Yu Cihang, Leitch Jamie A, Gierlichs Lukas, Das Sampurna, Porch Adrian, Melen Rebecca L, Browne Duncan L
Department of Pharmaceutical and Biological Chemistry, University College London, School of Pharmacy, 29-39 Brunswick Square, Bloomsbury, London W1CN 1AX, U.K.
Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Translational Research Hub, Maindy Road, Cathays, Cardiff, Cymru/Wales CF24 4HQ, U.K.
J Am Chem Soc. 2024 Jul 24;146(29):19809-19817. doi: 10.1021/jacs.4c02736. Epub 2024 Jul 16.
Frustrated Lewis pairs (FLPs) offer an important and promising paradigm for main group catalysis. Reported here is the use of microwave dielectric spectroscopy for the detection of FLP encounter complexes. This technique focuses on the room-temperature measurement of the loss component of microwave permittivity (ε) over the bandwidth from 0.5 to 6.8 GHz. The microwave loss measured for a Lewis pair in a toluene host solution is compared with the losses of the individual components when measured separately, and the difference in loss Δε is used to characterize the electrostatic interaction between the pair. The Δε value shows a direct correlation with an ability for the FLP encounter complex to split hydrogen gas and abstract hydrogen from γ-terpinene and has led to the identification of a novel FLP encounter complex, tris-pentafluorophenyl borane-eucalyptol pairing.
受阻路易斯酸碱对（FLPs）为主族催化提供了一个重要且有前景的范例。本文报道了利用微波介电谱检测FLP遭遇络合物。该技术着重于在0.5至6.8 GHz带宽范围内对室温下微波介电常数（ε）的损耗分量进行测量。将甲苯主体溶液中路易斯酸碱对的微波损耗与各单独组分分别测量时的损耗进行比较，损耗差值Δε用于表征该酸碱对之间的静电相互作用。Δε值与FLP遭遇络合物分解氢气以及从γ-萜品烯中提取氢的能力直接相关，并已鉴定出一种新型的FLP遭遇络合物，即三（五氟苯基）硼烷-桉叶油醇配对物。
