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    北理工前沿交叉院王博教授在Angew. Chem. Int. Ed.期刊發表重要研究成果

    供稿: 前沿交叉學院、新能源前線 編輯: 朱倩云
    (2018-11-29) 閱讀次數:
    【字號  大

      近日,在北京理工大學王博教授、陳世稆教授和馬小杰助理教授團隊(共同通訊作者)帶領下,提出了一種含鐵金屬有機框架MIL-100(Fe),用于去除臭氧。相關成果以題為“An Iron-Containing Metal–Organic Framework as a Highly Efficient Catalyst for Ozone Decomposition”發表在國際頂級期刊Angew. Chem. Int. Ed.上。

      MIL-100(Fe)在室溫下相對濕度為45%,空間速度為1.9×105 h-1時,在100小時內具有100%的持久臭氧轉化效率,遠遠超出大多數的性能,顯示出優異且穩定的催化效率。該MOF優于許多吸附劑和催化劑,如活性炭和α-MnO2(12小時后分別降至臭氧分解的18%和60%)。更重要的是,團隊發現水在MOF催化臭氧分解中起協同作用,即使在極端潮濕的條件下(例如> 90%RH)也能實現完全去除臭氧。為了進一步的實際應用,團隊還用熱壓(HoP)法對MIL-100(Fe)進行了加工,制造了一種基于MOF的催化過濾器;作為口罩上的過濾器,它顯示了對低濃度臭氧幾乎完全的保護。本研究證明了MOF在臭氧污染控制方面的巨大潛力,也為臭氧分解催化劑的設計提供了新的見解。

      地面臭氧是世界上主要的空氣污染物之一,由于其高反應性和強氧化能力,直接導致光化學煙霧。長期暴露于臭氧會導致嚴重的肺損傷,并增加因呼吸道疾病而早死的風險。臭氧去除的主要方法有活性炭吸附、化學吸附和催化分解。吸附劑再生和廢液處理的不可避免的問題意味著多相催化是目前最有效的方法。迄今為止,通過使用貴金屬和過渡金屬氧化物作為催化劑分解消除臭氧。在這些報道的催化劑中,MnO2具有較好的分解活性和較低的成本。然而,由于吸附在表面的氧物質的積累,其活性急劇下降。更重要的是,由于水在反應性位點上的競爭性吸附,MnO2在水蒸氣存在的情況下顯示出降低的活性。盡管為了在高濕度環境下獲得良好的活性,貴金屬催化劑一直是人們關注的焦點,但由于其高成本和稀缺性,貴金屬的大規模應用受到了限制。因此,開發具有優異活性和在潮濕環境下性能穩定的非貴金屬催化劑是非常有必要的。

    圖1 MIL-100(Fe)作為臭氧分解的催化劑

    圖2 MIL-100(Fe)物理性能表征及對臭氧轉化率

    (a)MIL-100(Fe)的臭氧轉化率。b)模擬的、合成的和暴露于臭氧的MIL-100(Fe)的粉末XRD圖案。c)在暴露于臭氧之前和之后,MIL-100(Fe)的N2吸附等溫線。插圖:MIL-100(Fe)的孔徑分布。d)分別對MIL-100(Fe)、α-MnO2、活性炭、α-Fe2O3和β-MnO2進行臭氧轉化。條件:用0.27g石英砂稀釋的0.03g催化劑, C( O3)= 45ppm,流速="1000mL" min-1,RH="45%,室溫。)

    圖3 MIL-100(Fe)在不同高濕度環境下對臭氧的轉化率

    (a)分別在<5%RH、20%RH、30%RH、40%RH和> 90%RH下MIL-100(Fe)的臭氧轉化率。b)在交替相對濕度下MIL-100(Fe)上的臭氧轉化率。c)優化了在MIL‐100(Fe)催化臭氧分解過程中沿路徑穩定點的結構和相應的勢能曲線。藍色和紅線分別表示六重態和四重態MIL-100(Fe)氫氧化物復合物的能級。實驗條件:用0.27g石英砂稀釋0.03g催化劑, C( O3)= 45ppm,流速="1000mL" min-1,RH="45%,室溫。)

    圖4 MOFilter的制作及其應用測試

    (a,b)MOFilter的照片和包含MOFilter的口罩。c)MOFilter的SEM圖像。d)(c)中方框的放大圖像。e)模擬MIL-100(Fe),無紡布和MOFilter的XRD圖案。f)MOFilter上的臭氧去除,入口臭氧濃度為200ppb,室溫下RH為45%。)

      團隊探索使用了MOF進行催化臭氧分解的可能性和詳細機理。研究了在潮濕環境中的催化活性,發現使用MIL-100(Fe)的臭氧去除效率可以達到100%并且在45%RH的高流速下持續超過100小時。通過與多孔吸附劑(活性炭)和過渡金屬氧化物催化劑(α-MnO2)的比較,進一步驗證了MIL-100(Fe)的優異活性),用臭氧快速停用,在12小時內分別降至18%和60%。研究發現,當使用MOF作為活性催化劑時,水的存在有利于消除臭氧,并且在相對濕度為40%至大于90%的范圍內實現臭氧的完全分解。此外,MOFilter已經被制作并用作口罩中的過濾層,以防止低水平的臭氧。這些研究結果強調了MOF對污染控制的重要性,并可能為開發臭氧分解的其他催化劑開辟新的可能性。

      文獻鏈接:An Iron-Containing Metal–Organic Framework as a Highly Efficient Catalyst for Ozone Decomposition(Angew. Chem. Int. Ed., 2018, DOI: 10.1002/anie.201810268)

      

    【個人簡介】

      王博,2004年畢業于北京大學化學學院,獲學士學位;2006年畢業于美國密歇根大學,獲理學碩士學位;2008年畢業于美國加州大學洛杉磯分校化學系,獲理學博士學位。

      2008-2011年任職于德國巴斯夫公司,任研究員、項目負責人;2011年底入職北京理工大學化學學院。現任北京理工大學學部委員、特聘教授、爆炸科學與技術國家重點實驗室防護技術方向學術帶頭人。2015年獲中國化學會青年化學獎,2016年獲國家杰出青年科學基金資助,2017年入選科技部中青年科技創新領軍人才。

      近五年來,已作為通訊作者在JACS(7篇)、Angew.(4篇)、Adv. Mater.(4篇)、Chem. Soc. Rev. (2篇)、EES (2篇)、Chem. Sci.(2篇)等國際學術期刊上發表50余篇論文,其中SCI影響因子10.0以上超過20篇。全部已發表論文SCI他引超過7000次,單篇最高他引1800次,共計有超過12篇文章入選ESI高被引論文。已經獲批美國發明專利3項,中國發明專利2項。研究成果受到國內外學者的廣泛認可和關注,被國際專業期刊多次正面評述報道。開拓的MOF薄膜防護與檢測研究及其成膜理論已經被國內外多個著名MOF研究課題組追蹤報道和借鑒,并應用到了多個重要科學研究和應用領域。


    (審核:王博)

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