Programmed alternating current optimization of Cu-catalyzed C-H bond transformations

• 成果类型: Article
• 署名作者: Zeng, Li; Yang, Qinghong; Wang, Jianxing; Wang, Xin; Wang, Pengjie; Wang, Shengchun; Lv, Shide; Muhammad, Shabbir; Liu, Yichang; Yi, Hong; Lei, Aiwen
• 署名单位: Wuhan University; Jiangxi Normal University
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-11816
• DOI: 10.1126/science.ado0875
• 发表日期: 2024-07-12
• 页码: 216-223
• 关键词: electrosynthesis; EVOLUTION; oxygen

摘要

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.