Step-Edge Assisted Direct Linear Alkane Coupling
Step-Edge Assisted Direct Linear Alkane Coupling
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阶梯边缘辅助直接线性烷烃耦合
DOI：
10.1002/chem.201605744
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发表时间：
2017
期刊：
影响因子：
--
通讯作者：
Chi Lifeng
中科院分区：
文献类型：
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作者：
Zhang Junjie;Chang Chun-ran;Yang Biao;Cao Nan;Peng Chencheng;Zhang Haiming;Tang Dan-Tam D.;Glorius Frank;Erker Gerhard;Fuchs Harald;Li Qing;Chi Lifeng
通过末端甲基的C-H活化直接偶联烷烃在科学和技术上都获得了巨大的兴趣。在这里，我们提出了在调制温度下的Cu表面的台阶边缘的直链烷烃耦合的结果。结合扫描隧道显微镜（STM）的观察与密度泛函理论加上色散（DFT-D）计算，我们阐明了反应的机制，并证明了低活化势垒依赖于在上台阶边缘的非均相催化，其中存在低配位的表面原子。我们进一步揭示了反应的通用性，使它可以应用于不同的表面刻面的台阶边缘。
Direct coupling of alkanes via C−H activation of terminal methyl groups has acquired tremendous interests both scientifically and technically. Herein we present the results of linear alkane‐coupling at the step edges of Cu surfaces at modulated temperatures. Combining the observations of scanning tunneling microscopy (STM) with density functional theory plus dispersion (DFT‐D) calculations, we elucidate the mechanism of the reaction and demonstrate that the low activation barrier relies on heterogeneous catalysis at the upper step edges, where low‐coordinated surface atoms are present. We further reveal the generality of the reaction, so that it can be applied on the step edges of different facets of surfaces.