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Ir/Co-N-C的制备及其氧双功能催化性能研究
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Abstract:
构建清洁低碳的能源体系已成为全球可持续发展的关键任务,在这一转型过程中,发展高效储能技术对于提升可再生能源利用效率具有战略意义。开发具有氧双功能活性(OER/ORR)的催化剂对于燃料电池、金属空气电池器件的效率是至关重要的,贵金属铱(Ir)表现出比较优异的OER性能,然而,Ir作为贵金属,储量极为稀少,致使其成本居高不下,这一现状成为阻碍其大规模商业化推广应用的严重桎梏。开发兼具高活性、高稳定性且成本可控的非贵金属催化剂已成为推动锌空气电池产业化进程的核心课题。本文利用两步退火法结合湿法浸渍制备了低载量Ir的Ir/Co-N-C。首先通过制备金属有机骨架衍生的Co-N-C,再利用浸渍法将Ir负载在Co-N-C上获得的具有双金属位点的Ir/Co-N-C,过电位为304 mV,其过电位低于商业催化剂IrO2,且E1/2 (半波电位)达到0.824 V,表现出良好的双功能催化活性。Ir/Co-N-C的制备还提高了贵金属的原子利用率。通过本文的研究工作为双金属位点的双功能氧电催化剂的制备具有一定的参考意义。
Constructing a clean and low-carbon energy system has become a crucial task for global sustainable development. In the process of this transformation, the development of efficient energy storage technologies is of strategic significance for improving the utilization efficiency of renewable energy. Developing catalysts with bifunctional oxygen activity (OER/ORR) is of vital importance for the efficiency of fuel cells and metal-air battery devices. The noble metal iridium (Ir) exhibits relatively excellent OER performance. However, as a noble metal, Ir has an extremely scarce reserve, leading to its persistently high cost. This situation has become a serious obstacle hindering its large-scale commercial promotion and application. Developing non-noble metal catalysts with high activity, high stability, and controllable cost has become the core issue in promoting the industrialization process of zinc-air batteries. In this paper, Ir/Co-N-C was prepared by using a two-step annealing method combined with the impregnation method. Firstly, Co-N-C derived from a metal-organic framework was prepared, and then Ir was loaded onto Co-N-C by the impregnation method to obtain Ir/Co-N-C with bimetallic sites. The overpotential of Ir/Co-N-C is 304 mV, which is lower than that of the commercial catalyst IrO?, and its E?/? (half-wave potential) reaches 0.824 V, showing good bifunctional catalytic activity. The preparation of Ir/Co-N-C also improves the atomic utilization rate of noble metals. The research work in this paper has certain reference significance for the preparation of bifunctional oxygen electro-catalysts with bimetallic sites.
[1] | Cui, H., Guo, Y., Guo, L., Wang, L., Zhou, Z. and Peng, Z. (2018) Heteroatom-Doped Carbon Materials and Their Composites as Electrocatalysts for CO2 Reduction. Journal of Materials Chemistry A, 6, 18782-18793. https://doi.org/10.1039/c8ta07430e |
[2] | Luo, M., Sun, W., Xu, B.B., Pan, H. and Jiang, Y. (2020) Interface Engineering of Air Electrocatalysts for Rechargeable Zinc-Air Batteries. Advanced Energy Materials, 11, Article ID: 2002762. https://doi.org/10.1002/aenm.202002762 |
[3] | Liu, D., Tong, Y., Yan, X., Liang, J. and Dou, S.X. (2019) Recent Advances in Carbon‐Based Bifunctional Oxygen Catalysts for Zinc‐Air Batteries. Batteries & Supercaps, 2, 743-765. https://doi.org/10.1002/batt.201900052 |
[4] | Khalid, M., Bhardwaj, P.A., Honorato, A.M.B. and Varela, H. (2020) Metallic Single-Atoms Confined in Carbon Nanomaterials for the Electrocatalysis of Oxygen Reduction, Oxygen Evolution, and Hydrogen Evolution Reactions. Catalysis Science & Technology, 10, 6420-6448. https://doi.org/10.1039/d0cy01408g |
[5] | Wu, M., Zhang, G., Qiao, J., Chen, N., Chen, W. and Sun, S. (2019) Ultra-Long Life Rechargeable Zinc-Air Battery Based on High-Performance Trimetallic Nitride and NCNT Hybrid Bifunctional Electrocatalysts. Nano Energy, 61, 86-95. https://doi.org/10.1016/j.nanoen.2019.04.031 |
