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      化學所在高載量單原子分散金屬-氮催化劑的普適性宏量制備研究方面取得新進展
      2019-05-13 | 編輯:lidan | 【 】【打印】【關閉

        近年來,單原子催化劑因其高的原子利用率、明確的催化活性中心和高的催化性能而成為研究前沿與熱點。但由于在制備過程中活性原子易于遷移和聚集,使得單原子催化劑的高載量可控制備仍存在巨大挑戰。如何實現高密度的單原子催化活性位點,以及如何實現其低成本宏量制備是單原子分散催化劑邁向應用的關鍵。金屬-氮類催化劑在燃料電池、鋅空電池、電解水等電化學能源器件中有著廣泛的應用,但其形成通常需要高溫,金屬原子更易團聚,因此制備高密度、單原子分散的金屬-(M-Nx)催化劑更具挑戰。 

        在國家自然科學基金委、科技部和中國科學院的支持下中科院化學所分子納米結構與納米技術院重點實驗室胡勁松課題組致力于高性能非貴金屬電催化劑的設計、可控構筑與催化機制研究。近期,他們在前期關于金屬-氮類氧還原電催化劑(J. Am. Chem. Soc. 2016, 138, 3570ACS Catal. 2015, 5, 2903ACS Appl. Mater. Interfaces 2015, 7, 115082017, 9, 5272Carbon 2016, 107, 162J. Mater. Chem. A 2016, 4, 7781Chem. Commun. 2018, 54, 8190Appl. Catal. B Environ. 2019, 251, 240)和單原子分散Fe-N-C電催化劑(Chem. Commun. 2018, 54, 1307)的研究基礎上,發展了一種簡便的級聯錨定新策略,實現了金屬載量可達12%的單原子分散金屬-氮催化劑的普適性宏量制備,催化劑表現出優異且穩定的電催化性能,相關工作發表于Nat. Commun. 2019, 10, 1278 

        為了獲得高載量的單原子分散金屬-氮位點,研究人員通過1) 使用絡合劑(如廉價葡萄糖等)與金屬離子形成絡合物在原子尺度上物理隔離金屬源;2) 采用高比表面積、表面富有含氧官能團的、兼顧高速傳質與傳荷特點的三維多孔碳載體實現了金屬絡合物在載體表面的高密度負載;3) 同時使用過量絡合劑在分子尺度上物理分隔金屬絡合物;4) 高溫熱解時含氮前體(如三聚氰胺等)原位分解生成的CNx片斷可在與絡合物分解的金屬原子形成M-Nx結構的同時,與裂解生成的碳在載體表面形成多孔碳網絡,從而原位錨定M-Nx并使其暴露成為有效催化位點。 

        實驗中,只需將葡萄糖溶液與多孔碳載體及金屬鹽前體混合,再與三聚氰胺一起熱處理即可獲得高密度、穩定的單原子分散的M-Nx催化劑。該策略對多種金屬、載體、絡合劑普遍適用;制備過程簡單,成本低,可規模化制備;催化劑性能優異。例如,Fe-Nx催化劑堿性氧還原半波電位可達0.90 V,在此電位下動力學質量活性可達100.7 A/g,明顯優于商業20 wt% Pt/C催化劑;Ni-Nx催化劑電催化還原CO2時在30 mA/cm2的電流密度下法拉弟效率也可達89%。這一逐級錨定新策略為宏量制備高密度、高活性、高穩定性的單原子分散M-Nx類催化劑提供了一種新的普適的方法 Nat. Commun. 2019, 10, 1278  

          

        級聯錨定策略宏量制備高載量單原子金屬-催化劑 

          

        分子納米結構與納米技術院重點實驗室 

          2019513     

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