Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 142, Issue 39, Pages 16579-16586Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.0c04311
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Funding
- National Natural Science Foundation of China [21421004, 21925201, 91845110, 21672059]
- Shanghai Municipal Science and Technology Major Project [2018SHZDZX03]
- Programme of Introducing Talents of Discipline to Universities [B16017]
- Program of the Shanghai Committee of Sci. Tech. [18520760700]
- Program for Eastern Scholar Distinguished Professor
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One of the most appealing topics in the study of metal-organic networks is the growth mechanism. However, its study is still considered a significant challenge. Herein, using scanning tunneling microscopy, the growth mechanisms of metal-alkynyl networks on Ag(111) and Au(111) surfaces were investigated at the atomic scale. During the reaction of 1,3,5-tris(chloroethynyl)benzene on Ag(111), honeycomb Ag-alkynyl networks formed at 393 K, and only short chain intermediates were observed. By contrast, the same precursor formed honeycomb Au-alkynyl networks on Au(111) at 503 K. Progression annealing led to a stepwise evolution process, in which the sequential activation of three Cl-alkynyl bonds led to the formation of dimers, zigzag chains, and novel chiral networks as the intermediates. Moreover, density functional theory calculations indicate that chlorine atoms are crucial in assisting the breakage of metal-alkynyl bonds to form Cl-metal-alkynyl, which guarantees the reversibility of the break/formation equilibration as the key to forming regular large-scale organometallic networks.
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