[6] | Wu, M., Tang, Q., Dong, F., Wang, Y., Li, D., Guo, Q., et al. (2016) The Design of Fe,N-Doped Hierarchically Porous Carbons as Highly Active and Durable Electrocatalysts for a Zn-Air Battery. Physical Chemistry Chemical Physics, 18, 18665-18669. https://doi.org/10.1039/c6cp02785g |
[7] | Dong, F., Liu, C., Wu, M., Guo, J., Li, K. and Qiao, J. (2019) Hierarchical Porous Carbon Derived from Coal Tar Pitch Containing Discrete Co-Nx-C Active Sites for Efficient Oxygen Electrocatalysis and Rechargeable Zn-Air Batteries. ACS Sustainable Chemistry & Engineering, 7, 8587-8596. https://doi.org/10.1021/acssuschemeng.9b00373 |
[8] | Chen, T., Wu, J., Zhu, C., Liu, Z., Zhou, W., Zhu, C., et al. (2021) Rational Design of Iron Single Atom Anchored on Nitrogen Doped Carbon as a High-Performance Electrocatalyst for All-Solid-State Flexible Zinc-Air Batteries. Chemical Engineering Journal, 405, Article ID: 125956. https://doi.org/10.1016/j.cej.2020.125956 |
[9] | Zhao, C., Liu, J., Wang, J., Ren, D., Yu, J., Chen, X., et al. (2021) Zinc‐Air Batteries: A δe = 0.63 V Bifunctional Oxygen Electrocatalyst Enables High‐Rate and Long‐Cycling Zinc-Air Batteries (Adv. Mater. 15/2021). Advanced Materials, 33, Article ID: 2170117. https://doi.org/10.1002/adma.202170117 |
[10] | Ma, L., Chen, S., Pei, Z., Huang, Y., Liang, G., Mo, F., et al. (2018) Single-Site Active Iron-Based Bifunctional Oxygen Catalyst for a Compressible and Rechargeable Zinc-Air Battery. ACS Nano, 12, 1949-1958. https://doi.org/10.1021/acsnano.7b09064 |
[11] | Zhou, T., Zhang, N., Wu, C. and Xie, Y. (2020) Surface/Interface Nanoengineering for Rechargeable Zn-Air Batteries. Energy & Environmental Science, 13, 1132-1153. https://doi.org/10.1039/c9ee03634b |
[12] | Wang, M., Ji, H., Liu, S., Sun, H., Liu, J., Yan, C., et al. (2020) Single-Atom Scale Metal Vacancy Engineering in Heteroatom-Doped Carbon for Rechargeable Zinc-Air Battery with Reduced Overpotential. Chemical Engineering Journal, 393, Article ID: 124702. https://doi.org/10.1016/j.cej.2020.124702 |
[13] | Yang, D., Tan, H., Rui, X. and Yu, Y. (2019) Electrode Materials for Rechargeable Zinc-Ion and Zinc-Air Batteries: Current Status and Future Perspectives. Electrochemical Energy Reviews, 2, 395-427. https://doi.org/10.1007/s41918-019-00035-5 |
[14] | Zang, W., Sumboja, A., Ma, Y., Zhang, H., Wu, Y., Wu, S., et al. (2018) Single Co Atoms Anchored in Porous N-Doped Carbon for Efficient Zinc-Air Battery Cathodes. ACS Catalysis, 8, 8961-8969. https://doi.org/10.1021/acscatal.8b02556 |
[15] | Zhong, Y., Xu, X., Wang, W. and Shao, Z. (2018) Recent Advances in Metal‐Organic Framework Derivatives as Oxygen Catalysts for Zinc‐Air Batteries. Batteries & Supercaps, 2, 272-289. https://doi.org/10.1002/batt.201800093 |
[16] | Wang, X., Liao, Z., Fu, Y., Neumann, C., Turchanin, A., Nam, G., et al. (2020) Confined Growth of Porous Nitrogen-Doped Cobalt Oxide Nanoarrays as Bifunctional Oxygen Electrocatalysts for Rechargeable Zinc-Air Batteries. Energy Storage Materials, 26, 157-164. https://doi.org/10.1016/j.ensm.2019.12.043 |
[17] | Xia, C., Zhou, Y., He, C., Douka, A.I., Guo, W., Qi, K., et al. (2021) Recent Advances on Electrospun Nanomaterials for Zinc-Air Batteries. Small Science, 1, Article ID: 2100010. https://doi.org/10.1002/smsc.202100010 |
[18] | Wang, Y., Kumar, A., Ma, M., Jia, Y., Wang, Y., Zhang, Y., et al. (2020) Hierarchical Peony-Like Feco-Nc with Conductive Network and Highly Active Sites as Efficient Electrocatalyst for Rechargeable Zn-Air Battery. Nano Research, 13, 1090-1099. https://doi.org/10.1007/s12274-020-2751-7 |
