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Open AccessOpen Access JUSTC Chemistry 15 July 2024

Synergistic effect of heterogeneous single atoms and clusters for improved catalytic performance

  • 1.

    Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, China

  • 2.

    School of Chemistry & Chemical Engineering, Anhui University of Technology, Ma’anshan 243002, China

Cite this:
https://doi.org/10.52396/JUSTC-2024-0046
More Information
  • Author Bio:

    Long Liu is currently a graduate student in the Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, under the supervision of Prof. Jie Zeng. His research mainly focuses on the preparation of single-atom catalysts and their applications in the oxygen evolution reaction

    Zhirong Zhang is currently an Associate Professor in the Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China (USTC). He received his Ph.D. degree from USTC under the tutelage of Prof. Jie Zeng in 2020. His research interests include the preparation of single-atom catalysts and their applications in electrocatalysis

    Jie Zeng is currently a Professor of Chemistry at Anhui University of Technology and Chair Professor at the University of Science and Technology of China (USTC). He received his B.S. degree from USTC in 2002 and Ph.D. degree in Condensed Matter Physics from USTC under the tutelage of Prof. Jianguo Hou and Prof. Xiaoping Wang in 2007. His research interests include selective and efficient conversion of carbon-based small molecules (such as CO, CO2 and CH4) to liquid fuels and high value-added chemicals from both material and mechanistic aspects

  • Corresponding author: E-mail: zzhirong@ustc.edu.cn; E-mail: zengj@ustc.edu.cn
  • Received Date: 25 March 2024
  • Accepted Date: 08 May 2024
    • Available Online: 15 July 2024
    Abstract

  • Abstract

    Electrocatalytic water splitting provides an efficient method for the production of hydrogen. In electrocatalytic water splitting, the oxygen evolution reaction (OER) involves a kinetically sluggish four-electron transfer process, which limits the efficiency of electrocatalytic water splitting. Therefore, it is urgent to develop highly active OER catalysts to accelerate reaction kinetics. Coupling single atoms and clusters in one system is an innovative approach for developing efficient catalysts that can synergistically optimize the adsorption and configuration of intermediates and improve catalytic activity. However, research in this area is still scarce. Herein, we constructed a heterogeneous single-atom cluster system by anchoring Ir single atoms and Co clusters on the surface of Ni(OH)2 nanosheets. Ir single atoms and Co clusters synergistically improved the catalytic activity toward the OER. Specifically, ConIr1/Ni(OH)2 required an overpotential of 255 mV at a current density of 10 mA·cm−2, which was 60 mV and 67 mV lower than those of Con/Ni(OH)2 and Ir1/Ni(OH)2, respectively. The turnover frequency of ConIr1/Ni(OH)2 was 0.49 s−1, which was 4.9 times greater than that of Con/Ni(OH)2 at an overpotential of 300 mV.

    Graphical abstract

    Ir single atoms and Co clusters synergistically improved the catalytic activity toward the oxygen evolution reaction.

    Abstract

    Electrocatalytic water splitting provides an efficient method for the production of hydrogen. In electrocatalytic water splitting, the oxygen evolution reaction (OER) involves a kinetically sluggish four-electron transfer process, which limits the efficiency of electrocatalytic water splitting. Therefore, it is urgent to develop highly active OER catalysts to accelerate reaction kinetics. Coupling single atoms and clusters in one system is an innovative approach for developing efficient catalysts that can synergistically optimize the adsorption and configuration of intermediates and improve catalytic activity. However, research in this area is still scarce. Herein, we constructed a heterogeneous single-atom cluster system by anchoring Ir single atoms and Co clusters on the surface of Ni(OH)2 nanosheets. Ir single atoms and Co clusters synergistically improved the catalytic activity toward the OER. Specifically, ConIr1/Ni(OH)2 required an overpotential of 255 mV at a current density of 10 mA·cm−2, which was 60 mV and 67 mV lower than those of Con/Ni(OH)2 and Ir1/Ni(OH)2, respectively. The turnover frequency of ConIr1/Ni(OH)2 was 0.49 s−1, which was 4.9 times greater than that of Con/Ni(OH)2 at an overpotential of 300 mV.

