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通过空气煅烧氧化的炭黑用于增强羟基自由基生成及有效降解有机物

Carbon Black Oxidized by Air Calcination for Enhanced HO Generation and Effective Organics Degradation.

作者信息

Zhang Haichuan, Li Yingjie, Zhao Yingshuang, Li Guanghe, Zhang Fang

机构信息

National Engineering Laboratory for Site Remediation Technologies , Beijing 100015 , China.

Department of Materials Science and Engineering, College of Engineering , Peking University , Beijing 100871 , China.

出版信息

ACS Appl Mater Interfaces. 2019 Aug 7;11(31):27846-27853. doi: 10.1021/acsami.9b07765. Epub 2019 Jul 23.

Abstract

Carbon black (CB) has a high conductivity and a large surface area, which are the basis of an excellent electrocatalyst. However, CB itself is usually less active or even inactive toward two-electron oxygen reduction reaction (2e ORR) due to the absence of highly active functional groups with low oxygen content. To activate commercial CB for 2e ORR, oxygen-containing functional groups were introduced onto the CB surface by a simple air calcination method. After the oxidation treatment at 600 °C (CB600), the oxygen content increased from the initial 1.17 ± 0.15 to 4.08 ± 0.60%, leading to a dramatic increase of the cathodic current from only -8.1 mA (CB) to -117.6 mA (CB600). The air cathode made of CB600 achieved the maximum HO production of 517.7 ± 2.4 mg L within 30 min, resulting in the removal of ∼91.1% rhodamine B in 2 min and an effective mineralization of ∼76.3% in an electro-Fenton reactor. This performance was much better than that obtained using the CB catalyst (65.3 ± 5.6 mg L HO production, and ∼20.3% mineralization). This excellent activity of CB600 toward 2e ORR was greatly improved by the introduction of O═C-OH and C-O-C groups. The successful improvement of the 2e ORR activity of CB using air calcination enables its practical application in electrochemical advanced oxidation processes.

摘要

炭黑(CB)具有高导电性和大表面积,这是其成为优异电催化剂的基础。然而,由于缺乏低氧含量的高活性官能团,CB本身对两电子氧还原反应(2e ORR)通常活性较低甚至无活性。为了使商用CB对2e ORR具有活性,通过简单的空气煅烧方法在CB表面引入含氧官能团。在600℃氧化处理后(CB600),氧含量从初始的1.17±0.15增加到4.08±0.60%,导致阴极电流从仅-8.1 mA(CB)急剧增加到-117.6 mA(CB600)。由CB600制成的空气阴极在30分钟内实现了517.7±2.4 mg L的最大H₂O₂产量,在2分钟内去除了约91.1%的罗丹明B,在电芬顿反应器中有效矿化率约为76.3%。该性能远优于使用CB催化剂获得的性能(H₂O₂产量为65.3±5.6 mg L,矿化率约为20.3%)。O═C-OH和C-O-C基团的引入极大地提高了CB600对2e ORR的优异活性。通过空气煅烧成功提高了CB的2e ORR活性,使其能够在电化学高级氧化过程中实际应用。

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