Toward Pt-Free Anion-Exchange Membrane Fuel Cells: Fe–Sn Carbon Nitride–Graphene Core–Shell Electrocatalysts for the Oxygen Reduction Reaction,Chemistry of Materials

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Toward Pt-Free Anion-Exchange Membrane Fuel Cells: Fe–Sn Carbon Nitride–Graphene Core–Shell Electrocatalysts for the Oxygen Reduction Reaction
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-03-25 00:00:00 , DOI: 10.1021/acs.chemmater.7b05323
Enrico Negro _{1,

2,

3} , Antoine Bach Delpeuch ₁ , Keti Vezzù _{1,

3} , Graeme Nawn ₁ , Federico Bertasi _{1,

2} , Alberto Ansaldo ₄ , Vittorio Pellegrini ₄ , Beata Dembinska ₅ , Sylwia Zoladek ₅ , Krzysztof Miecznikowski ₅ , Iwona A. Rutkowska ₅ , Magdalena Skunik-Nuckowska ₅ , Pawel J. Kulesza ₅ , Francesco Bonaccorso ₂ , Vito Di Noto _{1,

3,

6}

Affiliation

We report on the development of two new Pt-free electrocatalysts (ECs) for the oxygen reduction reaction (ORR) process based on graphene nanoplatelets (GNPs). We designed the ECs with a core–shell morphology, where a GNP core support is covered by a carbon nitride (CN) shell. The proposed ECs present ORR active sites that are not associated with nanoparticles of metal/alloy/oxide but are instead based on Fe and Sn subnanometric clusters bound in coordination nests formed by carbon and nitrogen ligands of the CN shell. The performance and reaction mechanism of the ECs in the ORR are evaluated in an alkaline medium by cyclic voltammetry with the thin-film rotating ring-disk approach and confirmed by measurements on gas-diffusion electrodes. The proposed GNP-supported ECs present an ORR overpotential of only ca. 70 mV higher with respect to a conventional Pt/C reference EC including a XC-72R carbon black support. These results make the reported ECs very promising for application in anion-exchange membrane fuel cells. Moreover, our methodology provides an example of a general synthesis protocol for the development of new Pt-free ECs for the ORR having ample room for further performance improvement beyond the state of the art.

中文翻译：

迈向无Pt阴离子交换膜燃料电池：氧还原反应的Fe-Sn氮化碳-石墨烯核-壳电催化剂

我们报告了基于石墨烯纳米片（GNP）的两种新的无铂电催化剂（ECs）的氧还原反应（ORR）过程的开发。我们设计了具有核-壳形态的EC ，其中GNP核支架被氮化碳（CN）壳覆盖。拟议的EC呈现ORR活性位点，该活性位点与金属/合金/氧化物的纳米颗粒无关，而是基于Fe和Sn的亚纳米簇，它们结合在CN壳的碳和氮配体形成的配位巢中。在碱性介质中，采用薄膜旋转环盘法，通过循环伏安法评估了ORR中EC的性能和反应机理，并通过在气体扩散电极上的测量来证实。拟议中的由GNP支持的EC的ORR超电势仅约为。相对于包括XC-72R炭黑载体的常规Pt / C参考EC高70 mV。这些结果使所报道的EC在阴离子交换膜燃料电池中的应用非常有前途。此外，我们的方法论为开发用于ORR的新型无Pt EC提供了通用综合协议的示例，该协议具有足够的空间来进一步提高性能，超越现有技术水平。

更新日期：2018-03-25

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