Oxygen vacancies-promoted oxidative esterification of ethylene glycol to methyl glycolate over Au/ZnO catalyst

IF 6.3 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Applied Surface Science Pub Date : 2024-11-21 DOI:10.1016/j.apsusc.2024.161855

Yanhong Quan, Zihui Qin, Xueyang Ren, Jun Ren

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Abstract

Au/ZnO-x with different morphologies were prepared by controlling the amount of (NH₄)₂CO₃ (x) using deposition precipitation method and applied for the one-step oxidative esterification of methanol and ethylene glycol (EG) to methyl glycolate (MG). The catalytic performance of Au/ZnO-x firstly increases and then decreases with the increase of the amount of (NH₄)₂CO₃, and the maximum is achieved in Au/ZnO-4, with EG conversion of 89.6 % and 96.4 % selectivity to MG, significantly higher than the reported Au-based catalysts. The superior catalytic behavior is mainly derived from the most oxygen vacancy concentration (V_o⁺) accompanied with the highest I₁₀₀/I₁₀₁ ratio at moderate (NH₄)₂CO₃ dosage, promoting the adsorption and dissociation of O₂ molecular. Specifically, different preferential growth ratio between the (100) and (101) crystal plane accounts for Au/ZnO-2, Au/ZnO-4, and Au/ZnO-6 with lamellar stacking morphology, orderly layer structure, and randomly stacked layers, respectively. Significantly, it was found that there was a linear positive correlation between the V_o⁺ and the EG conversion. Innovatively, the oxygen vacancy played the predominant role in Au/ZnO-x for the catalyzed oxidative esterification of EG, which provided a new idea for the design of efficient catalysts for the reaction.

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金/氧化锌催化剂上氧空位促进的乙二醇氧化酯化反应生成乙醇酸甲酯

利用沉积沉淀法，通过控制（NH4）2CO3（x）的用量制备了不同形貌的 Au/ZnO-x，并将其应用于甲醇和乙二醇（EG）一步氧化酯化制乙醇酸甲酯（MG）。Au/ZnO-x 的催化性能随着（NH4）2CO3 量的增加先增大后减小，在 Au/ZnO-4 中达到最大，EG 转化率为 89.6%，对 MG 的选择性为 96.4%，明显高于已报道的金基催化剂。这种优异的催化性能主要源于在中等（NH4）2CO3 用量下，氧空位浓度（Vo+）最高，同时 I100/I101 比值最大，促进了 O2 分子的吸附和解离。具体而言，(100)和(101)晶面之间不同的优先生长比分别导致 Au/ZnO-2、Au/ZnO-4 和 Au/ZnO-6 具有片状堆叠形态、有序层结构和不规则团簇。值得注意的是，研究发现 Vo+ 与 EG 转化率之间存在线性正相关。创新性地提出了氧空位催化 EG 氧化酯化反应的机理，为设计该反应的高效催化剂提供了新思路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Applied Surface Science 工程技术-材料科学：膜

CiteScore

12.50

自引率

7.50%

发文量

3393

审稿时长

67 days

期刊介绍： Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.