Electrolyzer Design for Flexible Decoupled Water Splitting and Organic Upgrading with Electron Reservoirs
Electrolyzer Design for Flexible Decoupled Water Splitting and Organic Upgrading with Electron Reservoirs
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DOI：
10.1016/j.chempr.2017.12.019
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发表时间：
2018-03-08
期刊：
影响因子：
23.5
通讯作者：
Sun, Yujie
中科院分区：
文献类型：
--
作者：
Li, Wei;Jiang, Nan;Sun, Yujie
传统的水分解电解在大电压输入下同时驱动H-2和O-2的演化反应（分别为HER和OER）。本文描述了两种廉价的铁配合物作为质子独立的电子储层（ERs）用于解耦的水电解。（二茂铁甲基）三甲基氯化铵和Na-4[Fe(CN)(6)]在水介质中具有适当的氧化还原电位，能够与HER偶联氧化。随后氧化ER+的还原与OER配对。这两个步骤所需的电压都比直接劈水所需的电压小得多。两种er均获得近100%的法拉第效率和显著的循环稳定性。这种解耦的水分解也可以由在阳光照射下具有小光伏的光伏电池驱动。此外，在碱性条件下，证明了Na-4[Fe(CN)(6)]介导HER的两步电解和5-羟甲基糠醛的氧化，生成H-2和2,5-呋喃二羧酸。本文提出了一种具有极大灵活性和安全性的解耦式水电解槽设计方案。
Conventional water-splitting electrolysis drives the H-2 and O-2 evolution reactions (HER and OER, respectively) simultaneously with large voltage inputs. Herein, two inexpensive iron complexes as proton-independent electron reservoirs (ERs) are described for decoupled water electrolysis. (Ferrocenylmethyl) trimethylammonium chloride and Na-4[Fe(CN)(6)], which have proper redox potentials in aqueous media, are able to couple their oxidation with HER. The subsequent reduction of the oxidized ER+ is then paired with OER. Both steps require much smaller voltage than that of direct water splitting. Nearly 100% Faradic efficiency and remarkable cycling stability were obtained for both ERs. Such decoupled water splitting could also be driven by photovoltaic cells with small photovoltages under sunlight irradiation. Furthermore, a two-step electrolysis of HER and the oxidation of 5-hydroxymethylfurfural mediated by Na-4[Fe(CN)(6)] was demonstrated under alkaline conditions, producing H-2 and 2,5-furandicarboxylic acid. This work presents a decoupled water electrolyzer design with great flexibility and safety advantages.