Renewable Zn/S-1 catalyst with dual active sites for acetylene acetoxylation

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials Pub Date : 2024-09-11 DOI:10.1016/j.micromeso.2024.113333

Ying Zhang , Qinqin Wang , Mingyuan Zhu , Bin Dai

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Abstract

The prevailing Zn/AC catalysts was plagued by limited lifetime and difficulties in regeneration for acetylene acetoxylation. In order to exploring renewable catalyst for acetylene acetoxylation, Zn/S-1 catalyst was synthesized using Silicalite-1(S-1) as support. The catalytic performance of Zn/S-1 was compared with Zn/AC catalyst using active carbon as support. The CH₃COOH conversion of Zn/S-1 catalyst only decreased 15 % after running 225 h, much better than the 66 % of Zn/AC after 154 h. TG analysis revealed that the improved stability of Zn/S-1 catalyst was attributed to its better resistance for carbon deposition with the presence of S-1 support. A series of characterizations and DFT results elucidated that the Lewis acid sites of S-1 support and Zn component serve as dual active sites, which enhanced the adsorption of CH₃COOH and inhibited the carbon deposition. In addition, the deactivated Zn/S-1 catalyst could be regenerated by calcination in air atmosphere due to the thermal stability of S-1, and the regenerated Zn/S-1 catalyst showed similar catalytic activity with the fresh catalyst.

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用于乙炔乙酰氧基化的具有双活性位点的可再生 Zn/S-1 催化剂

现有的 Zn/AC 催化剂在乙炔乙氧基化过程中存在使用寿命有限和再生困难的问题。为了探索乙炔乙氧基化的可再生催化剂，研究人员以硅灰石-1（S-1）为载体合成了 Zn/S-1 催化剂。将 Zn/S-1 催化剂的催化性能与以活性炭为载体的 Zn/AC 催化剂进行了比较。TG 分析表明，Zn/S-1 催化剂稳定性的提高归因于其在 S-1 支持下具有更好的抗碳沉积能力。一系列表征和 DFT 结果表明，S-1 载体的路易斯酸位点和 Zn 成分是双重活性位点，可增强对 CH3COOH 的吸附并抑制碳沉积。此外，由于 S-1 具有热稳定性，失活的 Zn/S-1 催化剂可在空气中煅烧再生，再生后的 Zn/S-1 催化剂具有与新鲜催化剂相似的催化活性。

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来源期刊

Microporous and Mesoporous Materials 化学-材料科学：综合

CiteScore

10.70

自引率

5.80%

发文量

649

审稿时长

26 days

期刊介绍： Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.