MIL-53(Fe)-based catalysts: CO2 hydrogenation performance and three-dimensional structures

IF 3.9 3区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Materials Science and Engineering B-advanced Functional Solid-state Materials Pub Date : 2024-10-25 DOI:10.1016/j.mseb.2024.117767

Tianhe Gao , Jingwei Yuan , Wanyin Xu , Ronghui Hao , Wenkang Miao , Zihan Wang , Yubing Dong , Wenxin Lin , Qianqian Li

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Abstract

Transition based metal–organic frameworks (MOFs) demonstrate significant potential for thermal catalysis owing to their high density of active metal sites, and tunable porous structure. Especially understanding the correlation between the three-dimensional (3D) structure and its catalytic performance is pivotal for designing highly efficient, stable, and selectively active thermal catalysts. Here, based on MIL-53(Fe) and its derivatives heat-treated at varying temperatures, we comprehensively investigated their 3D structures and properties using 3D reconstruction techniques in transmission electron microscopy. The specimen, pyrolysis at 800 °C in air, exhibits optimal performance used as the catalyst for CO₂ hydrogenation, achieving 21.4 % CO₂ conversion and 100 % CO selectivity. Additionally, it presents exceptionally high activity and thermal stability after reaction for 120 h. Detailed insights into the morphology, composition, pore, and surface crystallography of an individual MIL-53(Fe) and its pyrolysis product particle, respectively, are provided by 3D reconstruction at nanoscale to correlate these structural features with their catalytic performance. This research contributes valuable experimental data and theoretical insights for the structural modulation and performance enhancement of MOF-based catalysts.

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MIL-53(Fe)基催化剂：二氧化碳加氢性能和三维结构

过渡金属有机框架（MOFs）具有高密度的活性金属位点和可调的多孔结构，因此在热催化方面具有巨大的潜力。尤其是了解三维（3D）结构与其催化性能之间的相关性，对于设计高效、稳定和具有选择性活性的热催化剂至关重要。在此，我们以经过不同温度热处理的 MIL-53（Fe）及其衍生物为基础，利用透射电子显微镜中的三维重建技术全面研究了它们的三维结构和性能。在空气中于 800 °C 高温分解的试样表现出最佳性能，可用作二氧化碳加氢催化剂，实现 21.4% 的二氧化碳转化率和 100% 的二氧化碳选择性。通过纳米尺度的三维重建，详细了解了单个 MIL-53(Fe)及其热解产物颗粒的形态、组成、孔隙和表面晶体学，并将这些结构特征与其催化性能联系起来。这项研究为基于 MOF 的催化剂的结构调控和性能提升提供了宝贵的实验数据和理论见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Materials Science and Engineering B-advanced Functional Solid-state Materials 工程技术-材料科学：综合

CiteScore

5.60

自引率

2.80%

发文量

481

审稿时长

3.5 months

期刊介绍： The journal provides an international medium for the publication of theoretical and experimental studies and reviews related to the electronic, electrochemical, ionic, magnetic, optical, and biosensing properties of solid state materials in bulk, thin film and particulate forms. Papers dealing with synthesis, processing, characterization, structure, physical properties and computational aspects of nano-crystalline, crystalline, amorphous and glassy forms of ceramics, semiconductors, layered insertion compounds, low-dimensional compounds and systems, fast-ion conductors, polymers and dielectrics are viewed as suitable for publication. Articles focused on nano-structured aspects of these advanced solid-state materials will also be considered suitable.