生物质底物在无膜固体电解质反应器中的连续双加氢。

IF 16.9
Yanjie Zhai, Weisong Li, Xin Gao, Shanhe Gong, Qing Xia, Jie Wu, Shuting Wei, Yingying Zhou, Xiao Zhang
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引用次数: 0

摘要

通过电催化加氢从生物质中生产化学品,在可持续材料、医药、食品等领域的各种应用中显示出巨大的潜力,可以减少对环境的影响。特别是双电催化加氢,利用阳极和阴极的同步反应,以最大的电子效率(~ 200%)和产率脱颖而出。然而,在较高的电压下,阳极氢原子(H*)倾向于还原为质子。这种趋势导致了诸如低转化率和选择性以及难以维持连续生产等挑战。本文分别以肼和水作为氢源进行正极和负极反应,实现了马来酸高效双加氢制琥珀酸。这种方法每个转移的电子产生两个H*原子,促进阴极和阳极有效的碳-碳(C-C)键形成。我们进一步开发了一种模块化的无膜固体电解质反应器,用于使用商用钴催化剂连续双加氢马来酸。通过利用肼氧化和水还原,反应器在100 mA下持续200小时,法拉第效率约为180%。我们的方法在绿色化学的实际应用中显示出巨大的潜力,特别是在有效的生物质转化方面。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Continuous Dual Hydrogenation of Biomass Substrates in a Membrane-Free Solid Electrolyte Reactor.

Production of chemicals from biomass through electrocatalytic hydrogenation shows great potential to reduce environmental impact across various applications in sustainable materials, medicine, food, and more. Particularly, dual electrocatalytic hydrogenation, leveraging concurrent reactions at both anode and cathode stand out with maximized electron efficiency (∼200%) and production yield. However, at higher voltages, anodic hydrogen atoms (H*) tend to revert to protons. This tendency results in challenges such as low conversion rates and selectivity, and difficulties in maintaining continuous production. Herein, by employing hydrazine and water as the hydrogen sources for anode and cathode reactions, respectively, we achieved efficient dual hydrogenation of maleic acid to succinic acid. This approach produces two H* atoms per electron transferred, promoting effective carbon-carbon (C-C) bond formation at both cathode and anode. We further developed a modular, membrane-free solid electrolyte reactor for continuous dual hydrogenation of maleic acid using a commercial cobalt catalyst. By leveraging the hydrazine oxidation and water reduction, the reactor consistently produces succinic acid with a Faraday efficiency of approximately 180% for over 200 h at 100 mA. Our approach shows significant potential for practical applications in green chemistry, particularly in efficient biomass conversion.

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