Experimental and theoretical evidence for unprecedented strong interactions of gold atoms with boron on boron/sulfur-doped carbon surfaces
Experimental and theoretical evidence for unprecedented strong interactions of gold atoms with boron on boron/sulfur-doped carbon surfaces
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DOI：
10.1039/d3na00956d
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发表时间：
2023-12
影响因子：
4.7
通讯作者：
Samya Banerjee;J. Wolny;Mohsen Danaie;Nicolas P. E. Barry;Yisong Han;Houari Amari;Richard Beanland;Volker Schünemann;Peter J Sadler
中科院分区：
文献类型：
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作者：
Samya Banerjee;J. Wolny;Mohsen Danaie;Nicolas P. E. Barry;Yisong Han;Houari Amari;Richard Beanland;Volker Schünemann;Peter J Sadler
合成了16E正方形平面双硫代金(Ⅲ)配合物[AuIII(1，2-dicarba-closo-dodecarborane-1，2-dithiolato)2][NBu4](Au-1)和[AuIII(4-methyl-1，2-benzenedithiolato)2][NBu4](Au-2)，并对其进行了表征。将Au-1和Au-2包裹在含有聚环氧乙烷和聚环氧丙烷嵌段的对称三嵌段共聚物Poloxamer(Pluronic®)P123中，得到胶束AUMS-1和AUMS-2。利用高电子通量扫描电子显微镜分别在掺B/S的石墨表面和S掺杂的非晶碳表面制备了Au原子和Au纳米晶。电子能量损失谱(EELS)数据表明，在B/S掺杂的石墨体中，金原子/纳米晶与硼发生了强烈的相互作用。密度泛函理论(DFT)的计算也支持实验结果，指出了强烈的Au-B键，这取决于Au-(B-石墨烯)碎片上的电荷和石墨烯晶格中进一步缺陷的存在。
The 16e square-planar bis-thiolato-Au(iii) complexes [AuIII(1,2-dicarba-closo-dodecarborane-1,2-dithiolato)2][NBu4] (Au-1) and [AuIII(4-methyl-1,2-benzenedithiolato)2][NBu4] (Au-2) have been synthesized and fully characterized. Au-1 and Au-2 were encapsulated in the symmetrical triblock copolymer poloxamer (Pluronic®) P123 containing blocks of poly(ethylene oxide) and poly(propylene oxide), giving micelles AuMs-1 and AuMs-2. High electron flux in scanning transmission electron microscopy (STEM) was used to generate single gold atoms and gold nanocrystals on B/S-doped graphitic surfaces, or S-doped amorphous carbon surfaces from AuMs-1 and AuMs-2, respectively. Electron energy loss spectroscopy (EELS) data suggested strong interactions of gold atoms/nanocrystals with boron in the B/S-doped graphitic matrix. Density-functional theory (DFT) calculations, also supported the experimental findings, pointing towards strong Au–B bonds, depending on the charge on the Au–(B-graphene) fragment and the presence of further defects in the graphene lattice.