ACS Publications. Most Trusted. Most Cited. Most Read
My Activity

A High-Performance Ruddlesden–Popper Perovskite for Bifunctional Oxygen Electrocatalysis

Cite this: ACS Catal. 2020, 10, 22, 13437–13444
Publication Date (Web):November 4, 2020
Copyright © 2020 American Chemical Society

    Article Views





    Read OnlinePDF (3 MB)
    Supporting Info (1)»


    Abstract Image

    Highly active and stable bifunctional materials for the oxygen evolution/reduction reaction (OER/ORR) are critical for developing high-performance metal–air batteries and fuel cells. This study demonstrates the significantly enhanced electrocatalytic activity of a Ruddlesden–Popper (RP) perovskite (An+1BnO3n+1, n = 3) as a bifunctional material [i.e., RP-LaSr3(Co0.5Fe0.5)3O10−δ] for oxygen electrocatalysis via an optimal doping strategy. The improved performance mainly benefits from the enhanced oxygen vacancies, the facile oxygen release and incorporation abilities, the synergistic interplay of Co and Fe together with the increased amounts of adsorbed OH/O2, and the highly oxidative O22–/O. The more positive onset potential (Eonset) and the highest half wave potential (E1/2) of RP-LaSr3(Co0.5Fe0.5)3O10−δ imply a better ORR activity relative to those of the benchmark Ba0.5Sr0.5Co0.8Fe0.2O2.59 (BSCF) and the widely referred cubic perovskite (La0.6Sr0.4)0.95Co0.2Fe0.8O3−δ (CP-LSCF). Furthermore, this material enables the electrochemical reduction of O2 by 4e to OH with an impressive stability. More importantly, RP-LaSr3Co1.5Fe1.5O10−δ shows a largely narrowed potential gap (ΔE) and achieves its minimum value of 0.91 V, remarkably smaller than those of CP-LSCF (1.01 V), BSCF (1.04 V), and most of the state-of-the-art bifunctional materials. This study paves an attractive way to accurately fabricate RP-type perovskites as highly efficient and stable materials for bifunctional oxygen electrocatalysis.

    Supporting Information

    Jump To

    The Supporting Information is available free of charge at

    • Preparations and characterizations of materials; electrode preparation and electrochemical measurements; XRD patterns and XPS spectra of Co 2p, Fe 2p, and O 1s of CP-LSCF and BSCF; SEM images, representative XPS spectra, oxygen vacancy (δ), BET specific surface areas, LSVs, and CVs of RP-LaSr3ComFe3–mO10−δ, BSCF, and CP-LSCF; K–L plots of RP-LaSr3ComFe3–mO10−δ at 0.4 V; LSVs for the determination of NC; transferred electron numbers and H2O2 selectivity against potential; long-term stabilities; TEM images and XRD patterns of LaSr3Co1.5Fe1.5O10−δ after tests; stabilities using a graphite rod and Pt mesh as auxiliary electrodes; LSVs at 1600 rpm, Tafel plots, MAs, and SAs for the OER; CVs of RP-LaSr3ComFe3–mO10−δ in 0.1, 1.0, and 5.0 M KOH; and ratios of Co2+/Co3+ and Fe2+/Fe3+ of RP-LaSr3ComFe3–mO10−δ (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system:

    Cited By

    This article is cited by 36 publications.

