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Defective g-C3N4 optimizes phosphate distribution in the catalytic layer and boosts the performance of high-temperature proton exchange membrane fuel cells

缺陷g-C3N4优化催化层的磷酸分布以提高高温质子 膜燃料电池的性能

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Abstract

Phosphoric acid (PA) is a vital proton-conducting medium for high-temperature proton exchange membrane fuel cells (HT-PEMFCs); however, regulating its distribution to decrease poisoning on the electrocatalysts and maintain elevated reactivity durability remains a significant challenge. In this work, defective g-C3N4 (D-C3N4) was incorporated into Pt/C catalyst layers to promote PA distribution for enhancing the intrinsic reactivity expression of catalysts. Following decoration of D-C3N4, HT-PEMFCs with low Pt loading in both the anode (0.20 mgPt cm−2) and the cathode (0.40 mgPt cm−2) exhibited a high peak power density of 672 mW cm−2 and excellent high reactivity durability (above 620 mW cm−2) after accelerated 3500 cycles, which is far superior to previously published results. This work first reveals that the acid/base interaction of D-C3N4 with PA modulates PA distribution in the catalytic layer, thereby enhancing the intrinsic reactivity expression and utilization efficiency of catalysts in HT-PEMFCs.

摘要

磷酸作为质子传导介质对于高温质子膜燃料电池是至关重要的, 但调节磷酸分布来减少电催化剂中毒及保持高反应性的稳定性仍面临 挑战. 在本工作中, 缺陷g-C3N4被分散到Pt/C催化层中促进磷酸的分布 来提高催化剂的本征活性表达. 由于缺陷g-C3N4修饰, 低铂负载量在阳 极(0.20 mgPt cm−2)和阴极(0.40 mgPt cm−2)条件下, 高温质子膜燃料电池 呈现一个高的峰功率672 mW cm−2和高反应性(高于620 mW cm−2), 且 具有3500个加速循环的优越稳定性, 该性能优于目前报道的结果. 本工 作首次揭示了缺陷g-C3N4与磷酸的酸碱相互作用可调节催化层的磷酸 分布, 从而提高催化剂的本征活性表达和利用率.

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Acknowledgements

This work was financially supported by the National Key R&D Program of China (2021YFA1500900), the National Natural Science Foundation of China (22102053, 21825201 and U19A2017), the Provincial Natural Science Foundation of Hunan (2016TP1009, 2020JJ5045 and 2022JJ10006), the Science and Technology Innovation Program of Hunan Province (2022RC1036), the Major Program of the Natural Science Foundation of Hunan Province (2021JC0006), Hunan Graduate Education Innovation Project and Professional Ability Improvement Project (CX20210400), the Basic and Applied Basic Research Foundation of Guangdong Province-Regional joint fund project (2021B1515120024), and Shenzhen Science and Technology Programs (JCYJ20200109110416441).

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Authors and Affiliations

  1. State Key Laboratory of Chem/Bio-Sensing and Chemometrics, Provincial Hunan Key Laboratory for Graphene Materials and Devices, College of Chemistry and Chemical Engineering, the National Supercomputer Centers in Changsha, Hunan University, Changsha, 410082, China

    Dongcai Zhang  (张东材), Zhijie Kong  (孔志杰), Gen Huang  (黄根), Shiqian Du  (杜石谦), Jiaqi Lin  (林嘉祺), Yanyong Wang  (王燕勇), Gang Yu  (余刚), Li Tao  (陶李) & Shuangyin Wang  (王双印)

  2. Shenzhen Research Institute, Hunan University, Shenzhen, 518000, China

    Li Tao  (陶李) & Shuangyin Wang  (王双印)

Authors
  1. Dongcai Zhang  (张东材)
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  2. Zhijie Kong  (孔志杰)
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  3. Gen Huang  (黄根)
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  4. Shiqian Du  (杜石谦)
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  5. Jiaqi Lin  (林嘉祺)
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  6. Yanyong Wang  (王燕勇)
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  7. Gang Yu  (余刚)
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  8. Li Tao  (陶李)
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  9. Shuangyin Wang  (王双印)
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Contributions

Zhang D, Yu G, Tao L, and Wang S designed the project. Zhang D, Kong Z, Huang G, Du S and Lin J synthesized the compounds and performed the sample characterizations; Zhang D and Du S performed multiple information encryption applications. Zhang D, Yu G, Tao L, and Wang S analyzed the experimental data and co-wrote the manuscript. All the authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Gang Yu  (余刚), Li Tao  (陶李) or Shuangyin Wang  (王双印).

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The authors declare that they have no conflict of interest.

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Supplementary information

Experimental details and supporting data are available in the online version of the paper.

Dongcai Zhang received his Master’s degree in 2019 from the Central South University. He is currently a PhD candidate under the supervision of Prof. Shuangyin Wang at Hunan University. His research interest is now focused on advanced materials for electrochemical energy conversion and storage systems including high-temperature proton exchange membrane fuel cells and lithium-ion batteries.

Li Tao received his Master degree in 2016 and his PhD degree in 2019 from Hunan University under the supervision of Prof. Shuangyin Wang. He is currently an assistant professor at the Key Laboratory for Graphene Materials and Devices and the College of Chemistry and Chemical Engineering, Hunan University. His research interests are plasma technology, defect chemistry and fuel cells.

Shuangyin Wang received his Bachelor’s degree in 2006 from Zhejiang University and his PhD degree in 2010 from Nanyang Technological University, Singapore. He is currently a professor at the Key Laboratory for Graphene Materials and Devices and the College of Chemistry and Chemical Engineering, Hunan University. His research interests are defect chemistry of electrocatalysts, HT-PEMFC, and electrosynthesis.

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Defective g-C3N4 optimizes phosphate distribution in the catalytic layer and boosts the performance of high-temperature proton exchange membrane fuel cells

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Zhang, D., Kong, Z., Huang, G. et al. Defective g-C3N4 optimizes phosphate distribution in the catalytic layer and boosts the performance of high-temperature proton exchange membrane fuel cells. Sci. China Mater. 66, 3468–3474 (2023). https://doi.org/10.1007/s40843-023-2486-3

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  • DOI: https://doi.org/10.1007/s40843-023-2486-3

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