Linear paired electrochemical valorization of glycerol enabled by the electro-Fenton process using a stable NiSe2 cathode
Linear paired electrochemical valorization of glycerol enabled by the electro-Fenton process using a stable NiSe2 cathode
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DOI：
10.1038/s41929-022-00826-y
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发表时间：
2022-08
期刊：
影响因子：
37.8
通讯作者：
Hongyuan Sheng;Aurora N. Janes;R. Ross;H. Hofstetter;Kwan-Young Lee;J. Schmidt;S. Jin
中科院分区：
文献类型：
--
作者：
Hongyuan Sheng;Aurora N. Janes;R. Ross;H. Hofstetter;Kwan-Young Lee;J. Schmidt;S. Jin
剩余的生物质衍生的原料（如甘油）的电化学增值为高价值化学品提供了生物质资源利用和化学制造脱碳的可持续途径;然而，甘油通常仅通过阳极氧化增值，在阴极产生较低价值的产物（如氢气）。在这里，我们建立了有效的阴极valorization甘油的理想的C3氧化产物，通过电芬顿过程在一个稳定的NiSe 2阴极，建立在理论上的理解和实验证明的高选择性和稳定性的NiSe 2对酸性H2 O2电合成。一个概念验证的线性配对电化学过程，同时在NiSe 2阴极和Pt阳极的甘油成相同的氧化产物的增值实现了高选择性的附加值C3产品和高甘油转化率，需要很少的外部能量输入，当电芬顿生成的羟基自由基是仔细控制。这种线性配对的概念策略可推广用于实现不同生物质衍生原料的原子效率电精炼。
Electrochemical valorization of surplus biomass-derived feedstocks, such as glycerol, into high-value chemicals offers a sustainable route for utilization of biomass resources and decarbonization of chemical manufacturing; however, glycerol is typically valorized solely via anodic oxidation, with lower-value products such as hydrogen gas generated at the cathode. Here, we establish the efficient cathodic valorization of glycerol to the desirable C3oxidation products via the electro-Fenton process at a stable NiSe2cathode, built upon the theoretical understanding and experimental demonstration of the high selectivity and stability of NiSe2toward acidic H2O2electrosynthesis. A proof-of-concept linear paired electrochemical process for concurrent valorization of glycerol into the same oxidation products at both NiSe2cathode and Pt anode achieves high selectivity for value-added C3products and high glycerol conversion with little external energy input needed, when the electro-Fenton generation of hydroxyl radicals is carefully controlled. This conceptual strategy of linear pairing is generalizable for enabling atom-efficient electro-refinery of diverse biomass-derived feedstocks.