Abstract
Aldol condensation of the syngas-methanol derivatives is an important renewable route for acrylic acid production and coal clean-efficient utilization. In this work, a series of mesoporous alkaline earth metal (x) oxide-modified VPxO/SiO2 catalysts were designed and prepared for gas-aldol condensation of formaldehyde and acetic acid to acrylic acid. The doping of alkaline earth metal oxide into VPO/SiO2 effectively promoted the dispersion and exposure of the VPO species and adjusted the amount of surface (VO)2P2O7/γ-VOPO4 (V4+/V5+). Especially, the SrO and BaO obviously altered the surface chemical environment of VPO species and the strength of acid-base sites, exhibiting strong interaction with both (VO)2P2O7 and γ-VOPO4. The formaldehyde conversion and acrylic acid selectivity over the VPxO/SiO2 increased with about 5.0–10.0 % and 8.0–16.0 % comparing with the VPO/SiO2, respectively. By optimizing the doping amount of BaO and reaction temperature, the VPBaO/SiO2 catalyst achieved a formaldehyde conversion of 70.4 % and an acrylic acid yield of approximately 65.5 % (with formation rate of 12.5 mmol gcat−1 h−1). The VPxO/SiO2 catalysts also showed slightly improved catalytic stability than the VPO/SiO2.
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