Simultaneous synthesis of oxygen doped carbon electrodes at the anode and cathode via potential cycling for promoted H2O2 electrosynthesis†

IF 6.1 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR
Suhua Mao, Xin Li, Bingshuang Li, Jin Li and Xiaoxi Huang
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Abstract

Carbon materials functionalized with oxygenated groups are promising catalysts for the electrochemical production of hydrogen peroxide (H2O2) through the two-electron oxygen reduction reaction (ORR). Compared to chemical oxidation methods, the electrochemical activation of carbon materials to incorporate oxygenated groups offers several appealing advantages. However, the knowledge is limited as to how electrochemical treatment influences the resulting ORR performance. Herein, we describe the synthesis of carbon electrodes modified with oxygenated groups at both anodic and cathodic sides by using potential cycling in neutral Na2SO4 solution. XPS composition analysis and electrochemical FTIR confirm the successful introduction of oxygenated groups. The H2O2 production rate increases significantly after potential cycling. The oxidized carbon electrode can catalyze the ORR at an industrial current density to produce H2O2 with selectivity close to 100% in a flow cell. Density functional theory (DFT) calculations demonstrate that the binding energy of *OOH is promoted after the modification of oxygenated groups, such as quinone/carbonyl and hydroxyl groups. These findings highlight the advantages of the electrochemical method on carbon surface functionalization and provide some guidelines for catalyst design.

Abstract Image

利用电位循环法在阳极和阴极同时合成氧掺杂碳电极,促进H2O2电合成
氧基功能化碳材料是电化学制备过氧化氢(H2O2)双电子氧还原反应(ORR)的重要催化剂。与化学氧化法相比,电化学活化碳材料引入含氧基团表现出了诱人的特点。然而,关于电化学处理如何影响ORR性能的知识是有限的。在此,我们描述了在中性Na2SO4溶液中利用电位循环在阳极和阴极两侧都修饰了氧基的碳电极的合成。基于XPS和电化学FTIR的成分分析表明,氧基修饰成功。电位循环后H2O2的产率显著提高。氧化碳电极可以在工业电流密度下催化ORR,在流动池中产生选择性接近100%的H2O2。密度泛函理论(DFT)计算表明,氧基修饰后*OOH的结合能提高。这些发现突出了电化学方法在碳表面功能化方面的优势,并为催化剂的设计提供了一些指导。
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来源期刊
Inorganic Chemistry Frontiers
Inorganic Chemistry Frontiers CHEMISTRY, INORGANIC & NUCLEAR-
CiteScore
10.40
自引率
7.10%
发文量
587
审稿时长
1.2 months
期刊介绍: The international, high quality journal for interdisciplinary research between inorganic chemistry and related subjects
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