张宁
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祝贺课题组在《Nature Communications》上发表有关流动相电解反应器设计用于提升C-N偶联合成肟类化合物效率的研究论文!第一作者为博士生李嘉威!
Title: Managing electrolyte flow boosts the efficiency of continuous oxime electrosynthesis to over 95%
Abstract: Electrified chemosynthesis shows great promise for sustainable chemical manufacturing. However, the reaction efficiency of continuous flow electrochemistry is currently unsatisfactory due to restricted mass transport at the two-phase boundary. Here, we present an effective flow management strategy involving electrolyzer structural optimization to intensify the localized electrochemical process. We demonstrate this approach using the electrosynthesis of cyclohexanone oxime from cyclohexanone and nitrite as a representative example. The cathodic counterpart is regulated by a unique flow-through channel architecture that drives the significant electrolyte convection throughout the porous electrode matrix and minimizes the hydrodynamic diffusion distance, giving the catalyst full accessibility to the feedstock. Using an optimal cobalt single-atom catalyst, we demonstrate the oxime electrosynthesis with a Faradaic efficiency of over 95%, regardless of the operating conditions. Furthermore, we achieve a high single-pass conversion efficiency of up to 95% by balancing the supply of feedstocks between the cyclohexanone feeding and the in situ generated hydroxylamine through subtle control of the electrolyte flow rate. This continuous-flow electrosynthesis process demonstrates long-term stability, operating for up to 110 hours without any loss of activity, which highlights its great potential for practical implementation.
