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具有多孔海绵状结构的锚定(Fe)/FeO/N 掺杂石墨碳负载金属态 FeS 作为用于增强生物电能产生的耐用催化剂。

Metallic State FeS Anchored (Fe)/FeO/N-Doped Graphitic Carbon with Porous Spongelike Structure as Durable Catalysts for Enhancing Bioelectricity Generation.

机构信息

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, School of Chemistry and Materials Science, Heilongjiang University , Harbin 150080, China.

School of Civil Engineering, Heilongjiang Institute of Technology , Harbin 150050, China.

出版信息

ACS Appl Mater Interfaces. 2017 Mar 29;9(12):10777-10787. doi: 10.1021/acsami.7b01531. Epub 2017 Mar 20.

DOI:10.1021/acsami.7b01531
PMID:28291333
Abstract

The critical issues in practical application of microbial fuel cells (MFCs) for wastewater treatment are the high cost and poor activity and durability of precious metal catalysts. To alleviate the activity loss and kinetic barriers for oxygen reduction reaction (ORR) on cathode, (Fe)/FeO/FeS/N-doped graphitic carbon ((Fe)/FeO/FeS/NGC) is prepared as ORR catalyst through a one-step method using waste pomelo skins as carbon source. Various characterization techniques and electrochemical analyses are conducted to illustrate the correlation between structural characteristics and catalytic activity. MFCs with Fe/FeO/FeS/NGC (900 °C) cathode produces the maximum power density of 930 ± 10 mW m (Pt/C of 489 mW m) and maintains a good long-term durability, which only declines 18% after 90 day operation. Coulombic efficiency (22.2%) obtained by Fe/FeO/FeS/NGC (900 °C) cathode is significantly higher than that of Pt/C (17.3%). Metallic state FeS anchored in porous NGC skeleton can boost electron transport through the interconnected channels in spongelike structure to improve catalytic activity. Charge delocalization of C atoms can be strengthened by N atoms incorporation into carbon skeleton, which correspondingly contributes to the O chemisorptions and O-O bond weakening during ORR. Energetically existed active components (Fe and N species) are more efficient than Pt to trap and consume electrons in catalyzing ORR in wastewater containing Pt-poisoning substances (bacterial metabolites). (Fe)/FeO/FeS/NGC catalysts with the advantages of durable power outputs and environmental-friendly raw material can cover the shortages of Pt/C and provide an outlook for further applications of these catalysts.

摘要

用于废水处理的微生物燃料电池(MFC)在实际应用中存在的关键问题是贵金属催化剂成本高、活性和耐久性差。为了缓解阴极上氧气还原反应(ORR)的活性损失和动力学障碍,(Fe)/FeO/FeS/N 掺杂石墨碳((Fe)/FeO/FeS/NGC)通过一步法用废柚子皮作为碳源制备为 ORR 催化剂。采用多种表征技术和电化学分析方法阐明了结构特征与催化活性之间的关系。具有 Fe/FeO/FeS/NGC(900°C)阴极的 MFC 产生的最大功率密度为 930±10 mW m(Pt/C 为 489 mW m),并具有良好的长期耐久性,在 90 天的运行后仅下降 18%。Fe/FeO/FeS/NGC(900°C)阴极获得的库仑效率(22.2%)明显高于 Pt/C(17.3%)。锚定在多孔 NGC 骨架中的金属态 FeS 可以通过在海绵状结构中的互连通道促进电子传输,从而提高催化活性。碳原子的电荷离域可以通过氮原子掺入碳骨架得到加强,这相应地有助于 ORR 过程中的 O 化学吸附和 O-O 键削弱。在含有 Pt 中毒物质(细菌代谢物)的废水中,存在于活性组分(Fe 和 N 物种)中的能量比 Pt 更有效地捕获和消耗电子来催化 ORR。(Fe)/FeO/FeS/NGC 催化剂具有持久的功率输出和环保原料的优势,可以弥补 Pt/C 的不足,为这些催化剂的进一步应用提供了前景。

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