Pt-MoO3/TiO2催化氨基酸选择性加氢的双功能活性位点研究

IF 7.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yundao Jing, Xiaohu Ge, Rui Song, Ningchao Zhu, Jinquan Ming, Nihong An, Yueqiang Cao, Gang Qian, Xuezhi Duan, Xing-Gui Zhou
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引用次数: 0

摘要

氨基酸选择性氢化为氨基醇是合成药物、精细化学品和手性构建块的一种有价值的转化。然而,由于需要同时进行氢活化和底物配位,在温和条件下实现高活性和选择性仍然具有挑战性。在这里,我们报道了一系列的Pt-MoO3双功能催化剂,用于l -丙氨酸(Ala)加氢成丙氨酸醇(AlaOH),重点是调节金属氧化物协同作用。通过高角环形暗场扫描透射电镜、x射线光电子能谱和x射线吸附能谱等手段进行结构和电子表征,发现Pt-MoO3相互作用强,以部分电子转移为特征。催化试验表明,Pt/Mo比对火山型催化剂具有依赖性,其中4-Pt-MoO3催化剂的性能最高。H2温度程序解吸实验和原位弥反射红外傅里叶变换光谱结合理论计算,支持了Pt作为H2活化的主要位点,MoO3促进极性丙氨酸的吸附和稳定的双功能机制。通过热处理进一步调整表明,在500 °C的适度处理下,MoO3的氧化还原状态得到了最佳平衡,而不影响Pt的分散,从而提高了加氢性能。这项工作不仅促进了对金属-氧化物界面催化的认识,而且为高效选择性加氢氨基酸提供了合理的设计策略。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Insights into bifunctional active sites of Pt-MoO3/TiO2 catalyst enabling selective hydrogenation of amino acid
Selective hydrogenation of amino acids to amino alcohols is a valuable transformation in the synthesis of pharmaceuticals, fine chemicals, and chiral building blocks. However, achieving high activity and selectivity under mild conditions remains challenging due to the need for simultaneous hydrogen activation and substrate coordination. Here, we report a series of Pt–MoO3 bifunctional catalysts for the hydrogenation of L-alanine (Ala) to alaninol (AlaOH), with a focus on tuning metal–oxide synergy. Structural and electronic characterization by high-angle annular dark-field scanning transmission electron microscopy, X-ray photoelectron spectroscopy and X-ray adsorption spectroscopy reveal strong Pt–MoO3 interactions, characterized by partial electron transfer. Catalytic tests reveal a volcano-type dependence on Pt/Mo ratio, with the 4-Pt-MoO3 catalyst achieving the highest performance. The experiments of H2 temperature programmed desorption and in-situ diffuse reflectance infrared Fourier transform spectroscopy combined with theoretical calculations support a bifunctional mechanism, in which Pt serves as the primary site for H2 activation, while MoO3 facilitates adsorption and stabilization of polar alanine. Further tuning via thermal treatments show that the moderate treatment at 500 °C optimally balances the redox state of MoO3 without compromising Pt dispersion, leading to enhanced hydrogenation performance. This work not only advances understanding of metal-oxide interfacial catalysis but also provides a rational design strategy for efficient and selective hydrogenation amino acid.
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来源期刊
Chemical Science
Chemical Science CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
4.80%
发文量
1352
审稿时长
2.1 months
期刊介绍: Chemical Science is a journal that encompasses various disciplines within the chemical sciences. Its scope includes publishing ground-breaking research with significant implications for its respective field, as well as appealing to a wider audience in related areas. To be considered for publication, articles must showcase innovative and original advances in their field of study and be presented in a manner that is understandable to scientists from diverse backgrounds. However, the journal generally does not publish highly specialized research.
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