Engineering Triple Phase Interface and Axial Coordination Design of Single-Atom Electrocatalysts for Rechargeable Zn─air Batteries
Chun Hua
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorDaixin Ye
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorCong Chen
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorCongli Sun
States State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070 P. R. China
Search for more papers by this authorJianhui Fang
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorCorresponding Author
Lijia Liu
Department of Chemistry, Western University, 1151 Richmond Street, London, ON, N6A5B7 Canada
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorCorresponding Author
Hui Bai
State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, Shanxi, 030024 China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorYa Tang
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorCorresponding Author
Hongbin Zhao
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorJiujun Zhang
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorChun Hua
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorDaixin Ye
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorCong Chen
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorCongli Sun
States State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070 P. R. China
Search for more papers by this authorJianhui Fang
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorCorresponding Author
Lijia Liu
Department of Chemistry, Western University, 1151 Richmond Street, London, ON, N6A5B7 Canada
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorCorresponding Author
Hui Bai
State Key Laboratory of Clean and Efficient Coal Utilization, Taiyuan University of Technology, Taiyuan, Shanxi, 030024 China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorYa Tang
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorCorresponding Author
Hongbin Zhao
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
E-mail: [email protected]; [email protected]; [email protected]
Search for more papers by this authorJiujun Zhang
Department of Chemistry & Institute for Sustainable Energy/College of Sciences, Shanghai University, Shanghai, 200444 P. R. China
Search for more papers by this authorAbstract
Bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are highly desirable for rechargeable Zn─air batteries (rZABs). Herein, a space optimized 3D heterostructure Co-N-C@MoS2 catalyst with Co single atom and Co cluster sites is developed by pyrolysis of ZIF-67 and in situ grown ultrathin MoS2 nanosheets. The introduced MoS2 not only has abundant defective structures, but also regulates the Co electronic distribution, thus introducing additional active sites and enhancing Co-Nx activity. In addition, the MoS2 modification leads to an appropriate increase in hydrophilicity which can make a stable liquid/gas/solid triple phase interface, facilitating the approachability of electrolytes into the porous channels and promotes the mass transfer through ensuring a favorite contact among the catalyst, electrolyte and reactants and enhancing utility of active reaction sites. Comprehensive analysis and theoretical simulation indicate that the enhancement of activity stems from the axial coordination of Co cluster over Co single-atom active sites to regulate local electronic structure, thereby optimizing the adsorption of ORR intermediates and enhancing the catalytic activity. Compared with the commercial Pt/C and IrO2, the structurally optimized Co-N-C@MoS2 catalyst displays exceptional bifunctional electrocatalytic activity and long-time stability toward both OER and ORR. Moreover, the Co-N-C@MoS2 catalyst exhibits higher peak power density and superior stability in liquid and flexible ZABs compared to the commercial Pt/C + IrO2 catalyst.
Conflict of Interest
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
Supporting Information
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| smll202412696-sup-0001-SuppMat.docx2.6 MB | Supporting Information |
Please note: The publisher is not responsible for the content or functionality of any supporting information supplied by the authors. Any queries (other than missing content) should be directed to the corresponding author for the article.
References
- 1D. Wu, C. Peng, C. Yin, H. Tang, Electrochem. Energy Rev. 2020, 3, 466.
- 2J. Li, B. Jiang, L. Yang, Y. Sun, H. Li, H. Shen, H. Dou, X. Xiao, M. Xu, Y. Zhai, C. Zhang, L. Zhang, Z. Chen, Angew. Chem., Int. Ed. 2024, 63, 202412566.
- 3Y. Zhou, R. Lu, X. Tao, Z. Qiu, G. Chen, J. Yang, Y. Zhao, X. Feng, K. Müllen, J. Am. Chem. Soc. 2023, 145, 3647.
- 4S. Zago, L. C. Scarpetta-Pizo, J. H. Zagal, S. Specchia, Electrochem. Energy Rev. 2024, 7, 1.
- 5X. Hu, X. Chen, X. Li, C. Xu, Adv. Funct. Mater. 2024, 34, 2316699.
- 6X. Shi, Z. Pu, B. Chi, S. Yu, J. Hu, S. Sun, S. Liao, Small 2024, 20, 2307011.
- 7Y. Guo, P. Yuan, J. Zhang, H. Xia, F. Cheng, M. Zhou, J. Li, Y. Qiao, S. Mu, Q. Xu, Adv. Funct. Mater. 2018, 28, 1805641.
- 8A. Muthurasu, A. P. Tiwari, K. Chhetri, B. Dahal, H. Y. Kim, Nano Energy 2021, 88, 106238.
- 9E. V. Rebrov, P.-Z. Gao, Catalysts 2023, 13, 1289.
- 10X. F. Lu, Y. Chen, S. Wang, S. Gao, X. W. Lou, Adv. Mater. 2019, 31, 1902339.