    • Public Summary

    • A heterogeneous single-atom cluster system was constructed by anchoring Ir single atoms and Co clusters on the oxygen vacancy sites of the Ni(OH)2 nanosheets.
    • The Ir single atoms were mainly coordinated with oxygen, while the Co clusters were also coordinated with oxygen and formed by the second shell of the Co-Co coordination.
    • Ir single atoms and Co clusters synergistically improved the catalytic activity and accelerated the kinetics of the oxygen evolution reaction.

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    • References(37)
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    Zeng S P, Shi H, Dai T Y, et al. Lamella-heterostructured nanoporous bimetallic iron-cobalt alloy/oxyhydroxide and cerium oxynitride electrodes as stable catalysts for oxygen evolution. Nature Communications, 2023, 14 (1): 1811. doi: 10.1038/s41467-023-37597-4
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    Xin S S, Tang Y, Jia B H, et al. Coupling adsorbed evolution and lattice oxygen mechanism in Fe-Co(OH)2/Fe2O3 heterostructure for enhanced electrochemical water oxidation. Advanced Functional Materials, 2023, 33 (45): 2305243. doi: 10.1002/adfm.202305243
    [11]
    Liu H, Zhang T F, Cui D, et al. Defective ferrocene-based metal–organic frameworks for efficient solar-powered water oxidation via the ligand competition and etching effect. Journal of Colloid and Interface Science, 2024, 657: 664–671. doi: 10.1016/j.jcis.2023.12.024
    [12]
    Wu H, Huang Q X, Shi Y Y, et al. Electrocatalytic water splitting: Mechanism and electrocatalyst design. Nano Research, 2023, 16 (7): 9142–9157. doi: 10.1007/s12274-023-5502-8
    [13]
    Iqbal S, Safdar B, Hussain I, et al. Trends and prospects of bulk and single-atom catalysts for the oxygen evolution reaction. Advanced Energy Materials, 2023, 13 (17): 2203913. doi: 10.1002/aenm.202203913
    [14]
    Zhang N, Du J Y, Zhou N, et al. High-valence metal-doped amorphous IrO x as active and stable electrocatalyst for acidic oxygen evolution reaction. Chinese Journal of Catalysis, 2023, 53: 134–142. doi: 10.1016/S1872-2067(23)64517-6
    [15]
    Zhao F Z, Mao X Y, Zheng X, et al. Roles of the self-reconstruction layer in the catalytic stability of a NiFeP catalyst during the oxygen evolution reaction. Journal of Materials Chemistry A, 2023, 11 (1): 276–286. doi: 10.1039/D2TA06514B
    [16]
    Chang J W, Zhang Q, Yu J K, et al. A Fe single atom seed-mediated strategy toward Fe3C/Fe–N–C catalysts with outstanding bifunctional ORR/OER activities. Advanced Science, 2023, 10 (22): 2301656. doi: 10.1002/advs.202301656
    [17]
    Seitz L C, Dickens C F, Nishio K, et al. A highly active and stable IrO x/SrIrO3 catalyst for the oxygen evolution reaction. Science, 2016, 353 (6303): 1011–1014. doi: 10.1126/science.aaf5050
    [18]
    Bai X F, Zhang X P, Sun Y J, et al. Low ruthenium content confined on boron carbon nitride as an efficient and stable electrocatalyst for acidic oxygen evolution reaction. Angewandte Chemie International Edition, 2023, 62 (38): e202308704. doi: 10.1002/anie.202308704
    [19]
    Zheng Y R, Vernieres J, Wang Z B, et al. Monitoring oxygen production on mass-selected iridium–tantalum oxide electrocatalysts. Nature Energy, 2022, 7 (1): 55–64. doi: 10.1038/s41560-021-00948-w
    [20]
    Ma Y D, Zhang H, Xia J, et al. Reduced CoFe2O4/graphene composite with rich oxygen vacancies as a high efficient electrocatalyst for oxygen evolution reaction. International Journal of Hydrogen Energy, 2020, 45 (19): 11052–11061. doi: 10.1016/j.ijhydene.2020.02.045
    [21]
