Impact of Water Content on UiO-66 Synthesis and Catalyst Activation in Pd/UiO-66 Catalyzed Methyl Nitrite Carbonylation to Dimethyl Carbonate

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2025-09-20 DOI:10.1007/s10562-025-05178-3

Qiuyun Huang, Shiyu Liu, Weihua Shen, Yunjin Fang

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Abstract

Due to the modifiable properties and excellent stability, metal-organic frameworks (MOFs) are considered potential catalyst supports in heterogeneous reactions. UiO-66 with varying water contents were synthesized as supports of Pd for the carbonylation of methyl nitrite (MN) to dimethyl carbonate (DMC). In accordance with XRD, NH₃-TPD, and SEM, the water contents showed a negative correlation on the amounts of acid sites and accelerated crystal aggregation. The Pd/UiO-66(x) demonstrated perfect selectivity of DMC (> 99%) and good CO conversion which were increased with the decrease of water contents. Moreover, the catalysts deactivated at the beginning of the reaction, and the catalytic deactivation was due to the damage of the C = O structure in UiO-66 frameworks. This work revealed the influence of water contents on the synthesis of UiO-66 and the deactivation process of MOF-based catalysts in MN carbonylation to DMC.

Graphical Abstract

Abstract Image

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水含量对UiO-66合成及Pd/UiO-66催化亚硝酸盐甲酯羰基化制碳酸二甲酯催化剂活化的影响

由于金属有机骨架具有可修饰的性质和优异的稳定性，被认为是多相反应中潜在的催化剂载体。合成了不同含水量的UiO-66作为钯的载体，用于亚硝酸盐甲酯（MN）羰基化制碳酸二甲酯（DMC）。XRD、NH3-TPD和SEM分析表明，水的含量与酸位的数量和晶体加速聚集呈负相关。Pd/UiO-66(x)对DMC具有良好的选择性（> 99%）， CO转化率随含水量的降低而提高。催化剂在反应开始时失活，失活的原因是UiO-66框架中C = O结构的破坏。本工作揭示了水含量对UiO-66合成的影响以及mof基催化剂在MN羰基化制DMC过程中的失活过程。图形抽象

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来源期刊

Catalysis Letters 化学-物理化学

CiteScore

5.70

自引率

3.60%

发文量

327

审稿时长

1 months

期刊介绍： Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis. The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.