A series
of basicity-tunable ionic liquids with carboxylate and
sulfonate anion were designed, prepared, and applied in NO capture.
Both high absorption capacity and low desorption residue were achieved
through tuning the basicity of the anion, leading to a superhigh working
capacity of more than 6 mol per mol ionic liquid, which is superior
to that of traditional absorbents. Through a combination of absorption
experiments, quantum chemical calculations, and spectroscopic investigations,
the results indicated that such a high absorption capacity was originated
from multiple sites interaction between oxygen atoms of carboxylate
or sulfonate anion and NO, while the reduced interaction induced by
the decreased basicity of the O-site ionic liquid led to excellent
desorption. We show that the highly efficient and reversible NO capture
by these tunable ionic liquids provides a new strategy for improving
gas capture and utilization, which is also important for some other
fields such as material, biology, and medicine.
The strong chemisorption of CO2 is always accompanied by a high absorption enthalpy, and traditional methods to reduce the absorption enthalpy lead to decreased CO2 capacities. Through the introduction of a large π-conjugated structure into the anion, a dual-tuning approach for the improvement of CO2 capture by anion-functionalized ionic liquids (ILs) resulted in a high capacity of up to 0.96 molCO2 mol-1IL and excellent reversibility. The increased capacity and improved desorption were supported by quantum chemical calculations, spectroscopic investigations, and thermogravimetric analysis. The increased capacity may be a result of the strengthened dynamic covalent bonds in these π-electron-conjugated structures through anion aggregation upon the uptake of CO2 , and the improved desorption originates from the charge dispersion of interaction sites through the large π-electron delocalization. These results provide important insights into effective strategies for CO2 capture.
A synchronous strategy for improving the absorption/desorption to achieve highly efficient nitric oxide (NO) capture is proposed by the use of tetrakis(azolyl)borate ionic liquid (IL) [P 66614 ][B(Im) 4 ] with multiple nonconjugated interaction sites. This IL exhibited an ultrahigh absorption capacity up to 8.13 mol of NO per mol of IL, good desorption, and excellent reversibility. Through a combination of absorption experiments, DFT calculations, and FT-IR and NMR characterizations, the results indicate that the ultrahigh NO capacity by [P 66614 ][B(Im) 4 ] originated from multiple-sites chemisorption through the formation of diazeniumdiolates (NONOates), while uniform interaction of multiple nonconjugated sites was responsible for the unusual S-shaped absorption isobar, leading to good desorption and excellent reversibility, which was different from traditional ILs. We believe this work provides a new method for designing highly efficient gas absorbents.
The facile fabrication of low-cost and high active catalysts for selective hydrogenolysis of 5-hydroxymethlfurfural (5-HMF) to 2,5-dimethylfuran (2,5-DMF) using renewable and economical ethanol as hydrogen donor is still a significant...
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