催化作用
循环伏安法
电解
草酸盐
纳米颗粒
计时安培法
电催化剂
材料科学
化学工程
制氢
析氧
阳极
电解质
化学
无机化学
电化学
纳米技术
电极
有机化学
工程类
物理化学
作者
Dulce M. Morales,Daliborka Jambrec,Мariya A. Kazakova,Michael Braun,Nivedita Sikdar,Adarsh Koul,Ann Cathrin Brix,Sabine Seisel,Corina Andronescu,Wolfgang Schuhmann
标识
DOI:10.1021/acscatal.1c04150
摘要
Electrocatalytic oxidation of glycerol (GOR) as the anode reaction in water electrolysis facilitates the production of hydrogen at the cathode at a substantially lower cell voltage compared with the oxygen evolution reaction. It simultaneously provides the basis for the production of value-added compounds at the anode. We investigate earth-abundant transition-metal oxide nanoparticles (Fe, Ni, Mn, Co) embedded in multiwalled carbon nanotubes as GOR catalysts. Out of the four investigated composites, the Ni-based catalyst exhibits the highest catalytic activity toward the GOR according to rotating disk electrode voltammetry, reaching a current density of 10 mA cm–2 already at 1.31 V vs RHE, a potential below the formation of Ni3+. Chronoamperometry conducted in a flow-through cell followed by HPLC analysis is used to identify and quantify the GOR products over time, revealing that the applied potential, electrolyte concentration, and duration of the experiment impact strongly the composition of the products' mixture. Upon optimization, the GOR is directed toward oxalate production. Moreover, oxalate is not further converted and hence accumulates as a major organic product under the chosen conditions in a concentration ratio of 60:1 with acetate as a minor product after 48 h electrolysis in 7 M KOH, which represents a promising route for the synthesis of this highly valued product.
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