Acetylene hydrochlorination catalyzed by N/O-doped spiral mesoporous carbonaceous nanospheres

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials Pub Date : 2025-03-04 DOI:10.1016/j.micromeso.2025.113577

Zehong Zhu , Qingxin Wu , Xueying Wang , Haiyang Zhang , Jian Li , Yanzhao Dong , Yongsheng Xu , Yunsheng Dai , Jinli Zhang

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Abstract

Here, the spiral mesoporous hydrothermal carbonaceous nanospheres (SMHNs) were designed and fabricated from pentose precursors to enhance gas diffusion in acetylene hydrochlorination. Through the optimization of hydrothermal conditions, the optimized SMCNs-800 material showcased the highest catalytic activity with an acetylene conversion of 77 % under the condition of GHSV (C₂H₂) = 30 h⁻¹. The structural analysis indicated that the material with helical structure could provide larger pore sizes and abundant defect sites, exposing more active sites. The structure-activity relationship among acid-base properties of the catalyst surface, the adsorption-desorption capacity for the reactants and the catalytic activity jointly demonstrated that pyridine-N and -C=O could provide abundant basic sites for the adsorption and activation of H-Cl, thus accelerating the process of acetylene hydrochlorination reaction.

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N/ o掺杂螺旋介孔碳纳米球催化乙炔加氢氯化反应

本文以戊糖为原料，设计并制备了螺旋介孔水热碳质纳米球（SMHNs），以增强乙炔加氢氯化过程中的气体扩散。通过水热条件优化，优化后的SMCNs-800材料在GHSV (C2H2) = 30 h−1的条件下表现出最高的催化活性，乙炔转化率为77%。结构分析表明，螺旋结构的材料可以提供更大的孔径和丰富的缺陷位点，暴露出更多的活性位点。催化剂表面的酸碱性质、对反应物的吸附-解吸能力和催化活性之间的构效关系共同表明，吡啶- n和-C=O可以为H-Cl的吸附和活化提供丰富的碱性位点，从而加速了乙炔加氢氯化反应的过程。

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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.