Zeng Li, Yang Qinghong, Wang Jianxing, Wang Xin, Wang Pengjie, Wang Shengchun, Lv Shide, Muhammad Shabbir, Liu Yichang, Yi Hong, Lei Aiwen
Institute for Advanced Studies (IAS), College of Chemistry and Molecular Sciences, Wuhan University, Wuhan 430072, P. R. China.
National Research Center for Carbohydrate Synthesis, Jiangxi Normal University, Nanchang 330022, P. R. China.
Science. 2024 Jul 12;385(6705):216-223. doi: 10.1126/science.ado0875. Epub 2024 Jul 11.
Direct current (DC) electrosynthesis, which has undergone optimization over the past century, plays a pivotal role in a variety of industrial processes. Alternating current (AC) electrosynthesis, characterized by polarity reversal and periodic fluctuations, may be advantageous for multiple chemical reactions, but apparatus, principles, and application scenarios remain underdeveloped. In this work, we introduce a protocol for programmed AC (pAC) electrosynthesis that systematically adjusts currents, frequencies, and duty ratios. The application of representative pAC waveforms facilitates copper-catalyzed carbon-hydrogen bond cleavage in cross-coupling and difunctionalization reactions that exhibit suboptimal performance under DC and chemical oxidation conditions. Moreover, observing catalyst dynamic variation under diverse waveform applications provides mechanistic insight.
直流（DC）电合成在过去一个世纪中经过了优化，在各种工业过程中发挥着关键作用。交流（AC）电合成的特点是极性反转和周期性波动，可能对多种化学反应有利，但设备、原理和应用场景仍未充分发展。在这项工作中，我们介绍了一种用于编程交流（pAC）电合成的方案，该方案可系统地调节电流、频率和占空比。代表性pAC波形的应用促进了铜催化的交叉偶联和双官能化反应中的碳氢键裂解，这些反应在直流和化学氧化条件下表现欠佳。此外，观察不同波形应用下催化剂的动态变化提供了机理见解。
