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    您現在所在的位置:首頁» 新聞網» 科研學術» 正文

    北理工在可溶性有機多孔聚合物用于兩相催化方面取得研究進展

    供稿: 材料學院 付浩熹 編輯: 邵澤
    (2019-07-04) 閱讀次數:
    【字號  大

      有機多孔聚合物(POPs)是一種新興的多孔材料,具有廣泛的應用前景。北京理工大學材料學院的黃木華課題組長期以來關注功能性有機多孔聚合物的實用制備及應用技術。該小組先后實現了Cu粉催化的Ullmann偶聯反應制備硝基功能化的有機多孔材料NO2-PAF-1(Polym. Chem., 2016, 7, 770),利用NaBH4介導的還原偶聯反應,快速制備了偶氮鍵鏈接的有機多孔聚合物材料Azo-POP-1、Azo-POP-2和Azo-POP-3(J. Mater. Chem. A, 2018, 6, 5608)。該工作報道了第一例可溶性的Azo-POPs,并創新性地將可溶性的Azo-POPs用于有機/水兩相催化反應,取得了良好的催化效果和催化劑的循環使用性,為可持續發展提供了技術支持。該工作發表在《Journal of Materials Chemistry A》 (A Soluble Porous Organic Polymer for Highly Efficient Organic-Aqueous Biphasic Catalysis and Convenient Reuse of Catalysts, 2019. 7 (25): p. 15048-15053. DOI: 10.1039/C9TA04594E)(SCI頂級期刊,影響因子10.73)上。碩士研究生付浩熹為該論文的第一作者,黃木華特別研究員為通訊作者。該工作得到了國家自然科學基金(No. 21772013)、北京市自然科學基金(No. 2162039)以及中央高校基本科研業務費專項基金的大力資助。同時,該工作也得到了材料學院先進材料實驗中心的大力支持。

    圖1 Azo-POP-7的快速制備

      然而,目前報道的大部分有機多孔聚合物不熔融不溶解,一定程度上限制了其進一步應用。因此,從分子鏈的扭曲構象出發,以“逆合成”的思路選擇合適的聚合物單體和高效的聚合反應,制備新型的可溶性有機多孔聚合物材料,對推進有機多孔聚合物材料領域的研究具有重要意義,也成為一個研究熱點。最近,黃木華課題組利用重氮偶聯反應,從具有扭曲構象的9,9-二(4-羥基苯基)芴和9,9-二(4-胺基苯基)芴單體出發,實現了偶氮鍵鏈接的可溶性有機多孔聚合物材料Azo-POP-7的快速制備(圖1)。

      與文獻報道過的Azo-POPs相比,Azo-POP-7具有優異的溶解性,可溶于強極性的有機溶劑,如DMF、THF、DMSO、CHCl3、二氧六環和3-戊酮中。這是由于Azo-POP-7的分子鏈具有扭曲構象,能夠防止分子鏈間的緊密堆積,從而提高聚合物在有機溶劑中的溶解性。經過優化條件,Azo-POP-7的BET比表面積可以達到364 m2·g-1,平均孔徑為19.38 nm,孔容為1.76 cm3·g-1。Azo-POP-7的結構得到了溶液核磁氫譜,固體核磁碳譜,紫外-可見光譜,紅外,元素分析等多種分析手段的聯合驗證。通過凝膠滲透色譜(GPC)和核磁共振-二維擴散排序譜(2D 1H DOSY-NMR)得到了Azo-POP-7的分子量信息。

      廢水中對硝基苯酚的去除和轉化與人類的健康信息相關,是可持續發展研究的重要內容,也是檢驗催化劑性能的經典反應。通過“異相反應均相化”的策略,該工作利用可溶性的有機多孔聚合物Azo-POP-7負載貴金屬Pd,得到了分布均一,尺寸極小的納米Pd顆粒(< 2nm)。同時,負載金屬Pd后的Pd@Azo-POP-7仍能保持優異的溶解性,并用于有機/水兩相中催化對硝基苯酚的還原。

    圖2 Pd@AZO-POP-7的HR-TEM圖像和Pd納米顆粒的尺寸分布

    圖3 Pd@Azo-POP-7用于催化4-硝基苯酚的氫化還原

      利用有機/水兩相法催化還原4-硝基苯酚,具有反應高效,催化劑回收簡單,可重復使用等特點。利用紫外-可見光吸收光譜對催化反應進行跟蹤和動力學研究,發現Pd@Azo-POP-7作為催化劑,反應的速率常數高達4.95×10?2 s?1,是目前報道的最高值。

    圖4 Pd@Azo-POP-7的循環催化性能

      此外,Pd@Azo-POP-7具有優異的循環催化性能。在相同的反應條件下,以醋酸Pd作為反應的催化劑,只能進行3次循環催化。而以Pd@Azo-POP-7作為催化劑時,催化反應可以進行12次以上,仍然保持很高的催化活性(圖4)。這主要歸功于Azo-POP-7的羥基偶氮官能團與金屬Pd間存在配位作用,很好地分散了Pd納米粒子,防止聚集,并防止其流失。該工作為制備可溶性有機多孔聚合物材料提供了新的思路,拓展了有機多孔聚合物在兩相催化中的應用。

      原文鏈接:https://pubs.rsc.org/en/content/articlelanding/2019/TA/C9TA04594E#!divAbstract

     

    附黃木華特別研究員簡介:

      2001年獲北京師范大學化學系理學學士學位(化學教育專業),2006年獲中科院化學所理學博士學位(有機化學專業)。2006-2011年,先后在瑞士蘇黎世聯邦理工學院(ETH-Zürich)和英國利物浦大學(University of Liverpool)化學系進行博士后研究。2012年3月加入北京理工大學材料學院,開展有機高分子功能材料、含能材料和核磁共振波譜技術等方面的教學與科研工作。2017年1月起,受聘為北京理工大學特別研究員和博士生導師。為研究生講授《新型含能材料》課程,為本科生開設《Designing Organic Synthesis》和《核磁共振波譜技術實踐》課程。作為項目負責人承擔國家自然科學基金面上項目、國家自然科學基金青年項目、北京市自然科學基金面上項目、北京理工大學火炸藥全鏈條科技創新項目、北京理工大學優秀青年教師資助計劃以及橫向合作課題等。具體研究方向包括:(1)有機多孔聚合物材料;(2) 含能材料;(3)核磁共振波譜技術在材料科學研究中的應用。已在Nature Chemistry, Journal of Materials Chemistry A,Green Chemistry,Polymer Chemistry和Organic Letters等雜志上發表研究論文29篇,申請中國發明專利18項。同時,參與北京理工大學材料學院分析測試中心的籌建工作,具體負責核磁分中心的日常管理工作。


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