用于高效可见光光催化CO还原的氢键有机框架超薄纳米片
Hydrogen-Bonded Organic Framework Ultrathin Nanosheets for Efficient Visible-Light Photocatalytic CO Reduction.
作者信息
Yu Baoqiu, Meng Ting, Ding Xu, Liu Xiaolin, Wang Hailong, Chen Baotong, Zheng Tianyu, Li Wen, Zeng Qingdao, Jiang Jianzhuang
机构信息
Beijing Advanced Innovation Center for Materials Genome Engineering, Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline Materials, Department of Chemistry and Chemical Engineering, School of Chemistry and Biological Engineering, University of Science and Technology Beijing, Beijing, 100083, China.
CAS Key laboratory of standardization and Measurement for Nanotechnology, CAS Center for Excellence in nanoscience, National Center for Nanoscience and Technology (NCNST), Beijing, 100190, China.
出版信息
Angew Chem Int Ed Engl. 2022 Oct 24;61(43):e202211482. doi: 10.1002/anie.202211482. Epub 2022 Sep 23.
Post-modification of robust guanine-quadruplex-linked 2,2'-pyridine-containing HOF-25 with Ni(ClO ) ⋅ 6 H O followed by exfoliation using sonication method affords hydrogen-bonded organic framework (HOF) nanosheets (NSs) of HOF-25-Ni in the yield of 56 %. TEM and AFM technologies disclose the ultrathin nature of HOF-25-Ni NSs with thickness of 4.4 nm. STM observation determines the presence of sql segments assembled from HOF-25-Ni building blocks at the heptanoic acid/highly oriented pyrolytic graphite interface, supporting the simulated 2D supramolecular framework. ICP-MS, XAS, and XPS data prove the successful immobilization of atomic nickel sites on the 20 % total 2,2'-pyridine moieties in crystalline HOF-25-Ni. With the aid of [Ru(bpy) ] and triisopropanolamine, 10 wt% HOF-25-Ni NSs dispersed on graphene oxide efficiently promotes visible-light-driven CO reduction, showing a 96.3 % CO selectivity with a prominent conversion rate up to 24 323 μmol g h .
用六水合高氯酸镍对坚固的鸟嘌呤-四链体连接的含2,2'-吡啶的HOF-25进行后修饰，然后采用超声处理方法进行剥离，得到产率为56%的HOF-25-Ni氢键有机框架（HOF）纳米片（NSs）。透射电子显微镜（TEM）和原子力显微镜（AFM）技术揭示了HOF-25-Ni NSs的超薄性质，其厚度为4.4纳米。扫描隧道显微镜（STM）观察确定了在庚酸/高度定向热解石墨界面处存在由HOF-25-Ni结构单元组装而成的sql片段，支持了模拟的二维超分子框架。电感耦合等离子体质谱（ICP-MS）、X射线吸收光谱（XAS）和X射线光电子能谱（XPS）数据证明了原子镍位点成功固定在结晶HOF-25-Ni中20%的总2,2'-吡啶部分上。借助[Ru(bpy)₃]和三异丙醇胺，分散在氧化石墨烯上的10 wt% HOF-25-Ni NSs有效促进了可见光驱动的CO₂还原，显示出96.3%的CO₂选择性，突出的转化率高达24323 μmol g⁻¹ h⁻¹。
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