Department of Materials Science and Engineering, Peking University, Beijing 100871, China.
Nanoscale. 2018 Jun 14;10(23):11064-11071. doi: 10.1039/c8nr01855c.
The good performance of Cu displayed in CO2 conversion promotes the study on how to disperse Cu into 2D materials for better catalysis. Inspired by the recent studies on new 2D porous B sheets [Angew. Chem., Int. Ed., 2017, 56, 10093; Adv. Mater., 2018, 30, 1704025; Phys. Rev. Lett., 2017, 118, 096401], here for the first time we have explored the catalytic properties of Cu atomic chains on β-borophene sheets, and have found that the Cu-B sheet can break the scaling relationship through providing secondary adsorption sites, thus leading to small overpotentials in the preferable reaction pathway CO2 → COOH* → CO* → CHO* → CH2O* → CH3O* → CH3OH. The Cu atomic chains also lower the energy barrier by forming assistant adsorptions of H*. Electronic structure analyses further show that the Cu atomic chain structure stabilizes the CHO* bonding through an enhanced σ bonding-π back-bonding mode. Our study not only sheds light on the design of new catalysts for effective CO2 conversion but also expands the applications of B sheets.
铜在二氧化碳转化中表现出的优异性能，推动了将其分散到二维材料中以实现更好催化效果的研究。受最近关于新型二维多孔 B 片的研究的启发[Angew. Chem., Int. Ed., 2017, 56, 10093; Adv. Mater., 2018, 30, 1704025; Phys. Rev. Lett., 2017, 118, 096401]，我们首次探索了铜原子链在β-硼烯片上的催化性能，发现 Cu-B 片可以通过提供次级吸附位点打破比例关系，从而导致在更优选的反应途径 CO2 → COOH* → CO* → CHO* → CH2O* → CH3O* → CH3OH 中出现较小的过电势。铜原子链还通过形成 H的辅助吸附作用降低了能垒。电子结构分析进一步表明，铜原子链结构通过增强的σ键-π反键模式稳定了 CHO键合。我们的研究不仅为有效二氧化碳转化的新型催化剂设计提供了思路，还扩展了 B 片的应用。