    Cao D, Wang J Y, Xu H X, et al. Construction of dual-site atomically dispersed electrocatalysts with Ru-C5 single atoms and Ru-O4 nanoclusters for accelerated alkali hydrogen evolution. Small, 2021, 17 (31): 2101163. doi: 10.1002/smll.202101163
    [22]
    He T W, Santiago A R P, Kong Y C, et al. Atomically dispersed heteronuclear dual-atom catalysts: a new rising star in atomic catalysis. Small, 2022, 18 (12): 2106091. doi: 10.1002/smll.202106091
    [23]
    Zheng X B, Li B B, Wang Q S, et al. Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis. Nano Research, 2022, 15 (9): 7806–7839. doi: 10.1007/s12274-022-4429-9
    [24]
    Wang Z, Jin X Y, Xu R J, et al. Cooperation between dual metal atoms and nanoclusters enhances activity and stability for oxygen reduction and evolution. ACS Nano, 2023, 17 (9): 8622–8633. doi: 10.1021/acsnano.3c01287
    [25]
    Chen J J, Wang S D, Li Z Y, et al. Selective reduction of NO into N2 catalyzed by Rh1-doped cluster anions RhCe2O3-5−. Journal of the American Chemical Society, 2023, 145 (33): 18658–18667. doi: 10.1021/jacs.3c06565
    [26]
    Lee S, Bai L, Hu X. Deciphering iron-dependent activity in oxygen evolution catalyzed by nickel–iron layered double hydroxide. Angewandte Chemie International Edition, 2020, 59 (21): 8072–8077. doi: 10.1002/anie.201915803
    [27]
    Zhang Z R, Feng C, Liu C X, et al. Electrochemical deposition as a universal route for fabricating single-atom catalysts. Nature Communications, 2020, 11 (1): 1215. doi: 10.1038/s41467-020-14917-6
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    Yu J, Li Z, Liu T, et al. Morphology control and electronic tailoring of CoxAy (A = P, S, Se) electrocatalysts for water splitting. Chemical Engineering Journal, 2023, 460: 141674. doi: 10.1016/j.cej.2023.141674
    [29]
    Zhuang L, Ge L, Yang Y, et al. Ultrathin iron-cobalt oxide nanosheets with abundant oxygen vacancies for the oxygen evolution reaction. Advanced Materials, 2017, 29 (17): 1606793. doi: 10.1002/adma.201606793
    [30]
    Zheng X B, Yang J R, Xu Z F, et al. Ru–Co pair sites catalyst boosts the energetics for the oxygen evolution reaction. Angewandte Chemie International Edition, 2022, 61 (32): e202205946. doi: 10.1002/anie.202205946
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    Li W, Gao X, Xiong D, et al. Hydrothermal synthesis of monolithic Co3Se4 nanowire electrodes for oxygen evolution and overall water splitting with high efficiency and extraordinary catalytic stability. Advanced Energy Materials, 2017, 7 (17): 1602579. doi: 10.1002/aenm.201602579
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    Hou Y, Zuo F, Dagg A, et al. A three-dimensional branched cobalt-doped α-Fe2O3 nanorod/MgFe2O4 heterojunction array as a flexible photoanode for efficient photoelectrochemical water oxidation. Angewandte Chemie International Edition, 2013, 52 (4): 1248–1252. doi: 10.1002/anie.201207578
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    Figure  1.  Structural characterization of Con/Ni(OH)2, Ir1/Ni(OH)2, and ConIr1/Ni(OH)2. HAADF-STEM images of Con/Ni(OH)2 (a), Ir1/Ni(OH)2 (b), and ConIr1/Ni(OH)2 (c). EDX elemental mapping of Con/Ni(OH)2 (d), Ir1/Ni(OH)2 (e), and ConIr1/Ni(OH)2 (f).

    Figure  2.  Electronic structure characterization of Co clusters on Con/Ni(OH)2 and ConIr1/Ni(OH)2 and Ir single atoms on Ir1/Ni(OH)2 and ConIr1/Ni(OH)2. Normalized XANES (a) and EXAFS (b) spectra without phase correction at the Co K-edge of Con/Ni(OH)2 and ConIr1/Ni(OH)2. Co foil and Co2O3 were used as references. Normalized XANES (c) and EXAFS (d) spectra at the Ir L3 edge of Ir1/Ni(OH)2 and ConIr1/Ni(OH)2. Ir foil and IrO2 were used as references.

