Copper nanoparticles embedded flexible graphene aerogel for effective capture of iodine vapor

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED
Shengquan Liu , Xinli Gao , Peng Li , Xiaohua Zhang , Meihua Wang , Songtao Xiao , Xudong Zhao
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Abstract

Development of highly efficient and low-cost adsorbents for radioactive iodine vapor is significant but still challenged now. In this work, we reported a novel graphene aerogel (GA-Cu-ED) decorated by zero-valence copper and nitrogen active sites, prepared via a two-step route of hydrothermal reaction and freeze-drying processes. The combination of X-ray photoelectron spectroscopy (XPS) valence imaging and high-resolution transmission electron microscope (TEM) confirms the formation of Cu0 and its uniform distribution. Besides, the good elasticity and ultra-low density of this aerogel were proved. Adsorption experiments indicate that GA-Cu-ED has a high adsorption capacity of 3.76 g/g for gaseous iodine and short adsorption equilibrium time of 90 min. Even after three cycles, this aerogel still shows an almost unchanged adsorption capacity of 3.74 g/g. Meanwhile, this aerogel can be long-term stored under air atmosphere with only slight loss in adsorption performance. In addition, the captured iodine molecules can be tightly bound in this aerogel even after being exposed in air for three days. Mechanism analysis indicates the I-benzene conjugation, I–N charge transfer, and I2–Cu0 chemisorption contribute together to the capture of gaseous iodine. Therefore, our work provides a highly efficient and reliable adsorbent for radioactive iodine vapor, which may be worthy in large-scale application in future.

Abstract Image

嵌入柔性石墨烯气凝胶的纳米铜粒子可有效捕获碘蒸气
开发高效、低成本的放射性碘蒸气吸附剂意义重大,但目前仍面临挑战。在这项工作中,我们报道了一种由零价铜和氮活性位点装饰的新型石墨烯气凝胶(GA-Cu-ED),通过水热反应和冷冻干燥工艺两步制备而成。结合 X 射线光电子能谱(XPS)价谱成像和高分辨率透射电子显微镜(TEM),证实了 Cu0 的形成及其均匀分布。此外,该气凝胶的良好弹性和超低密度也得到了证实。吸附实验表明,GA-Cu-ED 对气态碘的吸附容量高达 3.76 g/g,吸附平衡时间短至 90 分钟。即使经过三次循环,这种气凝胶的吸附容量仍保持在 3.74 克/克,几乎没有变化。同时,这种气凝胶可以在空气中长期保存,吸附性能只有轻微的下降。此外,即使在空气中暴露三天,被捕获的碘分子也能紧密结合在气凝胶中。机理分析表明,I-苯共轭、I-N 电荷转移和 I2-Cu0 化学吸附共同促成了气态碘的捕获。因此,我们的工作提供了一种高效、可靠的放射性碘蒸气吸附剂,值得在未来大规模应用。
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来源期刊
Microporous and Mesoporous Materials
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.
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