Density functional theory study on catalytic performance of Si-doped and Mg-doped monoclinic ZrO2 for the direct synthesis of dimethyl carbonate from CO2 and methanol
Year: 2024
Type: article
Abstract: The direct synthesis of dimethyl carbonate ( DMC) from CO 2 and methanol over the single-atom Si-doped and Mg-doped hydroxylated monoclinic ( m ) ZrO 2 ( 1 ¯ 11 ) surface (named as SHM and MHM surfaces) was explored by density functional theory (DFT) calculations, which indicated that DMC formation originated from *CH 3 O reacting with *CH 3 OCO on both surfaces. Compared with the hydroxylated m -ZrO 2 ( 1 ¯ 11 ), the doping of Si atom significantly increased the catalytic activity , but the doping of Mg atom distinctly did the opposite. The excellent catalytic performance and adjusted reaction pathway on SHM surface were strongly attributed to the influence of decreased band gap greater than that of the enhanced Brønsted acidity. However, the hydroxyl group and hydrogen atom from the dissociation of H 2 O molecule on MHM surface were reduced to H 2 O molecule by the doping of single-atom Mg, which leaded to the inexistence of Brønsted acid site and the larger band gap for the decreased catalytic activity . The results provide a theoretical basis for the influences of the dopants on the catalytic performance of m -ZrO 2 , and help the design of high performance ZrO 2 catalysts for the direct synthesis of DMC.
Source: Materials Today Communications
Authors: Xuhui Wang, Jinxian Zhao, Shiping Wu, Ruina Shi, Jun Ren
Institutions: Shanxi University, Taiyuan University of Technology
Language: English
Subfield: Process Chemistry and Technology
Field: Chemical Engineering
Domain: Physical Sciences
Open Access status: hybrid
Estimated APC paid: $2,430
Awards: G3466613932, G5314786254
OpenAlex ID: W4401379311