南京大学丁梦宁/程旭/马晶JACS:通过氧化还原-去耦策略实现无金属参与的电化学脱硼氘代反应
Flow electrochemical synthesis is a promising platform for constructing value-added targets such as D-labeled compounds. However, its efficiency and broader application are limited by the unproductive or kinetically mismatched counter half-reactions and architectural constraints of conventional flow cell architectures. Here, we report a redox-decoupled strategy within a single-celltandem flow reactor that separates a classical substitutive deborylation−deuteration into sequential electrochemical steps. This approach enables the universal, metal-free deuteration of diverse organoboron species, including boronic acids, borate esters, and borates, across alkyl, (heterocyclic) aryl, alkenyl, andother derivatives (>100 examples). Using D2O as a cost-effective D-source, the system achieves excellent yields, D-incorporation, tolerance to the labile functional groups, and significantly improved Faradaic efficiency. The platform demonstrates industrial grade durability with continuous operation for over 1200 h and enables scalable, unprotected synthesis of deuterated drug D-mexiletine. Overall, this strategy significantly expands the design space of flow electrochemistry, paving an exciting path toward green, economic, and efficient electrosynthesis.图3. 氧化还原-去耦策略设计及单池串联流动反应器 (图片来源于JACS)图4. 磷酸修饰的锌电极表征及电催化性能 (图片来源于JACS)图6. 克级反应、长期稳定性及不同合成应用 (图片来源于JACS)图7. 机理研究及可能的反应途径 (图片来源于JACS)In summary, we have developed a redox-decoupled electrosynthesis strategy and a single-cell tandem flow cell that resolves the architectural and kinetic bottlenecks inherent in conventional redox-decoupled systems. By enabling sequential electrolyte progression through independently optimized electrode regions, assisted by the implementation of an AEM and a phosphoric acid-modified Zn (Zn-PA) cathode to improve the deuteration efficiency, we achieved the site-specific deuteration of over 100 diverse organoboron substrates. This methodology enables the first metal-free deuteration of nonactivated alkyl boronic acids at room temperature and was successfully applied to the scalable synthesis of the deuterated drug D-mexiletine with enhanced metabolic stability. With demonstrated industrial-grade dura bility over 1200 h of continuous operation, this platform offers a versatile engineering blueprint for optimizing complex tandem electrochemical processes, effectively bridging the gap between fundamental synthetic innovation and practical industrial application.DOI: https://doi.org/10.1021/jacs.6c09364声明：本文中广告内容由广告主提供，请您在购买任何商品或服务前，以书面合同形式明确约定双方权利义务，本账号不对其后续经营行为承担持续担保责任
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