Electrocatalytic hydrogen peroxide formation on mesoporous non-metal nitrogen-doped carbon catalyst
Electrocatalytic hydrogen peroxide formation on mesoporous non-metal nitrogen-doped carbon catalyst
复制标题
DOI：
10.1016/j.jechem.2016.01.024
复制
发表时间：
2016-03-01
影响因子：
13.1
通讯作者：
Fellinger, Tim-Patrick
中科院分区：
文献类型：
--
作者：
Hasche, Frederic;Oezaslan, Mehtap;Fellinger, Tim-Patrick
在廉价的无金属富土催化剂上，由纯O-2和H-2直接电化学生成过氧化氢（H2O2）已成为原子效率最高、环境友好的反应途径，因此从学术和工业角度来看都引起了极大的兴趣。近年来，新型无金属介孔氮掺杂碳催化剂因其独特的电化学过氧化氢反应活性和选择性而受到广泛关注[1-3]。在这项工作中，我们更深入地了解了新型无金属介孔氮掺杂碳催化剂对过氧化氢形成的电催化活性、选择性和耐久性，特别强调了实验反应参数（如pH值和三种不同电解质的电极电位）的影响。我们使用两种独立的方法来研究电化学过氧化氢的形成，即旋转环盘电极（RRDE）技术和光度法紫外-可见技术。我们的电化学和光度测定结果清楚地表明，在环境温度和压力下，在相同电极电位下的酸性和中性介质中，无金属氮掺杂碳催化剂材料具有相当大的过氧化物形成活性和高的催化剂耐久性。此外，得到的电化学反应性和选择性表明，过氧化氢的电化学形成和分解机制强烈依赖于pH值和电极电位。(C) 2016科学出版社，大连化学物理研究所。版权所有。
Direct electrochemical formation of hydrogen peroxide (H2O2) from pure O-2 and H-2 on cheap metal-free earth abundant catalysts has emerged as the highest atom-efficient and environmentally friendly reaction pathway and is therefore of great interest from an academic and industrial point of view. Very recently, novel metal-free mesoporous nitrogen-doped carbon catalysts have attracted large attention due to the unique reactivity and selectivity for the electrochemical hydrogen peroxide formation [1-3]. In this work, we provide deeper insights into the electrocatalytic activity, selectivity and durability of novel metal-free mesoporous nitrogen-doped carbon catalyst for the peroxide formation with a particular emphasis on the influence of experimental reaction parameters such as pH value and electrode potential for three different electrolytes. We used two independent approaches for the investigation of electrochemical hydrogen peroxide formation, namely rotating ring-disk electrode (RRDE) technique and photometric UV-VIS technique. Our electrochemical and photometric results clearly revealed a considerable peroxide formation activity as well as high catalyst durability for the metal-free nitrogen-doped carbon catalyst material in both acidic as well as neutral medium at the same electrode potential under ambient temperature and pressure. In addition, the obtained electrochemical reactivity and selectivity indicate that the mechanisms for the electrochemical formation and decomposition of peroxide are strongly dependent on the pH value and electrode potential. (C) 2016 Science Press and Dalian Institute of Chemical Physics. All rights reserved.