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在均相钌催化剂存在下,由碳酸氢钠水溶液产生的甲酸根离子的生成与定量分析。

Generation and Quantification of Formate Ion Produced from Aqueous Sodium Bicarbonate in the Presence of Homogeneous Ruthenium Catalyst.

作者信息

Treigerman Ziv, Sasson Yoel

机构信息

Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 9190401, Israel.

出版信息

ACS Omega. 2018 Oct 8;3(10):12797-12801. doi: 10.1021/acsomega.8b00599. eCollection 2018 Oct 31.

DOI:10.1021/acsomega.8b00599
PMID:31458005
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6644996/
Abstract

Formic acid and its salts are an alternative source for hydrogen generation. In this study, we store hydrogen using the formate-bicarbonate cycle. Aqueous sodium bicarbonate is hydrogenated to form sodium formate, which can then be decomposed to release hydrogen and sodium bicarbonate. The hydrogenation step is carried out under mild conditions in the presence of a homogeneous ruthenium catalyst. Hydrogen charge is realized at 70 °C under a hydrogen pressure of 20 bar, achieving yields > 80% and turnover number > 610. The catalyst is stable and robust through numerous cycles of the hydrogenation reaction. The formate ion formed during the bicarbonate hydrogenation is assayed and quantified by ion chromatography.

摘要

甲酸及其盐类是制氢的替代来源。在本研究中,我们利用甲酸盐 - 碳酸氢盐循环来储存氢气。碳酸氢钠水溶液被氢化形成甲酸钠,然后甲酸钠可以分解以释放氢气和碳酸氢钠。氢化步骤在温和条件下,在均相钌催化剂存在下进行。在70℃、20巴氢气压力下实现氢气充注,产率> 80%,周转数> 610。通过多次氢化反应循环,催化剂保持稳定且性能良好。在碳酸氢盐氢化过程中形成的甲酸根离子通过离子色谱法进行测定和定量。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c2/6644996/8aada83ef238/ao-2018-00599z_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c2/6644996/7f48fb524fbf/ao-2018-00599z_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c2/6644996/e6fa8a900025/ao-2018-00599z_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c2/6644996/944bebd909a1/ao-2018-00599z_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c2/6644996/8aada83ef238/ao-2018-00599z_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c2/6644996/7f48fb524fbf/ao-2018-00599z_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c2/6644996/e6fa8a900025/ao-2018-00599z_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c2/6644996/944bebd909a1/ao-2018-00599z_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e8c2/6644996/8aada83ef238/ao-2018-00599z_0003.jpg

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本文引用的文献

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钯修饰的功能化石墨相氮化碳:一种使用KHCO作为温和且无腐蚀性氢源的氢化反应高效非均相催化剂。
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Direct synthesis of formic acid from carbon dioxide by hydrogenation in acidic media.在酸性介质中通过二氧化碳加氢直接合成甲酸。
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Structure-reactivity relationships in the hydrogenation of carbon dioxide with ruthenium complexes bearing pyridinylazolato ligands.含吡啶基并唑基配体的钌配合物催化二氧化碳加氢的结构-反应性关系。
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