Guo Hong-Yang, Wan Qiang, Jiang Yunjia, Wang Bo, Wang Lingyao, Zheng Ju-Fang, Wang Ya-Hao, Zhang Yuanbin, Li Jian-Feng, Zhou Xiao-Shun
Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, College of Chemistry and Materials Science, Zhejiang Normal University, 321004, Jinhua, P. R. China.
State Key Laboratory of Physical Chemistry of Solid Surfaces, iChEM, College of Chemistry and Chemical Engineering, College of Energy, College of Material, Xiamen University, 361005, Xiamen, P. R. China.
Angew Chem Int Ed Engl. 2025 Jan 10;64(2):e202414867. doi: 10.1002/anie.202414867. Epub 2024 Nov 11.
The recent discovery of frustrated Lewis pairs (FLPs) during the activation of small molecules has inspired extensive research across the full span of chemical science. Owing to the nature of weak interactions, it is experimentally challenging to directly observe and modulate FLP at the molecular scale. Here we design a boron cluster anion building block (BH ) and organic amine cations ([NR], R=-CH, -CH) as the FLP to prove the feasibility of controlling their interaction in the electric double layer (EDL) via an electrochemical strategy. In situ single-molecule electrical measurements and Raman monitoring of BH -[NR] FLP formed at the positively charged Au(111) electrode surface, in contrast to the free-standing BH near or below the potential of zero charge (PZC). Furthermore, this FLP chemistry leads to a shift in the local density of states of boron clusters towards the E for enhancing electron transport, providing a new prototype of a reversible single-cluster switch that digitally switches upon controlling FLP chemistry in the electric double layer.
