Zhang Haichuan, Li Yingjie, Zhao Yingshuang, Li Guanghe, Zhang Fang
National Engineering Laboratory for Site Remediation Technologies , Beijing 100015 , China.
Department of Materials Science and Engineering, College of Engineering , Peking University , Beijing 100871 , China.
ACS Appl Mater Interfaces. 2019 Aug 7;11(31):27846-27853. doi: 10.1021/acsami.9b07765. Epub 2019 Jul 23.
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.
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。