SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2023, Vol. 61 ›› Issue (9): 140-146.DOI: 10.1016/j.cjche.2023.02.019

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Direct atomic-level insight into oxygen reduction reaction on size-dependent Pt-based electrocatalysts from density functional theory calculations

Fangren Qian1,2, Lishan Peng1,2, Yujuan Zhuang1,2, Lei Liu2,3, Qingjun Chen1,2,4,5   

  1. 1. School of Rare Earths, University of Science and Technology of China, Hefei 230026, China;
    2. Key Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341000, China;
    3. Center for Computational Chemistry, College of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan 430200, China;
    4. Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
    5. Langfang Technological Service Centre of Green Industry, Langfang 065001, China
  • Received:2022-11-27 Revised:2023-02-13 Online:2023-12-14 Published:2023-09-28
  • Contact: Lei Liu,E-mail:liulei@wtu.edu.cn;Qingjun Chen,E-mail:qjchen@gia.cas.cn
  • Supported by:
    The work was supported by the National Natural Science Foundation of China (92061125, 21978294), Beijing Natural Science Foundation (Z200012), Jiangxi Natural Science Foundation (20212ACB213009), DNL Cooperation Fund, CAS (DNL201921), Self-deployed Projects of Ganjiang Innovation Academy, Chinese Academy of Sciences (E055B003), and Hebei Natural Science Foundation (B2020103043).

Direct atomic-level insight into oxygen reduction reaction on size-dependent Pt-based electrocatalysts from density functional theory calculations

Fangren Qian1,2, Lishan Peng1,2, Yujuan Zhuang1,2, Lei Liu2,3, Qingjun Chen1,2,4,5   

  1. 1. School of Rare Earths, University of Science and Technology of China, Hefei 230026, China;
    2. Key Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, Ganzhou 341000, China;
    3. Center for Computational Chemistry, College of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan 430200, China;
    4. Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China;
    5. Langfang Technological Service Centre of Green Industry, Langfang 065001, China
  • 通讯作者: Lei Liu,E-mail:liulei@wtu.edu.cn;Qingjun Chen,E-mail:qjchen@gia.cas.cn
  • 基金资助:
    The work was supported by the National Natural Science Foundation of China (92061125, 21978294), Beijing Natural Science Foundation (Z200012), Jiangxi Natural Science Foundation (20212ACB213009), DNL Cooperation Fund, CAS (DNL201921), Self-deployed Projects of Ganjiang Innovation Academy, Chinese Academy of Sciences (E055B003), and Hebei Natural Science Foundation (B2020103043).

Abstract: Developing novel oxygen reduction reaction (ORR) catalysts with high activity is urgent for proton exchange membrane fuel cells. Herein, we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations, ranging from single-atom, nanocluster to bulk Pt catalysts. The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale, and the Pt38 cluster had the lowest ORR overpotential (0.46 V) compared with that of Pt111 (0.57 V) and single atom Pt (0.7 V). Moreover, we established a volcano curve relationship between the ORR overpotential and binding energy of O*EO*), confirming the intermediate species anchored on Pt38 cluster with suitable binding energy located at top of volcano curve. The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.

Key words: Density functional theory (DFT) calculations, Pt-based electrocatalysts, Oxygen reduction reaction

摘要: Developing novel oxygen reduction reaction (ORR) catalysts with high activity is urgent for proton exchange membrane fuel cells. Herein, we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations, ranging from single-atom, nanocluster to bulk Pt catalysts. The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale, and the Pt38 cluster had the lowest ORR overpotential (0.46 V) compared with that of Pt111 (0.57 V) and single atom Pt (0.7 V). Moreover, we established a volcano curve relationship between the ORR overpotential and binding energy of O*EO*), confirming the intermediate species anchored on Pt38 cluster with suitable binding energy located at top of volcano curve. The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.

关键词: Density functional theory (DFT) calculations, Pt-based electrocatalysts, Oxygen reduction reaction