Adsorption behavior of low-concentration nitrous oxide on natural mordenite zeolite

IF 4.7 3区材料科学 Q1 CHEMISTRY, APPLIED Microporous and Mesoporous Materials Pub Date : 2025-04-15 Epub Date: 2025-02-17 DOI:10.1016/j.micromeso.2025.113550

Saeko Yamaguchi , Peidong Hu , Hanlong Ya , Peipei Xiao , Ayako Nakata , Tsuyoshi Miyazaki , Yoshitada Morikawa , Junko N. Kondo , Kotaro Tange , Kenichi Tonokura , Masanori Takemoto , Yasuo Yonezawa , Toshiyuki Yokoi , Kenta Iyoki , Tatsuya Okubo , Toru Wakihara

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Abstract

Nitrous oxide (N₂O), the third most important greenhouse gas, is discharged from various anthropogenic sources and causes severe environmental problems. Herein, the natural mordenite zeolite is demonstrated to be an effective adsorbent to capture low-concentration N₂O (below 30 ppm). An adsorption capacity of 0.076 mmol g⁻¹ can be achieved at −7 °C with 1 ppm N₂O in the dynamic adsorption test, 6.3 times as high as that at 25 °C. The density functional theory calculations reveal that the Ca-exchanged MOR-type zeolite has stronger interactions with N₂O compared with the Na-exchanged one. However, as evidenced by the isosteric adsorption enthalpy analysis and the Fourier transform infrared spectroscopy, the natural mordenite zeolite with both Na⁺ and Ca²⁺, as well as the synthesized analogue, demonstrates stronger and distinctive interactions with trace N₂O in comparison to the MOR-type zeolites with single kind of extra-framework cation. These results provide experimental and theoretical foundations for the establishment of efficient N₂O removal system using well designed zeolite-based adsorbents under proper operating conditions.

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天然丝光沸石对低浓度氧化亚氮的吸附行为

一氧化二氮（N2O）是第三大温室气体，由各种人为来源排放，造成严重的环境问题。在这里，天然丝光沸石被证明是一种有效的吸附剂，可以捕获低浓度的N2O（低于30 ppm）。动态吸附试验中，在- 7℃、1 ppm N2O条件下，吸附量可达0.076 mmol g−1，是25℃条件下的6.3倍。密度泛函理论计算表明，钙交换型莫尔型沸石与N2O的相互作用较na交换型沸石强。然而，等等吸附焓分析和傅里叶变换红外光谱表明，天然丝光沸石与Na+和Ca2+以及合成的类似物相比，具有更强的和独特的与微量N2O的相互作用，与单一种框架外阳离子的莫尔型沸石相比。这些结果为在合适的操作条件下，利用精心设计的沸石基吸附剂建立高效的N2O去除体系提供了实验和理论基础。

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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.