Zhang Hanghang, Xu Gang
a, Polytechnic Institute, Zhejiang University Hangzhou 310015 China.
College of Chemical and Biological Engineering, Zhejiang University Hangzhou 310058 China
RSC Adv. 2025 Apr 1;15(13):9899-9909. doi: 10.1039/d5ra00463b. eCollection 2025 Mar 28.
Copper-based catalysts are widely employed in the catalytic conversion of aromatic compounds to phenolic derivatives. However, single-atom copper catalysts often exhibit limited reactivity and stability. In this study, we addressed these limitations by loading Cu onto NaY zeolite ion exchange to synthesize a CuY catalyst, followed by Yb modification. By optimizing the Yb content, we significantly enhanced the anisole conversion rate and guaiacol yield. Catalyst characterization revealed that Yb species modulate the electronic structure of copper, favoring the formation of abundant Cu species. This electronic modification promotes the catalytic generation of hydroxyl radicals (˙OH) from hydrogen peroxide, thereby accelerating the reaction kinetics. Furthermore, Yb incorporation into CuY induced the formation of oxygen vacancies, which improved hydroxyl radical adsorption and facilitated the generation of metal-oxo species. These synergistic effects collectively increased the reaction's overall conversion efficiency. Under optimized reaction conditions, the Yb/CuY catalyst achieved an anisole conversion of 56.2% and an -selectivity of 74.6%, clearly outperforming previous reports.
铜基催化剂广泛应用于芳香族化合物催化转化为酚类衍生物的过程中。然而，单原子铜催化剂的反应活性和稳定性往往有限。在本研究中，我们通过离子交换将铜负载到NaY沸石上合成了CuY催化剂，随后进行镱改性，以解决这些局限性。通过优化镱含量，我们显著提高了苯甲醚转化率和愈创木酚产率。催化剂表征表明，镱物种调节了铜的电子结构，有利于形成丰富的铜物种。这种电子修饰促进了过氧化氢催化生成羟基自由基(˙OH)，从而加快了反应动力学。此外，镱掺入CuY中诱导形成氧空位，改善了羟基自由基吸附并促进了金属氧物种的生成。这些协同效应共同提高了反应的整体转化效率。在优化的反应条件下，Yb/CuY催化剂的苯甲醚转化率达到56.2%，选择性达到74.6%，明显优于以往的报道。
