Novel Catalytic Transformations of Organoboron Species and the Development of Ultrastable Self-Assembled Monolayers on Metal Surfaces

这项研究是基于我们实验室的两个令人兴奋的发现。在2014年，我们证明了NHC在黄金上形成单层，可以承受前所未有的极端热量，氧化剂，酸和碱。这项工作被国际专家称为“改变游戏规则”，包括芬兰纳米科学中心主任Häkkinen。其他专家称之为“新的黄金标准”和“优雅”。已知NHC在过渡金属络合物中形成强键，但以前没有被检查为金属上自组装单层的硫醇的替代品。在本提案中，我们将探讨这一新颖而令人兴奋的发现的许多方面，包括：（1）NHC结构对膜质量和结合强度的影响，（2）使用NHC在包括Ag和Cu的其它金属上形成膜，其中NHC涂层可以帮助防止氧化和失泽，以及（3）在幻数Au簇中使用NHC，其是显著的分子材料，这些材料主要是用硫醇配体制备的，因此NHC将提供一种全新类型的纳米材料。在长期目标中，我们将（4）探索NHC在分子电子学中的应用以及作为催化活性表面和纳米颗粒的改性剂。该项目的许多合作已经到位，包括霍顿（表面科学，皇后），姆克林（STM成像，皇后物理），巴德利（STM成像，圣安德鲁斯），克拉茨（电化学，T疤痕U。），Häkkinen（理论，芬兰），Mosey（理论，女王）和Tsukuda（纳米团簇，日本）。

The proposed research is based on two exciting discoveries from our lab. In 2014, we demonstrated that NHCs form monolayers on gold that withstand unprecedented extremes of heat, oxidant, acid and base. This work was called "game changing" by international experts, including Häkkinen, director of the Nanoscience Centre in Finland. Other experts called it "the new gold standard" and "elegant". NHCs have been known to form strong bonds in transition metal complexes but had not previously been examined as alternatives to thiols for self-assembled monolayers on metals. In this proposal, we will explore many aspects of this novel and exciting discovery, including: (1) the effect of NHC structure on film quality and bond strength, (2) the use of NHCs to form films on other metals including Ag and Cu where the NHC coating may help prevent oxidation and tarnishing, and (3) the use of NHCs in magic number Au clusters, which are remarkable molecular materials, that have been largely prepared with thiol ligands and thus NHCs will provide a completely new type of nanomaterial. In long term goals, we will (4) explore the use of NHCs in molecular electronics and as modifiers for catalytically active surfaces and nanoparticles. Many collaborations for this project are already in place, including with Horton (surface science, Queen's), McLean (STM imaging, Queen's Physics), Baddeley (STM imaging, St. Andrews), Kraatz (Electrochemistry, U of T Scar.), Häkkinen (Theory, Finland), Mosey (Theory, Queen's) and Tsukuda (nanoclusters, Japan).