    1. K. Woon Tan, C. Yian Haw, Wee-Jun Ong, P. Sim Khiew, N. Aimi Jani, W. Siong Chiu. Surpassing 2D Photoabsorbers with Palm Fiber Upcycling as Highly Hydrophilic and Low-Cost Photothermal Materials for Improved Water Transport Interfacial Solar Steam Generation. ACS Applied Engineering Materials 2023, 1 (6) , 1482-1492.
    2. Yawen Dai, Jie Yu, Zhenbao Zhang, Shuo Zhai, Chun Cheng, Siyuan Zhao, Peng Tan, Zongping Shao, Meng Ni. Regulating the Interfacial Electron Density of La0.8Sr0.2Mn0.5Co0.5O3/RuOx for Efficient and Low-Cost Bifunctional Oxygen Electrocatalysts and Rechargeable Zn-Air Batteries. ACS Applied Materials & Interfaces 2021, 13 (51) , 61098-61106.
    3. Binze Zhang, Yanhong Wan, Zihui Hua, Kaibin Tang, Changrong Xia. Tungsten-Doped PrBaFe2O5+δ Double Perovskite as a High-Performance Electrode Material for Symmetrical Solid Oxide Fuel Cells. ACS Applied Energy Materials 2021, 4 (8) , 8401-8409.
    4. Hainan Sun, Wei Zhou. Progress on X-ray Absorption Spectroscopy for the Characterization of Perovskite-Type Oxide Electrocatalysts. Energy & Fuels 2021, 35 (7) , 5716-5737.
    5. Jiajia Huang, Tong Su, Huibin Zhao, Fengjiao Li, Te-Wei Chiu, Manish Singh, Qixing Wu, Liangdong Fan. Nano and phase engineering of Fe-Cu alloy exsolved perovskite oxide-based hetero-catalysts for efficient oxygen evolution reaction. Fuel 2024, 356 , 129479.
    6. Wenyun Zhu, Jiani Chen, Dongliang Liu, Guangming Yang, Wei Zhou, Ran Ran, Jie Yu, Zongping Shao. Engineering the oxygen-evolution activity by changing the A-site rare-earth elements in RSr 3 Fe 1.5 Co 1.5 O 10− δ (R = La, Nd, Pr) Ruddlesden–Popper perovskites. Materials Chemistry Frontiers 2023, 7 (19) , 4526-4534.
    7. Juan Bai, Jing Shang, Jun Mei, Dongchen Qi, Ting Liao, Ziqi Sun. Triphenylphosphine‐Assisted Exsolution Engineering on Ruddlesden–Popper Perovskites for Promoting Oxygen Evolution. ENERGY & ENVIRONMENTAL MATERIALS 2023, 1
    8. Yanzhu Deng, Juwei Du, Yan Zhu, Ling Zhao, Huanwen Wang, Yansheng Gong, Jun Jin, Beibei He, Rui Wang. Interface engineering of Ruddlesden–Popper perovskite/CeO2/carbon heterojunction for rechargeable zinc-air batteries. Journal of Colloid and Interface Science 2023, 51
    9. Xiaojing Liu, Shuyi Cao, Jingde Li, Yanji Wang, Wei Xue, Guihua Liu. Protective Cerium Oxide Coating Promoted Ce‐Doping and Reconstruction of High‐Valence NiFe Sulfide toward Robust Overall Water Splitting. Small 2023,
    10. Xiangrong Ren, Yiyue Zhai, Peijun Wang, Zhuo Xu, Shiqin Gao, Xiao Chen, Qinfen Gu, Bolun Wang, Jiyang Li, Shengzhong (Frank) Liu. Surface Restructuring of Zeolite‐Encapsulated Halide Perovskite to Activate Lattice Oxygen Oxidation for Water Electrolysis. Advanced Materials 2023, 593
    11. Shan Wang, Ping Xiao, Jie Yang, Sónia A. C. Carabineiro, Marek Wiśniewski, Junjiang Zhu, Xinying Liu. Catalytic combustion of volatile organic compounds using perovskite oxides catalysts—a review. Frontiers of Chemical Science and Engineering 2023, 235
    12. Lucia Hughes, Ahin Roy, Clive Downing, Michelle P. Browne, Ainur Zhussupbekova, Igor V. Shvets, Valeria Nicolosi. Surface Reduced Manganese States as a Source of Oxygen Reduction Activity in BaMnO 3. Advanced Functional Materials 2023, 33 (24)
