透视乙二醇胺化钴催化剂的晶体平面依赖性

IF 3.9 2区化学 Q2 CHEMISTRY, PHYSICAL

Molecular Catalysis Pub Date : 2024-11-13 DOI:10.1016/j.mcat.2024.114655

Kai Li , De Zhang , Heqin Guo , Xinqi Yang , Congcong Liang , Xu Wu , Qiang Wang , Debao Li , Litao Jia

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引用次数: 0

摘要

Co 具有出色的脱氢和加氢活性，是乙二醇胺化反应的合适催化剂。然而，Co 不同晶面的催化活性尚不明确，这阻碍了其催化效率的进一步提高。本研究采用实验和理论方法，全面考察了 Co 的晶面效应对乙二醇胺化反应的影响。通过水热法合成了三种单晶 Co 催化剂，其晶面主要暴露在 (10-11)、(0001) 和 (11-20) 面上，并对其进行了乙二醇胺化评估。实验结果表明，具有暴露 Co (11-20) 晶面的 c-Co-R 催化剂具有最佳性能，乙二醇转化率为 55.4%，伯胺（乙二胺和乙醇胺）选择性为 43.7%。结合密度泛函理论计算和实验表征，结果表明，Co（11-20）表面表现出强劲的 C-H 键解离和对乙二醇的强吸附，从而显著提高了乙二醇的脱氢效率，改善了乙二醇的转化率。此外，NH3 的弱吸附能力进一步提高了目标产物的选择性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

Insight into crystal-plane-dependent of cobalt catalysts for ethylene glycol amination

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Insight into crystal-plane-dependent of cobalt catalysts for ethylene glycol amination

Co possesses outstanding dehydrogenation and hydrogenation activitiy and is a suitable catalyst for the amination of ethylene glycol. Nevertheless, the catalytic activity of Co's different crystal surfaces remains unclear, which hinders the further advancements in its catalytic efficiency. This research comprehensively examines the influence of Co's crystal plane effect on the amination of ethylene glycol employing both experimental and theoretical methodologies. Three single-crystal Co catalysts with mainly exposed (10−11), (0001) and (11−20) crystal planes were synthesized by a hydrothermal method and evaluated for ethylene glycol amination. The experimental results indicated that the c-Co-R catalyst with exposed Co (11–20) crystal facets exhibits optimal performance, with a 55.4 % ethylene glycol conversion and a 43.7 % primary amines (ethylenediamine and ethanolamine) selectivity. Combined with density-functional theory calculations and experimental characterization, the results showed that the Co (11−20) surface exhibited robust C-H bond dissociation and strong adsorption of ethylene glycol, which markedly improved the dehydrogenation efficiency of ethylene glycol and improved ethylene glycol conversion. Furthermore, the weak adsorption capacity of NH₃ further promoted the selectivity of the target products.

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来源期刊

Molecular Catalysis Chemical Engineering-Process Chemistry and Technology

CiteScore

6.90

自引率

10.90%

发文量

700

审稿时长

40 days

期刊介绍： Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods