Application of sorption-enhanced catalysis to ethanol reforming

Sammanfattning: Lithium orthosilicate (Li4SiO4) is known to be a high temperature CO2 capture material. This work was focused on comparing Li4SiO4 to the extensively studied CaO as an adsorbent in sorption enhanced catalysis. Thermogravimetric analysis was used to study the effects of sorption temperature and compaction on Li4SiO4 using 15vol% CO2 in N2. After 2 hours of CO2 adsorption at 550°C the powder reached 35wt% uptake of CO2, corresponding to 93.6% of maximum efficiency and complete regeneration was possible at 700°C. Pressing Li4SiO4 to granular forms greatly decreased CO2 adsorption rates. Efforts to impregnate -Al2O3 with the suspended SiO2 solution from aqueous based sol-gel synthesis to produce nanodispersed Li4SiO4 failed due to the inability to form the targeted Li4SiO4 complex. X-ray diffraction analysis indicated the formation of the gel is crucial for the formation of the crystalline Li4SiO4 phase. A microreactor was used to study the steam reforming of ethanol over a series of 1% Pt on -Al2O3 catalyst composite impregnated over a range of nanodispersed CaO loading at S/C=1.5 in dilution. At 400°C enhancement could be observed with the presence of CaO sorbent compared to only 1% Pt/Al2O3. However, production quickly diminished due to high carbon deposition. For 1% Pt/Al2O3 tested at 400°C, ethylene production was 5 times higher than for hydrogen. Above 550°C the ethylene production was reduced to 0.18vol% and gas production stability was greatly improved for 1% Pt/Al2O3 and even more so with the addition of impregnated CaO sorbent. Hydrogen yields from homogeneous mixtures of 1%Pt/Al2O3 with Li4SiO4 powder in a microreactor were about 20% higher than those achievable of the same mixture with CaO powder. However, the composite 1%Pt/Al2O3 with 7.02wt% dispersed CaO gave 100% higher hydrogen production under similar conditions despite Li4SiO4 being a superior carbon capture material.