Subsurface-Carbon-Induced Local Charge of Copper for an On-Surface Displacement Reaction,Angewandte Chemie International Edition

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Subsurface-Carbon-Induced Local Charge of Copper for an On-Surface Displacement Reaction
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2021-08-26 , DOI: 10.1002/anie.202108712
Shaoshan Wang _{1,

2} , Pengcheng Ding _{1,

3} , Zhuo Li _{1,

2} , Cristina Mattioli ₄ , Wenlong E ₂ , Ye Sun ₃ , André Gourdon ₄ , Lev N Kantorovich ₅ , Flemming Besenbacher ₆ , Xueming Yang ₂ , Miao Yu _{1,

2}

Affiliation

Transition-metal carbides have sparked unprecedented enthusiasm as high-performance catalysts in recent years. Still, the catalytic properties of copper carbide remain unexplored. By introducing subsurface carbon to Cu(111), a displacement reaction of a proton in a carboxyl acid group with a single Cu atom is demonstrated at the atomic scale and room temperature. Its occurrence is attributed to the C-doping-induced local charge of surface Cu atoms (up to +0.30 e/atom), which accelerates the rate of on-surface deprotonation via reduction of the corresponding energy barrier, thus enabling the instant displacement of a proton with a Cu atom when the molecules adsorb on the surface. This well-defined and robust Cu^δ+ surface based on subsurface-carbon doping offers a novel catalytic platform for on-surface synthesis.

中文翻译：

用于表面置换反应的亚表面碳诱导铜局部电荷

近年来，过渡金属碳化物作为高性能催化剂引发了前所未有的热情。尽管如此，碳化铜的催化性能仍有待探索。通过将表面下的碳引入 Cu(111)，在原子尺度和室温下证明了羧酸基团中的质子与单个 Cu 原子的置换反应。它的发生归因于 C 掺杂引起的表面 Cu 原子的局部电荷（高达 +0.30 e/atom），通过减少相应的能垒来加速表面去质子化的速度，从而使当分子吸附在表面上时，质子带有一个铜原子。这种定义明确且稳健的 Cu ^δ+ 基于亚表面碳掺杂的表面为表面合成提供了一个新的催化平台。

更新日期：2021-10-12

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