Preparation of CuOx@PC derived from Cu-BTC with polyvinylpyrrolidone and the catalytic performance for oxidative carbonylation of methanol to dimethyl carbonate

Abstract

A series of Cu-BTC with different Polyvinylpyrrolidone (PVP) assisted amounts were pyrolyzed to prepare carbon supported copper and its oxides (CuOx/C without PVP and CuOx@PC with PVP) derivant. The structure of Cu-BTC and derivant was characterized by XRD, SEM, TEM, N2 adsorption isotherms et al., and the derivant was applied for oxidative carbonylation of methanol to dimethyl carbonate. The results show that the introduction of PVP is beneficial to improve the specific surface area of CuOx@PC and generate Cu–Cu2O heterojunctions. The activities of the catalysts containing Cu–Cu2O heterojunctions are higher than that of the catalysts without Cu–Cu2O. Compared with CuOx/C, the space-time yield of CuOx@PC-2 of dimethyl carbonate is significantly enhanced from 948 mg g−1 h−1 to 1295 mg g−1 h−1. Cu–Cu2O has a synergistic effect on the catalytic performance. The stability of the catalysts was evaluated. After eight cycles, the deactivation rate of CuOx@PC-2 (53 %) is lower than that of CuOx/C (74 %), because the aggregation of Cu is inhibited by the introduction of PVP. And the oxidation of Cu species is mainly responsible for the deactivation of the catalysts.