    13. Yiyue Zhai, Xiangrong Ren, Yu Sun, Deng Li, Bolun Wang, Shengzhong (Frank) Liu. Synergistic effect of multiple vacancies to induce lattice oxygen redox in NiFe-layered double hydroxide OER catalysts. Applied Catalysis B: Environmental 2023, 323 , 122091.
    14. Meng Chen, Nutthaphak Kitiphatpiboon, Changrui Feng, Abuliti Abudula, Yufei Ma, Guoqing Guan. Recent progress in transition-metal-oxide-based electrocatalysts for the oxygen evolution reaction in natural seawater splitting: A critical review. eScience 2023, 3 (2) , 100111.
    15. Shiyu Ma, Miao Yang, Na Han, Lifen Shi, Liang Wang, Jilin Bai, Dehua Xiong. CuCoO 2 nanocrystals derived from an isopropanol-modified Cu-BTC using alkaline water oxidation. New Journal of Chemistry 2023, 47 (11) , 5216-5223.
    16. Chaohang Liu, Feng Wang, Yue Ni, Shun Wang, Bin Qian, Qing Ni, Yifeng Zheng, Han Chen, Lin Ge. Ta-doped PrBaFe2O5+δ double perovskite as a high-performance electrode material for symmetrical solid oxide fuel cells. International Journal of Hydrogen Energy 2023, 48 (26) , 9812-9822.
    17. Chenyu Xu, Jing-Li Luo. Understanding the light-induced oxygen vacancy in the photochemical conversion. Journal of Physics: Energy 2023, 5 (1) , 011001.
    18. Shun Wang, Bin Qian, Yuxuan Tang, Qing Ni, Yifeng Zheng, Han Chen, Lin Ge, Hui Yang. Enhanced oxygen bulk diffusion of La0.6Sr0.4FeO3-δ fuel electrode by high valence transition metal doping for direct CO2 electrolysis in solid oxide electrolysis cells. Electrochimica Acta 2023, 439 , 141659.
    19. Shiyu Ma, Jilin Bai, Li Sun, Lihong Zhao, Hao Tan, Lifeng Liu, Zhigang Peng, Xiujian Zhao, Dehua Xiong. Investigation of polyethylene glycol (PEG) assisted solvothermal synthesis of CuCoO 2 nanosheets for efficient oxygen evolution reaction. Dalton Transactions 2023, 268
    20. Xiaolun Zhu, Nan He, Junxia Ding, Ruimei Yue, Simin He, Wentong Liu, Nijuan Liu, Ruibin Guo, Zunli Mo. Bimetal-anchored covalent organic frameworks derivatives for efficient alkaline electrolyte oxygen evolution. Journal of Alloys and Compounds 2022, 924 , 166442.
    21. Kaixin Li, Zhanhua Dong, Zhe Lü. Study of the bifunctional catalytic activity on Sr and Mn co-doped PrFeO3-δ Zinc-Air batteries cathode. Electrochimica Acta 2022, 430 , 141123.
    22. Wei Quan, Tianyi Chen, Siwen Sun, Chenghua Sun, Chengzhang Wu. Facile hybrid strategy of SrCo0.5Fe0.3Mo0.2O3-δ/Co3O4 heterostructure for efficient oxygen evolution reaction. Journal of Alloys and Compounds 2022, 917 , 165508.
    23. Mengfei Zhang, Peimiao Zou, Georgina Jeerh, Boyao Sun, Marc Walker, Shanwen Tao. Oxygen Vacancy‐Rich La 0.5 Sr 1.5 Ni 0.9 Cu 0.1 O 4–δ as a High‐Performance Bifunctional Catalyst for Symmetric Ammonia Electrolyzer. Advanced Functional Materials 2022, 32 (38)
    24. Fuyue Liu, Ruigan Hu, Haoqi Qiu, He Miao, Qin Wang, Jinliang Yuan. Constructing high-activity Cobalt‐based Perovskite hybrid by a top-down phase evolution method for the direct seawater electrolysis anode. Journal of Alloys and Compounds 2022, 913 , 165342.
    25. Guohong Pan, Yanzhu Deng, Ling Zhao, Huanwen Wang, Rui Wang, Jun Jin, Yansheng Gong, Beibei He. In-situ construction of Ruddlesden-Popper/perovskite heterointerface induces efficient bifunctional oxygen electrocatalyst for rechargeable zinc-air batteries. Electrochimica Acta 2022, 424 , 140673.