    Figure  3.  Electrocatalytic performances toward the OER. (a) Polarization curves of Ni(OH)2, Con/Ni(OH)2, Ir1/Ni(OH)2, ConIr1/Ni(OH)2 and IrO2. The measurements were conducted in 1.0 mol·L−1 KOH. (b) Overpotentials at a current density of 10 mA·cm−2 for Ni(OH)2, Con/Ni(OH)2, Ir1/Ni(OH)2, ConIr1/Ni(OH)2 and IrO2. (c) Mass activities and turnover frequencies of Con/Ni(OH)2 and ConIr1/Ni(OH)2 at an overpotential of 300 mV. (d) Comparison of the turnover frequencies of reported Co-based catalysts and ConIr1/Ni(OH)2 for the OER. (e) Tafel slopes of Ni(OH)2, Ir1/Ni(OH)2, Con/Ni(OH)2, and ConIr1/Ni(OH)2. (f) Chronopotentiometric curve of ConIr1/Ni(OH)2 toward the OER at a current density of 10 mA·cm−2 for 15 h.

    Figure  4.  Morphological and structural characterization of ConIr1/Ni(OH)2 after the durability test. (a) HAADF-STEM image. (b) EDX elemental mapping images. (c) XRD pattern. (d) Co L-edge XAS spectra. (e) Ni L-edge XAS spectra. (f) Ni 2p XPS spectra.

