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论文类型：期刊论文

发表时间：2014-07-01

发表刊物：APPLIED CATALYSIS B-ENVIRONMENTAL

收录刊物：SCIE、EI

卷号：154

页面范围：360-368

ISSN号：0926-3373

关键字：Selective oxidation; Glycerol; Gold nanoparticles; Fuel cell; Cogeneration

摘要：Sustainable cogeneration of tartronate (high yield of 61.8%) and electrical energy (1527 J, 12 h) has been achieved from direct electrocatalytic oxidation of glycerol on Au/C in a 5 cm(2) anion exchange membranedirect glycerol fuel cells (AEM-DGFCs). The electrode structure and reaction conditions exhibited strong effects on the anode potential, which can be tuned to <0.45 V in favor of oxidizing two primary OH groups of glycerol while minimizing over-oxidation of the secondary OH and C C bond cleavage, thereby promoting the tartronate production. The relatively low activity of partial oxidation products (glycerate, tartronate, mesoxalate) on Au/C revealed in half cell indicates that the tartronate generation in AEMDGFCs is through direct adsorbed C-3 intermediates oxidation. Mass transport of reactants and reaction intermediates governed by the operational conditions was also found to play a critical role in regulating reaction rate and the desired products selectivity. Furthermore, Au/C prepared via aqueous phase reduction method (Au/C-AQ) was compared with organic phase nanocapsule method (Au/C-NC), and it shows the residual surfactants have little effect on the tartronate yield. (C) 2014 Elsevier B.V. All rights reserved.