Lewis Acidic Zeolite-Encapsulated Bimetallic Au–Pt Nanoparticles as Robust Catalysts for the Conversion of Glycerol to Methyl Lactate

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Bo Tang*, , , Xu Zuo, , , Ang Li, , , Jiajun Wang, , , Haojun Zou, , , Lili Xu, , and , Weili Dai*, 
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引用次数: 0

Abstract

Alkyl lactates can be produced via a glycerol oxidation-rearrangement route, which is a promising alternative to the microbial fermentation-based technology but is still hindered by the lack of an efficient catalyst. Herein, we reported the successful fabrication of well-defined bimetallic Au–Pt nanoparticles confined inside the Snβ zeolite, i.e., AuxPty@Snβ, using a mercaptosilane-assisted structure reconstruction strategy. Owing to the synergistic effect of bimetallic Au–Pt species and the unique Lewis acidic framework Sn, the optimized Au1Pt3@Snβ demonstrated superior catalytic performance in the conversion of glycerol to methyl lactate, achieving a 78.8% methyl lactate yield and a TOF of 335 h–1 at 413 K and 0.5 MPa air, which surpasses most previously reported heterogeneous catalysts under similar reaction conditions. The confinement environment of zeolite can not only provide spatial restriction but also induce a strong interaction between encapsulated Au–Pt nanoparticles and framework Sn, thus inhibiting metal sintering and leaching during catalysis. Experimental and theoretical calculations (DFT) results explicated the critical role of bimetallic Au–Pt synergy in activating O2 and facilitating a lower energy barrier for glycerol dehydrogenation, thereby promoting the catalytic performance.

Abstract Image

Abstract Image

Lewis酸性沸石包封双金属Au-Pt纳米颗粒作为甘油转化为乳酸甲酯的稳健催化剂
通过甘油氧化重排的方法制备乳酸烷基酯是一种很有前途的替代微生物发酵技术,但由于缺乏有效的催化剂而受到阻碍。在此,我们报道了利用巯基硅烷辅助结构重建策略,成功地在Snβ沸石(即AuxPty@Snβ)内制备了定义良好的双金属Au-Pt纳米颗粒。由于双金属Au-Pt物种和独特的Lewis酸性骨架Sn的协同作用,优化后的Au1Pt3@Snβ在甘油转化为乳酸甲酯方面表现出优异的催化性能,在413 K和0.5 MPa空气条件下,乳酸甲酯收率为78.8%,TOF为335 h-1,超过了以往报道的大多数在类似反应条件下的多相催化剂。沸石的约束环境不仅可以提供空间限制,还可以诱导被封装的Au-Pt纳米颗粒与骨架Sn之间的强相互作用,从而抑制催化过程中金属的烧结和浸出。实验和理论计算(DFT)结果阐明了双金属Au-Pt协同作用在激活O2和促进甘油脱氢的较低能势中的关键作用,从而提高了催化性能。
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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