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Durability and degradation mechanism of titanium nitride based electrocatalysts for PEM (proton exchange membrane) fuel cell applications

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  • Avasarala, Bharat
  • Haldar, Pradeep

Abstract

Titanium nitride (TiN) is a promising material that has a higher potential for increasing electrocatalyst durability in PEM (proton exchange membrane) fuel cells. In this report we provide an explanation for the higher catalytic performance of titanium nitride nanoparticles (TiN NP) based electrocatalyst (Pt/TiN) when compared to that of Pt/C, using XPS (X-ray photoelectron spectroscopy). We also compare its durability with that of the conventional Pt/C electrocatalyst and explain its degradation mechanism under fuel cell conditions. Unlike Pt/C which degrades significantly via the Pt agglomeration and carbon support corrosion mechanisms, we show that Pt/TiN degrades predominantly via Pt agglomeration mechanism. TiN has a higher resistance to corrosion than carbon (C) under electrochemical conditions; as a result catalyst support corrosion mechanism plays a minor role in the degradation of Pt/TiN. For a given mass and particle diameter, TiN has higher no. of catalyst support particles than C due its higher material density. As a result it is hypothesized that, for the same amount of catalyst loading on both supports, the Pt/TiN has a higher Pt particle density on its surface compared to Pt/C and can result in a faster rate of Pt particle agglomeration during the electrocatalyst degradation. This hypothesis is tested theoretically by calculating the support to catalyst particle ratio. It is observed that the support to catalyst particle ratio is 1: 21 for 20 wt% Pt/C and 1: 60 for 20 wt% Pt/TiN. The hypothesis is also tested experimentally by two different methods, the first of which is by measuring and comparing the Pt particle sizes after subjecting the Pt/TiN and Pt/C to accelerated durability tests (ADT: 0–1.3 V RHE (reversible hydrogen electrode), 1100 cyc). Secondly, the Pt particle density on the electrocatalysts is changed by varying the amount of Pt loading (10 wt% and 30 wt%) and the Pt particle size is measured at the end of ADT. Both methods lead to the same conclusion that Pt/TiN has a significantly higher Pt particle size at the end of ADT (compared to Pt/C) indicating towards its increased rate of Pt agglomeration mechanism. Furthermore, a new approach is suggested where the oxynitride layer is grown on Pt/TiN resulting in partial encapsulation of Pt particles on the surface of TiN catalyst support thereby reducing the Pt agglomeration during fuel cell operation.

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  • Avasarala, Bharat & Haldar, Pradeep, 2013. "Durability and degradation mechanism of titanium nitride based electrocatalysts for PEM (proton exchange membrane) fuel cell applications," Energy, Elsevier, vol. 57(C), pages 545-553.
    • Handle: RePEc:eee:energy:v:57:y:2013:i:c:p:545-553
    DOI: 10.1016/j.energy.2013.05.021
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    2. Yang, H.N. & Lee, D.C. & Park, K.W. & Kim, W.J., 2015. "Platinum–boron doped graphene intercalated by carbon black for cathode catalyst in proton exchange membrane fuel cell," Energy, Elsevier, vol. 89(C), pages 500-510.
    3. Chou, Chang-Chen & Liu, Cheng-Hong & Chen, Bing-Hung, 2014. "Effects of reduction temperature and pH value of polyol process on reduced graphene oxide supported Pt electrocatalysts for oxygen reduction reaction," Energy, Elsevier, vol. 70(C), pages 231-238.
    4. Kakaei, Karim & Gharibi, Hussien, 2014. "Palladium nanoparticle catalysts synthesis on graphene in sodium dodecyl sulfate for oxygen reduction reaction," Energy, Elsevier, vol. 65(C), pages 166-171.
    5. Kim, Taegyu, 2014. "NaBH4 (sodium borohydride) hydrogen generator with a volume-exchange fuel tank for small unmanned aerial vehicles powered by a PEM (proton exchange membrane) fuel cell," Energy, Elsevier, vol. 69(C), pages 721-727.
    6. Ismail, M.S. & Ingham, D.B. & Ma, L. & Hughes, K.J. & Pourkashanian, M., 2017. "Effects of catalyst agglomerate shape in polymer electrolyte fuel cells investigated by a multi-scale modelling framework," Energy, Elsevier, vol. 122(C), pages 420-430.
    7. Huang, Zhen-Ming & Su, Ay & Liu, Ying-Chieh, 2014. "Development and testing of a hybrid system with a sub-kW open-cathode type PEM (proton exchange membrane) fuel cell stack," Energy, Elsevier, vol. 72(C), pages 547-553.
    8. Hidalgo, Diana & Tommasi, Tonia & Cauda, Valentina & Porro, Samuele & Chiodoni, Angelica & Bejtka, Katarzyna & Ruggeri, Bernardo, 2014. "Streamlining of commercial Berl saddles: A new material to improve the performance of microbial fuel cells," Energy, Elsevier, vol. 71(C), pages 615-623.
    9. Lin, Rui & Wang, Hong & Zhu, Yu, 2021. "Optimizing the structural design of cathode catalyst layer for PEM fuel cells for improving mass-specific power density," Energy, Elsevier, vol. 221(C).
    10. Roudbari, Mohsen Najafi & Ojani, Reza & Raoof, Jahan Bakhsh, 2019. "Performance improvement of polymer fuel cell by simultaneously inspection of catalyst loading, catalyst content and ionomer using home-made cathodic half-cell and response surface method," Energy, Elsevier, vol. 173(C), pages 151-161.
    11. Chen, Huicui & Pei, Pucheng & Song, Mancun, 2015. "Lifetime prediction and the economic lifetime of Proton Exchange Membrane fuel cells," Applied Energy, Elsevier, vol. 142(C), pages 154-163.
    12. Oh, Taek Hyun, 2016. "A formic acid hydrogen generator using Pd/C3N4 catalyst for mobile proton exchange membrane fuel cell systems," Energy, Elsevier, vol. 112(C), pages 679-685.
    13. Alipour Moghaddam, Jafar & Parnian, Mohammad Javad & Rowshanzamir, Soosan, 2018. "Preparation, characterization, and electrochemical properties investigation of recycled proton exchange membrane for fuel cell applications," Energy, Elsevier, vol. 161(C), pages 699-709.

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