Enhanced the Catalytic Performance of CeO2 by Tuning V5+ Doping Amount in Carbonylation of n-Butyl Amine with CO2

IF 2.3 4区化学 Q3 CHEMISTRY, PHYSICAL

Catalysis Letters Pub Date : 2024-09-12 DOI:10.1007/s10562-024-04806-8

Dalei Sun, Kang Cheng, Chen Zhou, Xiangye Liu, Zhiwu Liang

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Abstract

CO₂ regeneration and reutilization is considered to be a green and effective route with highly potential for development. CeO₂ showed high catalytic activity for the production of N,N′-dibutylurea through n-butyl amine and CO₂. Herein, V-doped CeO₂ with different molar ratios of V/Ce (V_x%-CeO₂, x = 0, 0.4, 0.6, 0.8 and 1.0) were further successfully synthesized and firstly applied to the reaction of CO₂ with n-butyl amine. The reaction results displayed the catalytic performance of CeO₂ were prominently enhanced by doping V⁵⁺ and followed an order of V_0.8%-CeO₂ > V_0.6%-CeO₂ > V_1.0%-CeO₂ > V_0.4%-CeO₂ > CeO₂. The reason for the changes in the catalytic activities of CeO₂ with different doping amounts of V⁵⁺ could be closely related to the surface oxygen vacancy and surface weak acidity and weak basicity based on specific analysis of relevant characterization including XRD, BET, Raman, XPS, EPR and NH₃/CO₂-TPD.

Graphical Abstract

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通过调节 V5+ 掺杂量提高 CeO2 在正丁基胺与 CO2 的羰基化反应中的催化性能

二氧化碳的再生和再利用被认为是一种极具发展潜力的绿色有效途径。CeO2 在通过正丁基胺和 CO2 生产 N,N′-二丁基脲方面表现出很高的催化活性。本文进一步成功合成了不同V/Ce摩尔比的掺V CeO2（Vx%-CeO2，x = 0、0.4、0.6、0.8和1.0），并首次应用于CO2与正丁胺的反应。反应结果表明，掺杂 V5+ 能显著提高 CeO2 的催化性能，其顺序为 V0.8%-CeO2 > V0.6%-CeO2 > V1.0%-CeO2 > V0.4%-CeO2 > CeO2。根据XRD、BET、拉曼、XPS、EPR和NH3/CO2-TPD等相关表征的具体分析，不同V5+掺杂量下CeO2催化活性变化的原因可能与表面氧空位、表面弱酸性和弱碱性密切相关。

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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.