framework flexibility,w hich generate kinetic selectivity.
High-efficiency electrocatalysts
for CO2 reduction reaction
are extremely desirable to produce valuable hydrocarbon productions,
as well as addressing the current environmental challenges. In this
work, we introduce a Cu-based metal–organic framework as a
catalyst for the efficient and selective reduction of CO2 to CH4 in neutral aqueous electrolytes. Detailed examination
of [Cu
4
ZnCl4(btdd)3]
(Cu
4
-MFU-4l
, H2btdd = bis(1H-1,2,3-triazolo-[4,5-b],[4′,5′-i])dibenzo-[1,4]-dioxin)
revealed the highest activity for yielding methane with a Faradaic
efficiency of 92%/88% and a partial current density of 9.8/18.3 mA
cm–2 at a potential of −1.2/–1.3 V
(vs RHE). In situ X-ray absorption and infrared spectroscopy
spectra, as well as density functional theory calculations, revealed
that the in situ generated trigonal pyramidal Cu(I)N3 acts as the electrochemical active site and that the strong
coordination ability of the Cu(I)N3 site and the synergistic
effect of adjacent aromatic hydrogen atoms, via hydrogen-bonding
interactions, play an important role in stabilizing the key intermediates
of carbon dioxide reduction and inhibiting the hydrogen evolution
reaction, thus showing a high performance of electroreduction of CO2 to CH4.
These results demonstrated that the TSR is a new prognostic factor for NSCLC. Stroma-poor tumors were associated with longer disease-free period and better prognosis than were stroma-rich tumors in NSCLC patients. The TSR may contribute to the development of individualized treatment for NSCLC in the future.
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