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                                                                              分子模拟与太阳能转化研究团队在金属咔咯死死基多孔有机聚合物促进氧气电地步催化研究中取得重要进展

                                                                              发布者:曹凯超  发布时间:2022-04-15 17:01:49  浏览:

                                                                              将〇分子催化剂集成到框架结构中,不仅能够将分子的催化特冷哼一聲性保留在框架材料内,还可以进一步怎么回事通过调控分子结构来▃设计框架材料。近年来,多孔框架材料由于自身▲具有较大的比表面积,容易暴露活性位点,方便结合底物以及♀可以加快传质效率等,被广泛地应用于ξ 催化领域。更重這么多人要的是,其周期性『网络结构会使具有分子性质的活性位点均匀分布到整个框架结构中。因此,分子基框架材料通常表现出比∮分子催化剂自︼身更高的活性和稳定性。

                                                                              金属卟啉经常被用于构建框架结构催化剂,但是基于金属咔咯的框架结构〓催化剂比较少见。作为卟啉←的类似物,咔咯配体可以与金属离子形成◣四配位的平面M-N4结构,其三价阴金光閃爍离子大环可以更好地稳定高价态金╱属离子。高价态金属是氧气还原反這道刀芒帶著一種令人心顫应(ORR)和氧〒气析出反应(OER)的关→键中间体。因此,金属咔咯分子催化剂通常在电催化ORR和OER过程卐中表现出优异的性能。然而,与卟啉黑風寨收服相比,meso-位缺少一个碳原子的咔咯配↙体对称性较低,这使得不由朝第九殿主點了點頭设计和合成基于金属咔咯的框架结构更具挑∏战性。因此,很少有金属咔咯好大框架结构被合成并用于▲电催化ORR和/或OER。

                                                                              近日,分子模拟与太阳◤能转化研究团队曹睿教授通外面才過一年过Sonogashira偶联↓反应合成了金属咔咯基多孔有机聚合物,并成功将其用于电白色長袍催化ORR和OER。发现,将钴咔咯分子自身优异的氧电催∞化性能与框架材料的结构优势相结合,能实现同时高效催化ORR和OER。


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                                                                              该研究工作主要成☉果如下:

                                                                              第一,使用10-苯基-5,10-(4-碘苯基)咔人手剛從我無月星離開咯配合物与四(4-炔基苯基)甲烷进行偶联◇反生成M-POPs(M=Mn,Fe,Co,Cu)。通过BET测试证明了M-POPs的多孔特性;通过红〖外光谱和13C NMR固体核磁等证明了多孔有看著陽正天頓時苦笑机聚合物的成功合成∩;进一步通过X-射线光电子能谱和X-射线元素映射等证明金属咔咯☆分子完整并均匀的分布在整哈哈一笑个多孔有机聚合物中。特别是,M-POPs中I 3d特征峰的消失,进一步证明了偶联反应的完成。

                                                                              第二,碱性条件(0.1 M KOH)下分别进行电催化ORR和OER测试。首先,在相同条件下与其他金属咔咯基多孔聚合物相比必須在它出現,钴咔咯※基多孔聚合物在所有催化剂中表现出最高的催化活性。这主要是由于钴咔咯分子自身的电催化性【能优于其他金属咔咯分子;其次,与相同钴含量的分子靈魂攻擊催化剂单体相比,钴咔咯基多孔聚合物在电催」化过程中具有更高的活性和稳那首領如果會來定性。电化学以及动力学研究表明,钴咔咯基多孔聚合物具有▆更高的活性表但這時候面积和传质效率;金属咔ω咯单体和M-POPs的电子结那不是遠古神器构(价□ 带和导带)在聚土行孫臉色不變合反应前后没有发生太大变化。这就说明钴咔咯基多孔聚合物表现◆出优于单体分子催化性能的主要原因是具有更高的活性表∴面积和传质过程。

                                                                              第三,基于钴咔咯基多孔聚合物¤优异的电催化ORR和OER性能,进一步将其应用王恒和董海濤連忙擺手搖頭于锌-空气电池组『装测试,表现出媲美贵金属体系的催化活性。

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                                                                              这项工作首∑ 次将金属咔咯框架结构应用于电催化氧气还原和氧气析出反应。这种将分子催化特性与框水之力噴涌而出架结构优势相结合的策略有望将来合成更▼多的分子基框架材料,应用于其他的能量转换技〖术中。

                                                                              该成哈哈一笑果发表在←《德国应用好處化学》期刊(Angew. Chem. Int. Ed., 2022, DOI: 10.1002/anie.202201104),论文第一作者为陕西】师范大学副研究员雷海涛和硕士研究生张清鑫,通讯作者ぷ为陕西师范大学曹睿教授。(论文链接:


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