- 11E. Y. Choi, D. E. Kim, S. Y. Lee, C. B. Park, C. K. Kim, Appl. Catal. B-Environ. 2023, 325, 122386.
- 12Z. Yang, C. Zhao, Y. Qu, H. Zhou, F. Zhou, J. Wang, Y. Wu, Y. Li, Adv. Mater. 2019, 31, 1808043.
- 13Z. Lu, B. Wang, Y. Hu, W. Liu, Y. Zhao, R. Yang, Z. Li, J. Luo, B. Chi, Z. Jiang, M. Li, S. Mu, S. Liao, J. Zhang, X. Sun, Angew. Chem., Int. Ed. 2019, 58, 2622.
- 14X. Tan, J. Zhang, F. Cao, Y. Liu, H. Yang, Q. Zhou, X. Li, R. Wang, Z. Li, H. Hu, Q. Zhao, M. Wu, Adv. Sci. 2024, 11, 2306599.
- 15H. Chang, Y.-F. Guo, X. Liu, P.-F. Wang, Y. Xie, T.-F. Yi, Appl. Catal. B-Environ. 2023, 327, 122469.
- 16J. Rong, E. Gao, N. Liu, W. Chen, X. Rong, Y. Zhang, X. Zheng, H. Ao, S. Xue, B. Huang, Z. Li, F. Qiu, Y. Qian, Energy Storage Mater. 2023, 56, 165.
- 17X. Sun, S. Sun, S. Gu, Z. Liang, J. Zhang, Y. Yang, Z. Deng, P. Wei, J. Peng, Y. Xu, C. Fang, Q. Li, J. Han, Z. Jiang, Y. Huang, Nano Energy 2019, 61, 245.
- 18Y. Guo, J. Tang, Z. Wang, Y.-M. Kang, Y. Bando, Y. Yamauchi, Nano Energy 2018, 47, 494.
- 19X. Wang, Y. Chen, F. Li, R. K. Miao, J. E. Huang, Z. Zhao, X.-Y. Li, R. Dorakhan, S. Chu, J. Wu, S. Zheng, W. Ni, D. Kim, S. Park, Y. Liang, A. Ozden, P. Ou, Y. Hou, D. Sinton, E. H. Sargent, Nat. Commun. 2024, 15, 616.
- 20L. Yan, B. Xie, C. Yang, Y. Wang, J. Ning, Y. Zhong, Y. Hu, Adv. Energy Mater. 2023, 13, 2204245.
- 21W. Fang, H. Hu, T. Jiang, G. Li, M. Wu, Carbon 2019, 146, 476.
- 22Y. Ma, D. Leng, X. Zhang, J. Fu, C. Pi, Y. Zheng, B. Gao, X. Li, N. Li, P. K. Chu, Y. Luo, K. Huo, Small 2022, 18, 2203173.
- 23N. Yu, H. Chen, J. Kuang, K. Bao, W. Yan, J. Ye, Z. Yang, Q. Huang, Y. Wu, S. Sun, Nano Res. 2022, 15, 7209.
- 24J. Dong, B. An, W. Liu, H. Su, N. Li, Y. Gao, L. Ge, Chem. Eng. J. 2024, 498, 155102.
- 25Q. Hua, K. E. Madsen, A. M. Esposito, X. Chen, T. J. Woods, R. T. Haasch, S. Xiang, A. I. Frenkel, T. T. Fister, A. A. Gewirth, ACS Catal. 2022, 12, 1139.
- 26C. He, L. Cui, X. Wu, Y. Cai, Z. Ma, X. Zhong, H. Wang, Q. Li, Y. Huang, Q. Pan, ACS Appl. Energy Mater. 2021, 4, 9498.
- 27X. Li, C. Wang, F. Liu, Z. Zhang, J. Ali, Q. Long, J. Zhang, Chem. Eng. J. 2021, 404, 126556.
- 28L. Zhu, Z. Wang, C. Li, H. Li, Y. Huang, H. Li, Z. Wu, S. Lin, N. Li, X. Zhu, Y. Sun, J. Mater. Chem. A 2022, 10, 21013.
- 29Y. He, S. Hwang, D. A. Cullen, M. A. Uddin, L. Langhorst, B. Li, S. Karakalos, A. J. Kropf, E. C. Wegener, J. Sokolowski, M. Chen, D. Myers, D. Su, K. L. More, G. Wang, S. Litster, G. Wu, Energy Environ. Sci. 2019, 12, 250.
- 30M. Wang, Z. Wan, X. Meng, Z. Li, X. Ding, P. Li, C. Li, J.-G. Wang, Z. Li, Appl. Catal. B-Environ. 2022, 309, 121272.
- 31P. Kumar, K. Kannimuthu, A. S. Zeraati, S. Roy, X. Wang, X. Wang, S. Samanta, K. A. Miller, M. Molina, D. Trivedi, J. Abed, M. A. Campos Mata, H. Al-Mahayni, J. Baltrusaitis, G. Shimizu, Y. A. Wu, A. Seifitokaldani, E. H. Sargent, P. M. Ajayan, J. Hu, M. G. Kibria, J. Am. Chem. Soc. 2023, 145, 8052.