[19] | Huang, K., Guo, S., Wang, R., Lin, S., Hussain, N., Wei, H., et al. (2020) Two-Dimensional MOF/MOF Derivative Arrays on Nickel Foam as Efficient Bifunctional Coupled Oxygen Electrodes. Chinese Journal of Catalysis, 41, 1754-1760. https://doi.org/10.1016/s1872-2067(20)63613-0 |
[20] | Xu, Y.Y., et al. (2019) 2D Nitrogen‐Doped Carbon Nanotubes/Graphene Hybrid as Bifunctional Oxygen Electrocatalyst for Long‐Life Rechargeable Zn-Air Batteries. Advanced Functional Materials, 30, Article ID: 1906081. |
[21] | Chen, J., Li, H., Fan, C., Meng, Q., Tang, Y., Qiu, X., et al. (2020) Dual Single‐Atomic Ni‐N4 and Fe‐N4 Sites Constructing Janus Hollow Graphene for Selective Oxygen Electrocatalysis. Advanced Materials, 32, Article ID: 2003134. https://doi.org/10.1002/adma.202003134 |
[22] | Zhang, K., Zhang, Y., Zhang, Q., Liang, Z., Gu, L., Guo, W., et al. (2020) Metal‐Organic Framework‐Derived Fe/Cu-Substituted Co Nanoparticles Embedded in CNTs‐Grafted Carbon Polyhedron for Zn‐Air Batteries. Carbon Energy, 2, 283-293. https://doi.org/10.1002/cey2.35 |
[23] | Wang, H., Tang, C. and Zhang, Q. (2018) A Review of Precious-Metal-Free Bifunctional Oxygen Electrocatalysts: Rational Design and Applications in Zn-Air Batteries. Advanced Functional Materials, 28, Article ID: 1803329. https://doi.org/10.1002/adfm.201803329 |
[24] | Dong, F., Cai, Y., Liu, C., Liu, J. and Qiao, J. (2018) Heteroatom (B, N and P) Doped Porous Graphene Foams for Efficient Oxygen Reduction Reaction Electrocatalysis. International Journal of Hydrogen Energy, 43, 12661-12670. https://doi.org/10.1016/j.ijhydene.2018.04.118 |
[25] | Li, X., Dong, F., Xu, N., Zhang, T., Li, K. and Qiao, J. (2018) Co3O4/MnO2/Hierarchically Porous Carbon as Superior Bifunctional Electrodes for Liquid and All-Solid-State Rechargeable Zinc-air Batteries. ACS Applied Materials & Interfaces, 10, 15591-15601. https://doi.org/10.1021/acsami.7b18684 |
[26] | Han, X., Wu, X., Zhong, C., Deng, Y., Zhao, N. and Hu, W. (2017) NiCo2S4 Nanocrystals Anchored on Nitrogen-Doped Carbon Nanotubes as a Highly Efficient Bifunctional Electrocatalyst for Rechargeable Zinc-Air Batteries. Nano Energy, 31, 541-550. https://doi.org/10.1016/j.nanoen.2016.12.008 |
[27] | Qiu, H., Du, P., Hu, K., Gao, J., Li, H., Liu, P., et al. (2021) Metal and Nonmetal Codoped 3D Nanoporous Graphene for Efficient Bifunctional Electrocatalysis and Rechargeable Zn-Air Batteries. Advanced Materials, 33, Article ID: 2101386. https://doi.org/10.1002/adma.202101386 |
[28] | Xia, B.Y., Yan, Y., Li, N., Wu, H.B., Lou, X.W. and Wang, X. (2016) A Metal-Organic Framework-Derived Bifunctional Oxygen Electrocatalyst. Nature Energy, 1, Article No. 15006. https://doi.org/10.1038/nenergy.2015.6 |
[29] | Wei, L., Ang, E.H., Yang, Y., Qin, Y., Zhang, Y., Ye, M., et al. (2020) Recent Advances of Transition Metal Based Bifunctional Electrocatalysts for Rechargeable Zinc-Air Batteries. Journal of Power Sources, 477, Article ID: 228696. https://doi.org/10.1016/j.jpowsour.2020.228696 |
[30] | Xu, H., Cheng, D., Cao, D. and Zeng, X.C. (2018) Retracted Article: A Universal Principle for a Rational Design of Single-Atom Electrocatalysts. Nature Catalysis, 1, 339-348. https://doi.org/10.1038/s41929-018-0063-z |
[31] | Sun, X., Sun, S., Gu, S., Liang, Z., Zhang, J., Yang, Y., et al. (2019) High-Performance Single Atom Bifunctional Oxygen Catalysts Derived from ZIF-67 Superstructures. Nano Energy, 61, 245-250. https://doi.org/10.1016/j.nanoen.2019.04.076 |