ABSTRACT
Deuterium-labeled polyols are one of the most extensive applied chemicals in biochemistry and biophysics. However, the deuteriation still is insufficient, exhibiting a low deuterated ratio and indistinct reaction mechanism. Herein, Ru supported on MnBCD (MnBDC, derived from Mn p-phthalic acid metal-organic framework) as nanocatalyst with an agglomerated sheet-type structure; this allows the possibility of achieving both thermo- and electrocatalytic hydrogen isotope exchange (HIE) reaction. Furthermore, XPS characterization confirmed that the specific structural changes in the electron density of Ru outer layers were modulated through the impregnation and reduction processes. According to the change of outer electronic structure, hydrogen spillover and electron-rich flow promote the reaction of the catalyst in thermo- and electrocatalytic systems, respectively. In addition, the results indicate that a high deuterated ratio of 97 % can be obtained, hence the catalytic technology has enormous potential for the synthesis of a broad variety of deuterium-labeled compounds.
ABSTRACT
The catalytic conversion of CO or CO/CO2 mixtures to higher alcohols (HAs) using hydrogenation reactions remains challenging in C1 chemistry and also one of the most promising reactions for the utilization of non-petroleum resources. Here, the experiment and characterization tests of CuCoMn/Al2O3 show that copper is much more dispersed on γ-Al2O3 than cobalt, and the interaction between cobalt and Mn metals is stronger. And, mixed cobalt-manganese oxides are formed in the calcined catalyst, promoting the formation of higher alcohols. Under the optimum conditions, the catalyst demonstrated a total alcohol selectivity of 44.6%, and the fraction of higher alcohols reached up to 85.3% among the total alcohol products, which is superior to the classical modified CuCo-based catalysts. And in the gas mixture reaction with a CO : CO2 ratio of 8 : 2, the conversion rate of the catalyst to CO and CO2 reached 34.8% and 27.3%, respectively, and the selectivity (C1+ slate 1-alcohol) was 53.2%.
