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关于金原子与硼掺杂/硫掺杂碳表面上的硼发生前所未有的强相互作用的实验和理论证据。

Experimental and theoretical evidence for unprecedented strong interactions of gold atoms with boron on boron/sulfur-doped carbon surfaces.

作者信息

Banerjee Samya, Wolny Juliusz A, Danaie Mohsen, Barry Nicolas P E, Han Yisong, Amari Houari, Beanland Richard, Schünemann Volker, Sadler Peter J

机构信息

Department of Chemistry, University of Warwick CV4 7AL Coventry UK

Department of Chemistry, Indian Institute of Technology (BHU) Varanasi Uttar Pradesh 221005 India

出版信息

Nanoscale Adv. 2023 Dec 11;6(7):1837-1846. doi: 10.1039/d3na00956d. eCollection 2024 Mar 26.

DOI:10.1039/d3na00956d
PMID:38545290
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10964758/
Abstract

The 16e square-planar bis-thiolato-Au(iii) complexes [Au(1,2-dicarba--dodecarborane-1,2-dithiolato)][NBu] (Au-1) and [Au(4-methyl-1,2-benzenedithiolato)][NBu] (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.

摘要

已合成并全面表征了十六面体平面双硫醇基 - 金（III）配合物[Au(1,2 - 二碳 - 十二硼烷 - 1,2 - 二硫醇基)][NBu]（Au - 1）和[Au(4 - 甲基 - 1,2 - 苯二硫醇基)][NBu]（Au - 2）。Au - 1和Au - 2被封装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泊洛沙姆（普朗尼克®）P123中，形成胶束AuMs - 1和AuMs - 2。在扫描透射电子显微镜（STEM）中利用高电子通量分别在B/S掺杂的石墨表面或S掺杂的非晶碳表面上由AuMs - 1和AuMs - 2生成单个金原子和金纳米晶体。电子能量损失谱（EELS）数据表明金原子/纳米晶体与B/S掺杂石墨基体中的硼有强烈相互作用。密度泛函理论（DFT）计算也支持了实验结果，表明存在强Au - B键，这取决于Au - （B - 石墨烯）片段上的电荷以及石墨烯晶格中进一步缺陷的存在情况。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/18bbeb055046/d3na00956d-f9.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/7b9fe9d45e08/d3na00956d-s1.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/889fa8e05041/d3na00956d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/2f34fad138af/d3na00956d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/e503a3efb35e/d3na00956d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/90f2d3fe86a6/d3na00956d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/081cb0b7652f/d3na00956d-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/d81899a63bdd/d3na00956d-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/64efe363cabf/d3na00956d-f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/18bbeb055046/d3na00956d-f9.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/7b9fe9d45e08/d3na00956d-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/dac1a6e53489/d3na00956d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/889fa8e05041/d3na00956d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/2f34fad138af/d3na00956d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/e503a3efb35e/d3na00956d-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/90f2d3fe86a6/d3na00956d-f5.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/081cb0b7652f/d3na00956d-f6.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/d81899a63bdd/d3na00956d-f7.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/64efe363cabf/d3na00956d-f8.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/ccae/10964758/18bbeb055046/d3na00956d-f9.jpg

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