    [1]
    Chong L N, Wen J G, Song E H, et al. Synergistic Co–Ir/Ru composite electrocatalysts impart efficient and durable oxygen evolution catalysis in acid. Advanced Energy Materials, 2023, 13 (37): 2302306. doi: 10.1002/aenm.202302306
    [2]
    Lu X, Xue H, Gong H, et al. 2D layered double hydroxide nanosheets and their derivatives toward efficient oxygen evolution reaction. Nano-Micro Letters, 2020, 12 (1): 86. doi: 10.1007/s40820-020-00421-5
    [3]
    Liao H X, Luo T, Tan P F, et al. Unveiling role of sulfate ion in nickel-iron (oxy)hydroxide with enhanced oxygen-evolving performance. Advanced Functional Materials, 2021, 31 (38): 2102772. doi: 10.1002/adfm.202102772
    [4]
    Zhang S H, Huang S C, Sun F Z, et al. Exciting lattice oxygen of nickel-iron bimetal alkoxide for efficient electrochemical oxygen evolution reaction. Journal of Energy Chemistry, 2024, 88: 194–201. doi: 10.1016/j.jechem.2023.09.013
    [5]
    Shi M M, Bao D, Yan J M, et al. Coordination and architecture regulation of electrocatalysts for sustainable hydrogen energy conversion. Accounts of Materials Research, 2024, 5 (2): 160–172. doi: 10.1021/accountsmr.3c00197
    [6]
    Tang Y, Wu C, Zhang Q, et al. Accelerated surface reconstruction through regulating the solid-liquid interface by oxyanions in perovskite electrocatalysts for enhanced oxygen evolution. Angewandte Chemie International Edition, 2023, 62 (37): e202309107. doi: 10.1002/anie.202309107
    [7]
    Wang X, Xi S, Huang P, et al. Pivotal role of reversible NiO6 geometric conversion in oxygen evolution. Nature, 2022, 611 (7937): 702–708. doi: 10.1038/s41586-022-05296-7
    [8]
    Huang Y, Jiang L W, Shi B Y, et al. Highly efficient oxygen evolution reaction enabled by phosphorus doping of the Fe electronic structure in iron-nickel selenide nanosheets. Advanced Science, 2021, 8 (18): 2101775. doi: 10.1002/advs.202101775
    [9]
    Zeng S P, Shi H, Dai T Y, et al. Lamella-heterostructured nanoporous bimetallic iron-cobalt alloy/oxyhydroxide and cerium oxynitride electrodes as stable catalysts for oxygen evolution. Nature Communications, 2023, 14 (1): 1811. doi: 10.1038/s41467-023-37597-4
    [10]
    Xin S S, Tang Y, Jia B H, et al. Coupling adsorbed evolution and lattice oxygen mechanism in Fe-Co(OH)2/Fe2O3 heterostructure for enhanced electrochemical water oxidation. Advanced Functional Materials, 2023, 33 (45): 2305243. doi: 10.1002/adfm.202305243
    [11]
    Liu H, Zhang T F, Cui D, et al. Defective ferrocene-based metal–organic frameworks for efficient solar-powered water oxidation via the ligand competition and etching effect. Journal of Colloid and Interface Science, 2024, 657: 664–671. doi: 10.1016/j.jcis.2023.12.024
    [12]
    Wu H, Huang Q X, Shi Y Y, et al. Electrocatalytic water splitting: Mechanism and electrocatalyst design. Nano Research, 2023, 16 (7): 9142–9157. doi: 10.1007/s12274-023-5502-8
    [13]
    Iqbal S, Safdar B, Hussain I, et al. Trends and prospects of bulk and single-atom catalysts for the oxygen evolution reaction. Advanced Energy Materials, 2023, 13 (17): 2203913. doi: 10.1002/aenm.202203913
    [14]
    Zhang N, Du J Y, Zhou N, et al. High-valence metal-doped amorphous IrO x as active and stable electrocatalyst for acidic oxygen evolution reaction. Chinese Journal of Catalysis, 2023, 53: 134–142. doi: 10.1016/S1872-2067(23)64517-6
    [15]
    Zhao F Z, Mao X Y, Zheng X, et al. Roles of the self-reconstruction layer in the catalytic stability of a NiFeP catalyst during the oxygen evolution reaction. Journal of Materials Chemistry A, 2023, 11 (1): 276–286. doi: 10.1039/D2TA06514B
    [16]
    Chang J W, Zhang Q, Yu J K, et al. A Fe single atom seed-mediated strategy toward Fe3C/Fe–N–C catalysts with outstanding bifunctional ORR/OER activities. Advanced Science, 2023, 10 (22): 2301656. doi: 10.1002/advs.202301656
    [17]
    Seitz L C, Dickens C F, Nishio K, et al. A highly active and stable IrO x/SrIrO3 catalyst for the oxygen evolution reaction. Science, 2016, 353 (6303): 1011–1014. doi: 10.1126/science.aaf5050
    [18]
    Bai X F, Zhang X P, Sun Y J, et al. Low ruthenium content confined on boron carbon nitride as an efficient and stable electrocatalyst for acidic oxygen evolution reaction. Angewandte Chemie International Edition, 2023, 62 (38): e202308704. doi: 10.1002/anie.202308704
    [19]