- 32Y. Li, Q. Gu, B. Johannessen, Z. Zheng, C. Li, Y. Luo, Z. Zhang, Q. Zhang, H. Fan, W. Luo, B. Liu, S. Dou, H. Liu, Nano Energy 2021, 84, 105898.
- 33Y. Yu, Y. Wang, F. Yang, D. Feng, M. Yang, P. F. Xie, Y. Zhu, M. Shao, Y. Mei, J. C. Li, Angew. Chem., Int. Ed. 2024, 64, 202415691.
- 34X. Guo, Q. Zhang, H. He, A. Cai, S. Xi, J. Du, F. Zhang, X. Fan, W. Peng, Y. Li, Appl. Catal. B-Environ. 2023, 335, 122886.
- 35J. Li, G. Wang, X. Wang, Y. Zhao, Y. Zhao, W. Sui, D. Wang, C. Si, ACS Catal. 2024, 14, 16003.
- 36P. Wang, T. Hayashi, Q. a. Meng, Q. Wang, H. Liu, K. Hashimoto, L. Jiang, Small 2017, 13, 1601250.
- 37N. Solati, C. Karakaya, S. Kaya, ACS Catal. 2022, 13, 342.
- 38H. Meng, X. Liu, X. Chen, Y. Han, C. Zhou, Q. Jiang, T. Tan, R. Zhang, J. Energy Chem. 2022, 71, 528.
- 39I. S. Kwon, I. H. Kwak, J. Y. Kim, H. G. Abbas, T. T. Debela, J. Seo, M. K. Cho, J.-P. Ahn, J. Park, H. S. Kang, Nanoscale 2019, 11, 14266.
- 40W. Xu, R. Zeng, M. Rebarchik, A. Posada-Borbón, H. Li, C. J. Pollock, M. Mavrikakis, H. D. Abruña, J. Am. Chem. Soc. 2024, 146, 2593.
- 41J. Li, W. Huang, M. Wang, S. Xi, J. Meng, K. Zhao, J. Jin, W. Xu, Z. Wang, X. Liu, Q. Chen, L. Xu, X. Liao, Y. Jiang, K. A. Owusu, B. Jiang, C. Chen, D. Fan, L. Zhou, L. Mai, ACS Energy Lett. 2019, 4, 285.
- 42B. Mohanty, M. Ghorbani-Asl, S. Kretschmer, A. Ghosh, P. Guha, S. K. Panda, B. Jena, A. V. Krasheninnikov, B. K. Jena, ACS Catal. 2018, 8, 1683.
- 43J. Li, G. Li, J. Wang, C. Xue, X. Li, S. Wang, B. Han, M. Yang, L. Li, Inorg. Chem. Front. 2020, 7, 191.
- 44D. Zhang, Z. Wang, F. Liu, P. Yi, L. Peng, Y. Chen, L. Wei, H. Li, J. Am. Chem. Soc. 2024, 146, 3210.
- 45K. Liu, J. Fu, Y. Lin, T. Luo, G. Ni, H. Li, Z. Lin, M. Liu, Nat. Commun. 2022, 13, 2075.
- 46J. Li, W. Xia, J. Tang, Y. Gao, C. Jiang, Y. Jia, T. Chen, Z. Hou, R. Qi, D. Jiang, T. Asahi, X. Xu, T. Wang, J. He, Y. Yamauchi, J. Am. Chem. Soc. 2022, 144, 9280.
- 47L. Peng, J. Yang, Y. Yang, F. Qian, Q. Wang, D. Sun-Waterhouse, L. Shang, T. Zhang, G. I. N. Waterhouse, Adv. Mater. 2022, 34, 2202544.
- 48L. Zhang, N. Jin, Y. Yang, X.-Y. Miao, H. Wang, J. Luo, L. Han, Nano-Micro Lett. 2023, 15, 228.
- 49L. Luo, Y. Xu, D. Wang, X. Qiu, Chem. Eng. J. 2023, 273, 118654.
- 50Y. Wang, B. Yu, K. Liu, X. Yang, M. Liu, T.-S. Chan, X. Qiu, J. Li, W. Li, J. Mater. Chem. A 2020, 8, 2131.
- 51H. Jiang, J. Gu, X. Zheng, M. Liu, X. Qiu, L. Wang, W. Li, Z. Chen, X. Ji, J. Li, Energy Environ. Sci. 2019, 12, 322.
- 52S. Chen, L. Zhang, Z. Liu, Y. Chen, S. Li, Y. Zhang, J. Chen, J. Yan, Adv. Sci. 2024, https://doi.org/10.1002/advs.202413796.
- 53Y. Shen, H. Mao, C. Li, K. Li, Y. Liu, J. Liao, S. Zhang, Y. Fang, X. Cai, Adv. Fiber Mater. 2024, 6, 1470.
