Sendaner Adelieti, Si-Qi Wu, Xian-Hao Wu, Rong Guo, Jian-Shan Chen, Zhi-Fang Diao, Zi-Yi Miao, Zhen-Hong Han, Ye-Yan Qin, Yuan-Gen Yao
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引用次数: 0
摘要
亚硝酸盐甲酯（MN）羰基化合成碳酸二甲酯（DMC）是一条很有前途的途径，但缺乏高效稳定的催化剂仍然是大规模应用的主要挑战。本研究通过调节初始凝胶的碱度，合成了酸度可调的NaY分子筛，并优化了Lewis酸位的数量。适量的Lewis酸位点促进了NaY分子筛与Pd的相互作用，有利于稳定Pd的氧化态，促进CO的吸附和活化，从而促进关键中间体*COOCH3的形成。催化剂PdCu/NaY-1（初始凝胶中碱度Na2O=9）对DMC的催化性能有显著改善，WTYDMC为1604 g kgcat−1⋅h−1，CO对DMC （CCO）的转化率为88.7%，基于CO （SDMC/CO）的DMC选择性高达100%。
Effect of Gel Alkalinity on the Catalytic Properties of PdCu/NaY Zeolites for Methyl Nitrite Carbonylation to Dimethyl Carbonate
The carbonylation of methyl nitrite (MN) to synthesize dimethyl carbonate (DMC) is a promising route, but the lack of efficient and stable catalysts remains a major challenge for large-scale applications. In this study, by adjusting the alkalinity of the initial gel, NaY zeolites with tunable acidity were synthesized, and the amount of Lewis acid sites was optimized. Appropriate amounts of Lewis acid sites facilitated the interaction between NaY zeolites and Pd species, which was beneficial for stabilizing the oxidation state of Pd and promoting CO adsorption and activation, thereby contributing to the formation of the key intermediate *COOCH3. The catalyst PdCu/NaY-1 (alkalinity in the initial gel Na2O=9) exhibited significant improvement in catalytic performance for the synthesis of DMC, with the WTYDMC of 1604 g kgcat−1⋅h−1, the conversion of CO to DMC (CCO) of 88.7 %, and the DMC selectivity based on CO (SDMC/CO) up to 100 %.
期刊介绍：
Helvetica Chimica Acta, founded by the Swiss Chemical Society in 1917, is a monthly multidisciplinary journal dedicated to the dissemination of knowledge in all disciplines of chemistry (organic, inorganic, physical, technical, theoretical and analytical chemistry) as well as research at the interface with other sciences, where molecular aspects are key to the findings. Helvetica Chimica Acta is committed to the publication of original, high quality papers at the frontier of scientific research. All contributions will be peer reviewed with the highest possible standards and published within 3 months of receipt, with no restriction on the length of the papers and in full color.
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