    Zheng Y R, Vernieres J, Wang Z B, et al. Monitoring oxygen production on mass-selected iridium–tantalum oxide electrocatalysts. Nature Energy, 2022, 7 (1): 55–64. doi: 10.1038/s41560-021-00948-w
    [20]
    Ma Y D, Zhang H, Xia J, et al. Reduced CoFe2O4/graphene composite with rich oxygen vacancies as a high efficient electrocatalyst for oxygen evolution reaction. International Journal of Hydrogen Energy, 2020, 45 (19): 11052–11061. doi: 10.1016/j.ijhydene.2020.02.045
    [21]
    Cao D, Wang J Y, Xu H X, et al. Construction of dual-site atomically dispersed electrocatalysts with Ru-C5 single atoms and Ru-O4 nanoclusters for accelerated alkali hydrogen evolution. Small, 2021, 17 (31): 2101163. doi: 10.1002/smll.202101163
    [22]
    He T W, Santiago A R P, Kong Y C, et al. Atomically dispersed heteronuclear dual-atom catalysts: a new rising star in atomic catalysis. Small, 2022, 18 (12): 2106091. doi: 10.1002/smll.202106091
    [23]
    Zheng X B, Li B B, Wang Q S, et al. Emerging low-nuclearity supported metal catalysts with atomic level precision for efficient heterogeneous catalysis. Nano Research, 2022, 15 (9): 7806–7839. doi: 10.1007/s12274-022-4429-9
    [24]
    Wang Z, Jin X Y, Xu R J, et al. Cooperation between dual metal atoms and nanoclusters enhances activity and stability for oxygen reduction and evolution. ACS Nano, 2023, 17 (9): 8622–8633. doi: 10.1021/acsnano.3c01287
    [25]
    Chen J J, Wang S D, Li Z Y, et al. Selective reduction of NO into N2 catalyzed by Rh1-doped cluster anions RhCe2O3-5−. Journal of the American Chemical Society, 2023, 145 (33): 18658–18667. doi: 10.1021/jacs.3c06565
    [26]
    Lee S, Bai L, Hu X. Deciphering iron-dependent activity in oxygen evolution catalyzed by nickel–iron layered double hydroxide. Angewandte Chemie International Edition, 2020, 59 (21): 8072–8077. doi: 10.1002/anie.201915803
    [27]
    Zhang Z R, Feng C, Liu C X, et al. Electrochemical deposition as a universal route for fabricating single-atom catalysts. Nature Communications, 2020, 11 (1): 1215. doi: 10.1038/s41467-020-14917-6
    [28]
    Yu J, Li Z, Liu T, et al. Morphology control and electronic tailoring of CoxAy (A = P, S, Se) electrocatalysts for water splitting. Chemical Engineering Journal, 2023, 460: 141674. doi: 10.1016/j.cej.2023.141674
    [29]
    Zhuang L, Ge L, Yang Y, et al. Ultrathin iron-cobalt oxide nanosheets with abundant oxygen vacancies for the oxygen evolution reaction. Advanced Materials, 2017, 29 (17): 1606793. doi: 10.1002/adma.201606793
    [30]
    Zheng X B, Yang J R, Xu Z F, et al. Ru–Co pair sites catalyst boosts the energetics for the oxygen evolution reaction. Angewandte Chemie International Edition, 2022, 61 (32): e202205946. doi: 10.1002/anie.202205946
    [31]
    Li W, Gao X, Xiong D, et al. Hydrothermal synthesis of monolithic Co3Se4 nanowire electrodes for oxygen evolution and overall water splitting with high efficiency and extraordinary catalytic stability. Advanced Energy Materials, 2017, 7 (17): 1602579. doi: 10.1002/aenm.201602579
    [32]
    Yan L T, Cao L, Dai P C, et al. Metal-organic frameworks derived nanotube of nickel–cobalt bimetal phosphides as highly efficient electrocatalysts for overall water splitting. Advanced Functional Materials, 2017, 27 (40): 1703455. doi: 10.1002/adfm.201703455
    [33]
    Li M, Wang X, Liu K, et al. Reinforcing Co–O covalency via Ce(4f)–O(2p)–Co(3d) gradient orbital coupling for high-efficiency oxygen evolution. Advanced Materials, 2023, 35 (30): 2302462. doi: 10.1002/adma.202302462
    [34]
    Feng C, Zhang Z R, Wang D D, et al. Tuning the electronic and steric interaction at the atomic interface for enhanced oxygen evolution. Journal of the American Chemical Society, 2022, 144 (21): 9271–9279. doi: 10.1021/jacs.2c00533
    [35]
    Kumar P, Kannimuthu K, Zeraati A S, et al. High-density cobalt single-atom catalysts for enhanced oxygen evolution reaction. Journal of the American Chemical Society, 2023, 145 (14): 8052–8063. doi: 10.1021/jacs.3c00537
    [36]
    Li Y, Li F M, Meng X Y, et al. Ultrathin Co3O4 nanomeshes for the oxygen evolution reaction. ACS Catalysis, 2018, 8 (3): 1913–1920. doi: 10.1021/acscatal.7b03949
    [37]
    Hou Y, Zuo F, Dagg A, et al. A three-dimensional branched cobalt-doped α-Fe2O3 nanorod/MgFe2O4 heterojunction array as a flexible photoanode for efficient photoelectrochemical water oxidation. Angewandte Chemie International Edition, 2013, 52 (4): 1248–1252. doi: 10.1002/anie.201207578
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