Sulfonic-Pendent Vinylene-Linked Covalent Organic Frameworks Enabling Benchmark Potential in Advanced Energy.
Sulfonic-Pendent Vinylene-Linked Covalent Organic Frameworks Enabling Benchmark Potential in Advanced Energy.
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DOI：
10.1002/advs.202300408
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发表时间：
2023-05
期刊：
影响因子：
15.1
通讯作者：
Luo, Feng
中科院分区：
文献类型：
--
作者：
Xu, Ying;Yu, Zhiwu;Zhang, Qingyun;Luo, Feng
关键词：
质子交换膜燃料电池和铀基核技术是两种绿色、先进的能源。然而，两者仍然面临一些棘手的科学和工业问题。对于前者，现有的质子传导材料总是存在这样或那样的缺陷，如质子电导率低、活化能高、耐久性差或产品规模小；而对于后者，在乏燃料后处理过程中，由于吸附部位失活或吸附剂在如此严苛的条件下发生分解，仍然缺乏可用的吸附剂来选择性地从浓硝酸（bbb1.0 M）中回收UO2 2+。研究发现，上述两个问题可以通过构建磺酸系乙烯链共价有机框架（COFs）来很好地解决，因为这些COFs含有丰富的磺酸单元，通过强配位固定和乙烯链来实现质子传导和UO2 2+捕获，从而提高了在12 M硝酸（12 M HNO3中存活的最佳材料之一）下的稳定性。大规模合成甲基磺酸衍生的乙烯链共价有机框架是首次通过使用HSO3活化方法实现的。所得到的共价有机框架不仅具有超高的化学稳定性，而且在质子交换膜燃料电池和铀基核能中都具有基准潜力。
Both proton exchange membrane fuel cells and uranium‐based nuclear techniques represent two green and advanced energies. However, both of them still face some intractable scientific and industrial problems. For the former, established proton‐conduction materials always suffer one or another defect such as low proton conductivity, high activation energy, bad durability, or just small‐scale product; while for the later, there still lacks available adsorbent to selectively recover of UO2 2+ from concentrated nitric acid (>1 M) during the spent fuel reprocessing due to the deactivation of the adsorption site or the decomposition of adsorbent under such rigorous conditions. It is found that the above two issues can be well solved by the construction of sulfonic‐pendent vinylene‐linked covalent organic frameworks (COFs), since these COFs contain abundant sulfonic units for both intrinsic proton conduction and UO2 2+ capture through strong coordination fixation and vinylene linkage that enhances the stability up to 12 M nitric acid (one of the best materials surviving in 12 M HNO3). Large‐scale synthesis of methylsulfonic‐derived vinylene‐linked covalent organic frameworks is for the first time achieved through using an HSO3‐activated approach. The resultant covalent organic frameworks afford not only ultrahigh chemical stability, but also benchmark potential in both proton exchange membrane fuel cells and uranium‐based nuclear energy.
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