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选择性地形成乙酸盐中间产物可在 0°C 下延长 15 天的稳定乙烯去除效果。

Selective formation of acetate intermediate prolongs robust ethylene removal at 0 °C for 15 days.

机构信息

Shanghai Environmental Protection Key Laboratory on Environmental Standard and Risk Management of Chemical Pollutants, State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai, 200237, PR China.

Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, PR China.

出版信息

Nat Commun. 2023 May 20;14(1):2885. doi: 10.1038/s41467-023-38686-0.

DOI:10.1038/s41467-023-38686-0
PMID:37210396
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10199933/
Abstract

Efficient ethylene (CH) removal below room temperatures, especially near 0  °C, is of great importance to suppress that the vegetables and fruits spoil during cold-chain transportation and storage. However, no catalysts have been developed to fulfill the longer-than-2-h CH removal at this low temperature effectively. Here we prepare gold-platinum (Au-Pt) nanoalloy catalysts that show robust CH (of 50 ppm) removal capacity at 0 °C for 15 days (360 h). We find, by virtue of operando Fourier transformed infrared spectroscopy and online temperature-programmed desorption equipped mass spectrometry, that the Au-Pt nanoalloys favor the formation of acetate from selective CH oxidation. And this on-site-formed acetate intermediate would partially cover the catalyst surface at 0 °C, thus exposing active sites to prolong the continuous and effective CH removal. We also demonstrate, by heat treatment, that the performance of the used catalysts will be fully recovered for at least two times.

摘要

高效去除室温以下(尤其是接近 0°C)的乙烯对于抑制蔬菜和水果在冷链运输和储存过程中的腐烂至关重要。然而,目前还没有开发出能够在如此低温下有效去除超过 2 小时的 CH 的催化剂。在这里,我们制备了金铂(Au-Pt)纳米合金催化剂,该催化剂在 0°C 下可稳定去除 50 ppm 的 CH 长达 15 天(360 h)。我们通过原位傅里叶变换红外光谱和在线程序升温脱附-质谱联用技术发现,Au-Pt 纳米合金有利于从选择性 CH 氧化生成乙酸盐。并且,在 0°C 时,这种原位形成的乙酸盐中间体部分覆盖催化剂表面,从而暴露活性位以延长连续和有效的 CH 去除。我们还通过热处理证明,至少可以两次完全恢复使用后的催化剂性能。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/de83f39fca05/41467_2023_38686_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/5bb479e8a386/41467_2023_38686_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/c41b10099e9c/41467_2023_38686_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/efac758484f4/41467_2023_38686_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/e7a77f5b257b/41467_2023_38686_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/de83f39fca05/41467_2023_38686_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/5bb479e8a386/41467_2023_38686_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/c41b10099e9c/41467_2023_38686_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/efac758484f4/41467_2023_38686_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/e7a77f5b257b/41467_2023_38686_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e834/10199933/de83f39fca05/41467_2023_38686_Fig5_HTML.jpg

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本文引用的文献

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Concerted Catalysis by Adjacent Palladium and Gold in Alloy Nanoparticles for the Versatile and Practical [2+2+2] Cycloaddition of Alkynes.合金纳米颗粒中相邻钯和金的协同催化作用实现炔烃通用且实用的[2+2+2]环加成反应
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在丝光沸石的纳米空间中从醇可逆地生成不稳定的仲碳正离子及其在环境温度下的长时间稳定保存。
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