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Highly active catalysis of methanol oxidative carbonylation over nano Cu2O supported on micropore-rich mesoporous carbon
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2021-11-06 , DOI: 10.1016/j.apcatb.2021.120890
Jiajun Wang 1 , Tingjun Fu 1 , Fanhui Meng 1 , Dan Zhao 1 , Steven S.C. Chuang 2 , Zhong Li 1
Affiliation  

A micropore-rich mesoporous carbon (MMC) derived from ordered mesoporous carbon (OMC) is fabricated as support to prepare a highly active nano Cu2O catalyst for methanol oxidation carbonylation. The well-dispersed ~3.3 nm Cu nanoparticles with ca. 90% purity of Cu2O are obtained. The space-time yield and turnover frequency of DMC are significantly enhanced to 34.2ggCu1h1 and 89.1 h−1, both of which are greater than that over the mesoporous-only Cu/OMC catalyst. It is found that plentiful under-coordinated carbon atoms are formed in the introduced micropores, which serve as binding sites to immobilize Cu precursors to form the well-dispersed Cu nanoparticles. A large number of these atoms are favorable to accelerate auto-reduction of CuO to Cu2O in kinetics and further promote to form high-purity Cu2O. Besides, the electrons of Cu2O are forced to transfer to the micropore surrounding, forming an electron-deficient Cu+ site in favor of intrinsic activity enhancement.



中文翻译:

富微孔介孔碳负载纳米Cu2O上甲醇氧化羰基化的高活性催化

由有序介孔碳(OMC)衍生的富含微孔的介孔碳(MMC)作为载体制备用于甲醇氧化羰基化的高活性纳米Cu 2 O催化剂。分散良好的~3.3 nm Cu纳米颗粒,具有约。获得90%纯度的Cu 2 O。DMC 的时空产率和周转频率显着提高到34.2GG-1H-1和 89.1 h -1,这两者都大于仅介孔 Cu/OMC 催化剂。发现在引入的微孔中形成了大量未配位的碳原子,这些碳原子作为结合位点固定 Cu 前驱体以形成分散良好的 Cu 纳米颗粒。大量这些原子有利于在动力学上加速CuO自动还原为Cu 2 O,进一步促进形成高纯度Cu 2 O。此外,Cu 2 O的电子被迫转移到周围的微孔中,形成缺电子的 Cu +位点,有利于提高本征活性。

更新日期:2021-11-18
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