Jiangsu Province Key Laboratory of Fine Petrochemical Engineering, Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, School of Petrochemical and Engineering, Changzhou University, Changzhou, 213164, P.R. China.
State Key Laboratory of High-Efficiency Coal Utilization and Green Chemical Engineering, College of Chemistry and Chemical Engineering, Ningxia University, Yinchuan, 750021, P.R. China.
Environ Sci Pollut Res Int. 2024 Jul;31(35):47911-47922. doi: 10.1007/s11356-024-34375-7. Epub 2024 Jul 16.
It is desirable but challenging to develop highly-efficient catalysts for the direct synthesis of dimethyl carbonate (DMC) from methanol and CO. The vacancy-mediated incorporation of heteroatom into surface reconstruction is an efficient method of defect engineering for enhancing the catalytic properties. In this work, manganese-doped cerium oxide porous nanoribbons (Mn/CeO-BTC) were prepared derived from a Ce-BTC by a sacrificial template approach. It is found that the catalytic activity of Mn/CeO-BTC catalysts can be readily controlled by varying the amount of Mn dopants and the as-synthesized 0.1-Mn/CeO-BTC exhibited an outstanding activity for the synthesis of DMC from CO and methanol, which reached a high DMC yield (6.53 mmol/g) without any dehydrating agents. Based on characterization results, the enhanced performance may be attributed to the defective structures caused by Mn doping and the porous nanoribbons of the CeO crystals, which provide more surface oxygen vacancies and acidic-basic sites, favoring adsorption and activation of CO and methanol.
理想情况下，从甲醇和 CO 直接合成碳酸二甲酯（DMC）需要开发高效的催化剂。空位介导的杂原子掺入表面重构是一种有效的缺陷工程方法，可增强催化性能。在这项工作中，通过牺牲模板方法由 Ce-BTC 制备了锰掺杂氧化铈多孔纳米带（Mn/CeO-BTC）。结果发现，通过改变 Mn 掺杂量可以轻松控制 Mn/CeO-BTC 催化剂的催化活性，而合成的 0.1-Mn/CeO-BTC 在 CO 和甲醇合成 DMC 方面表现出出色的活性，无需任何脱水剂即可达到 6.53mmol/g 的高 DMC 收率。基于表征结果，性能的提高可能归因于 Mn 掺杂引起的缺陷结构和 CeO 晶体的多孔纳米带，这提供了更多的表面氧空位和酸碱位，有利于 CO 和甲醇的吸附和活化。
