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Gallium‐Based Eutectic Alloys as Liquid Electron Donors to Ruthenium Single‐Atom Catalysts for Selective Hydrogenation of Vanillin
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2025-03-19 , DOI: 10.1002/anie.202505073
Jia Song 1 , Jianuo Liu 1 , Xiaorong Zhu 2 , Xiaoming Mou 3 , Handuo Zheng 4 , Huang Zhou 1 , Wenyu Wang 1 , Yong Guan 5 , Jun Tang 1 , Yue Lin 1 , Lirong Zheng 6 , Tao Yao 5 , Juncai Dong 6 , Shiqiang Wei 5 , Weixin Huang 1 , Lin Gu 7 , Jun Luo 8 , Yafei Li 2 , Yafei Zhao 1 , Yuen Wu 9
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2025-03-19 , DOI: 10.1002/anie.202505073
Jia Song 1 , Jianuo Liu 1 , Xiaorong Zhu 2 , Xiaoming Mou 3 , Handuo Zheng 4 , Huang Zhou 1 , Wenyu Wang 1 , Yong Guan 5 , Jun Tang 1 , Yue Lin 1 , Lirong Zheng 6 , Tao Yao 5 , Juncai Dong 6 , Shiqiang Wei 5 , Weixin Huang 1 , Lin Gu 7 , Jun Luo 8 , Yafei Li 2 , Yafei Zhao 1 , Yuen Wu 9
Affiliation
Tuning the catalytic pathways of atomically dispersed single‐atom catalysts (SAC) has emerged as an effective strategy to optimize their overall catalytic activity. Herein, we present Ru1@m‐tube, a hollow carbon nitride‐supported Ru SAC, coated with eutectic galinstan (GaInSn), as a model catalyst, we demonstrate a performance inversion in vanillin conversion. Vanillin, as a biomass‐derived compound with industrial relevance, presents challenges in catalytic hydrogenation, making it an ideal model reaction to test and compare the catalyst's selectivity and efficiency. The as‐obtained Ru1@m‐tube(GaInSn) achieved nearly 100% vanillin conversion within 5 hours and exhibited an impressive 93.8% selectivity for vanillyl alcohol . Electron spillover from gallium‐based eutectic alloys to highly diluted ruthenium sites enhances the desorption of vanillyl alcohol, resulting in an exceptional performance shift between hydrogenation and hydrodeoxygenation. Our findings not only offer a novel approach for modulating SAC performance via liquid‐metal interfaces but also expand the understanding of promoter screening for various challenging reactions.
中文翻译:
镓基共晶合金作为钌单原子催化剂的液电子供体,用于香兰素的选择性加氢反应
调整原子分散的单原子催化剂 (SAC) 的催化途径已成为优化其整体催化活性的有效策略。在此,我们提出了Ru1@m管,一种空心氮化碳负载的 Ru SAC,涂有共晶加林斯坦 (GaInSn),作为模型催化剂,我们展示了香兰素转化中的性能反转。香兰素作为一种具有工业意义的生物质衍生化合物,在催化加氢方面提出了挑战,使其成为测试和比较催化剂选择性和效率的理想模型反应。所获得的Ru1@m管 (GaInSn) 在 5 小时内实现了近 100% 的香兰素转化率,并且对香草醇表现出令人印象深刻的 93.8% 选择性。从镓基共晶合金到高度稀钌位点的电子溢出增强了香草醇的解吸,从而在加氢和加氢脱氧之间实现了非凡的性能转变。我们的研究结果不仅提供了一种通过液态-金属界面调节 SAC 性能的新方法,而且还扩展了对各种具有挑战性反应的启动子筛选的理解。
更新日期:2025-03-19
中文翻译:

镓基共晶合金作为钌单原子催化剂的液电子供体,用于香兰素的选择性加氢反应
调整原子分散的单原子催化剂 (SAC) 的催化途径已成为优化其整体催化活性的有效策略。在此,我们提出了Ru1@m管,一种空心氮化碳负载的 Ru SAC,涂有共晶加林斯坦 (GaInSn),作为模型催化剂,我们展示了香兰素转化中的性能反转。香兰素作为一种具有工业意义的生物质衍生化合物,在催化加氢方面提出了挑战,使其成为测试和比较催化剂选择性和效率的理想模型反应。所获得的Ru1@m管 (GaInSn) 在 5 小时内实现了近 100% 的香兰素转化率,并且对香草醇表现出令人印象深刻的 93.8% 选择性。从镓基共晶合金到高度稀钌位点的电子溢出增强了香草醇的解吸,从而在加氢和加氢脱氧之间实现了非凡的性能转变。我们的研究结果不仅提供了一种通过液态-金属界面调节 SAC 性能的新方法,而且还扩展了对各种具有挑战性反应的启动子筛选的理解。