    26. Qianwei Liang, Yawen Liu, Ziqian Xue, Ziyu Zhao, Guangqin Li, Jianqiang Hu. Multiscale structural regulation of metal–organic framework nanofilm arrays for efficient oxygen evolution reaction. Chemical Communications 2022, 58 (49) , 6966-6969.
    27. Han Gao, Miao Yang, Zijuan Du, Xing Liu, Xianglong Dai, Kun Lin, Xiao-Qing Bao, Hong Li, Dehua Xiong. Metal–organic framework derived bimetal oxide CuCoO 2 as efficient electrocatalyst for the oxygen evolution reaction. Dalton Transactions 2022, 51 (15) , 5997-6006.
    28. Suranjana Patowary, Rashmi Chetry, Chiranjita Goswami, Bhugendra Chutia, Pankaj Bharali. Oxygen Reduction Reaction Catalysed by Supported Nanoparticles: Advancements and Challenges. ChemCatChem 2022, 14 (7)
    29. Yan Hu, Man Guo, Chuan Hu, Jiaxin Dong, Puxuan Yan, Tayirjan Taylor Isimjan, Xiulin Yang. Engineering cobalt nitride nanosheet arrays with rich nitrogen defects as a bifunctional robust oxygen electrocatalyst in rechargeable Zn–air batteries. Journal of Colloid and Interface Science 2022, 608 , 2066-2074.
    30. Jing Li, Tongtao Wan, Jingde Li, Zisheng Zhang, Yanji Wang, Guihua Liu. Three-dimensionally ordered mesoporous trimetal sulfide as efficient electrocatalyst for rechargeable zinc-air batteries. Applied Surface Science 2022, 575 , 151728.
    31. Surendra B. Karki, Ram Krishna Hona, Farshid Ramezanipour. Electrocatalytic activity and structural transformation of Ca2Sr2Mn2MO10-δ (M = Fe, Co). Ionics 2022, 28 (1) , 397-406.
    32. Maria Laura Tummino. SrFeO3 peculiarities and exploitation in decontamination processes and environmentally-friendly energy applications. Current Research in Green and Sustainable Chemistry 2022, 5 , 100339.
    33. Chengzhang Wu, Wei Quan, Tianyi Chen, Siwen Sun, Chenghua Sun. Facile Hybrid Strategy of Srco0.5fe0.3mo0.2o3-Δ/Co3o4 Heterostructure for Efficient Oxygen Evolution Reaction. SSRN Electronic Journal 2022, 28
    34. Youngjae Hong, Pilgyu Byeon, Jumi Bak, Yoon Heo, Hye-Sung Kim, Hyung Bin Bae, Sung-Yoon Chung. Local-electrostatics-induced oxygen octahedral distortion in perovskite oxides and insight into the structure of Ruddlesden–Popper phases. Nature Communications 2021, 12 (1)
    35. Ruiqin Gao, Meng Deng, Qing Yan, Zhenxing Fang, Lichun Li, Haoyu Shen, Zhengfei Chen. Structural Variations of Metal Oxide‐Based Electrocatalysts for Oxygen Evolution Reaction. Small Methods 2021, 5 (12)
    36. Yichen Zhang, Shugui Hua, Xiaoqin Sun, Zhuoyue Liu, Yuan Dang, Liang Zhang, Yuanzhen Zhou. A novel electrochemical cathode based on sea urchin-like NiO/Co3O4 composite inducing efficient Fenton-like process for levofloxacin degradation. Applied Catalysis A: General 2021, 628 , 118403.

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    Pair your accounts.

    Export articles to Mendeley

    Get article recommendations from ACS based on references in your Mendeley library.

    You’ve supercharged your research process with ACS and Mendeley!

    STEP 1:
    Click to create an ACS ID

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Please note: If you switch to a different device, you may be asked to login again with only your ACS ID.

    Your Mendeley pairing has expired. Please reconnect