Mechanistic Investigation of Dimethyl Carbonate Synthesis Over Palladium Chloride Catalyst

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2024-12-02 DOI:10.1007/s10562-024-04855-z

Zhi-Shen Huang, Zhang-Feng Zhou, Lu-Yang Qiao, Yun-Yun Zeng, Shan-Shan Zong, Yuan-Gen Yao

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Abstract

The production of dimethyl carbonate (DMC) from CO and methyl nitrite (MN) is of great industrial interest for chemicals upgrading. As one of the most efficient catalysts, PdCl₂ based catalyst has been widely investigated and been verified to be highly selective toward DMC yielding. However, the underlying mechanism is unclear so far. Herein, we identified the active sites and corresponding reaction pathway on PdCl₂ (140) surface by the density functional theory (DFT) calculations, combining with X-ray absorption fine structure (XAFS) and in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) measurements. The dissociation of MN resulted in the construction of Cl vacancies on PdCl₂ (140) surface, which are the specific sites for DMC formation. On the other hand, the continuous loss of Cl induced the reduction of PdCl₂ to Pd, leading to changed pathway of reaction and decreased yield of DMC. These insights highlighted the importance of Cl-balance in PdCl₂ based catalyst system, which determined the final products of CO oxidative esterification.

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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.