College of Environmental Science and Engineering, Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria, Remediation and Pollution Control for Urban Ecological Environmental, Nankai University, Tianjin, 300350 China; State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, Heilongjiang Province, 150090, China.
College of Environmental Science and Engineering, Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria, Remediation and Pollution Control for Urban Ecological Environmental, Nankai University, Tianjin, 300350 China.
Environ Res. 2021 Jun;197:111054. doi: 10.1016/j.envres.2021.111054. Epub 2021 Mar 26.
Antibiotic wastewater presents serious challenges in water treatment. Metal-organic frameworks (MOFs) have received significant attention as promising precursors and sacrificial templates in the preparation of porous carbon-supported catalysts. Herein, we investigated the sulfamethoxazole (SMX) degradation and electrochemical performance of microbial fuel cells (MFCs) that applied as-prepared Ni-MOF-74 and Ni-N-C (Ni-MOF-74 underwent pyrolysis treatment at different temperatures) as air-cathode catalyst. Firstly, the electrocatalytic activity towards oxygen reduction reaction (ORR) of the catalyst was investigated by rotating disk electrode. The results showed that electron transfer number for Ni-MOF-74 was 2.12, while that of 800Ni-N-C was 3.44, which was close to four-electron reduction. Applying Ni-MOF-74 in MFCs, a maximum power density of 446 mW/m was obtained, which was close to that of 800Ni-N-C. Besides, using Ni-MOF-74 as cathode catalyst, a chemical oxygen demand removal rate of about 84% was obtained, and the degradation rate of 10 mg/L SMX was 61%. The degradation rate decreased with increasing antibiotic concentration, but the average degradation efficiency increased stepwise. Additionally, the relative abundance of resistant gene sul1 in the reactors of the new catalytic material was about 62% lower than that of sul1 in the control (Pt/C) reactors, and the relative abundance of sul2 was about 73% lower. Moreover, cost assessments related to the catalyst performance are presented. The findings of this study demonstrated that Ni-MOF-74 could be considered as a two-electron transfer ORR catalyst, and offers a promising technique for preparation of Ni-N-C for use as four-electron transfer ORR catalysts. In comparison, Ni-MOF-74 could be a promising ORR catalyst of MFCs for antibiotic degradation.
抗生素废水在水处理中带来了严峻的挑战。金属有机骨架（MOFs）作为有前途的前体和牺牲模板，在制备多孔碳负载催化剂方面受到了广泛关注。在此，我们研究了应用于制备的 Ni-MOF-74 和 Ni-N-C（Ni-MOF-74 在不同温度下进行热解处理）作为空气阴极催化剂的微生物燃料电池（MFC）中磺胺甲恶唑（SMX）的降解和电化学性能。首先，通过旋转圆盘电极研究了催化剂对氧还原反应（ORR）的电催化活性。结果表明，Ni-MOF-74 的电子转移数为 2.12，而 800Ni-N-C 的电子转移数为 3.44，接近四电子还原。在 MFC 中应用 Ni-MOF-74 时，获得了 446 mW/m 的最大功率密度，接近于 800Ni-N-C。此外，使用 Ni-MOF-74 作为阴极催化剂，获得了约 84%的化学需氧量去除率，且 10 mg/L SMX 的降解率为 61%。随着抗生素浓度的增加，降解率降低，但平均降解效率呈逐步增加趋势。此外，新催化材料反应器中抗性基因 sul1 的相对丰度比对照（Pt/C）反应器中的 sul1 低约 62%，而 sul2 的相对丰度低约 73%。此外，还提出了与催化剂性能相关的成本评估。本研究的结果表明，Ni-MOF-74 可以作为二电子转移 ORR 催化剂，为制备四电子转移 ORR 催化剂的 Ni-N-C 提供了一种有前途的技术。相比之下，Ni-MOF-74 可能是用于抗生素降解的 MFC 的有前途的 ORR 催化剂。
