Out-of-plane FeII–N4 moiety modified Fe–N co-doped porous carbons as high-performance electrocatalysts for the oxygen reduction reaction,Catalysis Science & Technology

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Out-of-plane FeII–N4 moiety modified Fe–N co-doped porous carbons as high-performance electrocatalysts for the oxygen reduction reaction
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2017-08-16 00:00:00 , DOI: 10.1039/c7cy01290j
Zhongjie Qian _{1,

2,

3,

4,

5} , Zhaowen Hu _{1,

2,

3,

4,

5} , Zhengping Zhang _{1,

2,

3,

4,

5} , Zhilin Li _{1,

2,

3,

4,

5} , Meiling Dou _{1,

2,

3,

4,

5} , Feng Wang _{1,

2,

3,

4,

5}

Affiliation

Exploring high-performance iron and nitrogen co-doped carbon (Fe–N–C) electrocatalysts with desirable active sites toward the oxygen reduction reaction (ORR) is extremely important for future applications of fuel cells and metal–air batteries. Herein, we demonstrate a facile and effective strategy for the synthesis of high-performance Fe–N–C electrocatalysts by pyrolyzing a physical mixture of conventional carbon black (Black Pearls 2000, BP2000) and Hemin followed by a post-treatment procedure including acid-washing and heat-treatment. The resultant Fe–N–C electrocatalysts possessed numerous out-of-plane Fe^II–N₄ moieties (D1 sites) uniformly distributed in the porous carbon matrix, and a well-defined micro/mesoporous structure that is expected to significantly improve the ORR activity in both alkaline and acidic electrolytes. In an alkaline electrolyte, the Fe–N–C electrocatalyst exhibited a remarkable ORR activity with a high onset potential of 0.942 V and a half-wave potential of 0.848 V, which were 9 mV and 12 mV more positive than those of the commercial Pt/C, respectively, while its half-wave potential was 0.73 V, only 60 mV less than that of Pt/C in an acidic electrolyte. Furthermore, the Fe–N–C electrocatalyst also demonstrated better electrochemical durability and methanol tolerance in comparison with Pt/C in both alkaline and acidic electrolytes. This work opens a new avenue for the rational design and synthesis of highly active and durable TM–N–C electrocatalysts towards ORR.

中文翻译：

平面外Fe ^II -N ₄部分改性的Fe-N共掺杂多孔碳作为氧还原反应的高性能电催化剂

探索高性能的铁和氮共掺杂碳（Fe–N–C）电催化剂，并具有朝着氧还原反应（ORR）的理想活性位，这对于燃料电池和金属空气电池的未来应用极为重要。本文中，我们通过热解常规炭黑（Black Pearls 2000，BP2000）和物理活性炭的物理混合物，然后进行包括酸法在内的后处理程序，展示了一种合成高效Fe–N–C电催化剂的简便有效的策略。洗涤和热处理。生成的Fe–N–C电催化剂具有大量平面外Fe ^II – N ₄的部分（D1位点）均匀地分布在多孔碳基质中，并且定义明确的微/介孔结构有望显着提高碱性和酸性电解质中的ORR活性。在碱性电解液中，Fe–N–C电催化剂表现出显着的ORR活性，具有0.942 V的高起始电势和0.848 V的半波电势，比市售Pt的正电势分别高9 mV和12 mV。 / C，虽然其半波电势为0.73 V，但仅比酸性电解质中的Pt / C低60 mV。此外，与碱性和酸性电解液中的Pt / C相比，Fe–N–C电催化剂也表现出更好的电化学耐久性和甲醇耐受性。

更新日期：2017-09-18

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