Turn the Harm into A Benefit: Axial Cl Adsorption on Curved Fe-N4 Single Sites for Boosted Oxygen Reduction Reaction in Seawater
Lei Wang
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorMengting Huang
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorJinyan Zhang
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorYun Han
School of Engineering and Built Environment, Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Queensland, 4111 Australia
Search for more papers by this authorXuan Liu
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorYing Chen
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorHelong Wu
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorXiaodong Qian
Beijing Key Laboratory of Metro Fire and Passenger Transportation Safety, China Academy of Safety Science and Technology, Beijing, 100012 China
Search for more papers by this authorAijun Du
School of Chemistry and Physics and Centre for Materials Science Queensland University of Technology, Gardens Point Campus, Brisbane, 4001 Australia
Search for more papers by this authorCorresponding Author
Xin Wang
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
E-mail: [email protected]
Search for more papers by this authorLei Wang
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorMengting Huang
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorJinyan Zhang
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorYun Han
School of Engineering and Built Environment, Queensland Micro- and Nanotechnology Centre, Griffith University, Nathan Campus, Queensland, 4111 Australia
Search for more papers by this authorXuan Liu
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorYing Chen
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorHelong Wu
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
Search for more papers by this authorXiaodong Qian
Beijing Key Laboratory of Metro Fire and Passenger Transportation Safety, China Academy of Safety Science and Technology, Beijing, 100012 China
Search for more papers by this authorAijun Du
School of Chemistry and Physics and Centre for Materials Science Queensland University of Technology, Gardens Point Campus, Brisbane, 4001 Australia
Search for more papers by this authorCorresponding Author
Xin Wang
College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310032 P. R. China
E-mail: [email protected]
Search for more papers by this authorAbstract
Seawater electrocatalysis is urgently needed for various energy storage and conversion systems. However, the adsorption of chloride ions (Cl−) to the active sites can degrade the oxygen reduction reaction (ORR) activity and stability, thus reducing the catalytic performance. In this paper, a curved FeN4 single atomic structure is designed by utilizing curvature engineering, which can turns the harmful Cl adsorption into a benefit on the Fe single site that changes the rate determining step of ORR and reduces the overall energy barrier according to density functional theory (DFT) calculation. Experimental studies reveal the prepared highly-curved single-atom iron catalyst (HC-FeSA) exhibits excellent ORR activity in different electrolytes, with half-wave potentials of 0.90 V in 0.1 M KOH, 0.90 V in simulated seawater, and 0.75 V in natural seawater, respectively. This work opens up an avenue for the synthesis of high-performance seawater-based single-atom ORR catalysts through regulating the local atomic curvature.
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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References
- 1B. Peng, Z. Liu, L. Sementa, Q. Jia, Q. Sun, C. U. Segre, E. Liu, M. Xu, Y.-H. Tsai, X. Yan, Z. Zhao, J. Huang, X. Pan, X. Duan, A. Fortunelli, Y. Huang, Nat. Catal. 2024, 7, 818.
- 2K. Jiao, J. Xuan, Q. Du, Z. Bao, B. Xie, B. Wang, Y. Zhao, L. Fan, H. Wang, Z. Hou, S. Huo, N. P. Brandon, Y. Yin, M. D. Guiver, Nature 2021, 595, 361.
- 3X. Zou, M. Tang, Q. Lu, Y. Wang, Z. Shao, L. An, Energy Environ. Sci. 2023, 17, 386.
- 4P. Cui, L. Zhao, Y. Long, L. Dai, C. Hu, Angew.Chem.,Int. Ed. 2023, 135, 202218269.
- 5X. Wang, Y. Jia, X. Mao, L. Zhang, D. Liu, L. Song, X. Yan, J. Chen, D. Yang, J. Zhou, K. Wang, A. Du, X. Yao, Chem 2020, 6, 2009.
- 6P. Liu, Y. Liu, K. Wang, S. Shi, M. Jin, J. Liu, T. Qin, Q. Liu, X. Liu, J. He, Nano Res. 2024, 17, 7957.
- 7T. Wang, S. Gao, T. Wei, Y. Qin, S. Zhang, J. Ding, Q. Liu, J. Luo, X. Liu, Chem. - Eur. J. 2023, 29, 202204034.
- 8X. Wang, Y. Jia, X. Mao, D. Liu, W. He, J. Li, J. Liu, X. Yan, J. Chen, L. Song, A. Du, X. Yao, Adv. Mater. 2020, 32, 2000966.
- 9X. Wang, C. Han, Y. Han, R. Huang, H. Sun, P. Guo, X. Liu, M. Huang, Y. Chen, H. Wu, J. Zhang, X. Yan, Z. Mao, A. Du, Y. Jia, L. Wang, Small 2024, 20, 2401447.
- 10X. Wang, H. Sun, T. He, P. Guo, R. Huang, Z. Mao, C. Han, X. Liu, M. Huang, L. Wang, Chem Catalysis 2024, 4, 101007.
- 11Z. Huang, M. Li, X. Yang, T. Zhang, X. Wang, W. Song, J. Zhang, H. Wang, Y. Chen, J. Ding, W. Hu, J. Am. Chem. Soc. 2024, 146, 24842.
- 12T. Wang, Q. Zhang, K. Lian, G. Qi, Q. Liu, L. Feng, G. Hu, J. Luo, X. Liu, J. Colloid Interface Sci. 2024, 655, 176.
- 13Z. Jin, P. Li, Y. Meng, Z. Fang, D. Xiao, G. Yu, Nat. Catal. 2021, 4, 615.
- 14C.-L. Yang, L.-N. Wang, P. Yin, J. Liu, M.-X. Chen, Q.-Q. Yan, Z.-S. Wang, S.-L. Xu, S.-Q. Chu, C. Cui, H. Ju, J. Zhu, Y. Lin, J. Shui, H.-W. Liang, Science 2021, 374, 459.
- 15X. Wang, N. Zhang, S. Guo, H. Shang, X. Luo, Z. Sun, Z. Wei, Y. Lei, L. Zhang, D. Wang, Y. Zhao, F. Zhang, L. Zhang, X. Xiang, W. Chen, B. Zhang, J. Am. Chem. Soc. 2024, 146, 21357.
- 16H. Hu, X. Wang, J. P. Attfield, M. Yang, Chem. Soc. Rev. 2024, 53, 163.
- 17J. N. Hausmann, L. R. Winter, M. A. Khan, M. Elimelech, M. G. Kibria, T. Sontheimer, P. W. Menezes, Joule 2024, 8, 2436.
- 18H. Jin, J. Xu, H. Liu, H. Shen, H. Yu, M. Jaroniec, Y. Zheng, S.-Z. Qiao, Sci. Adv. 2023, 9, eadi7755.
- 19H. Xie, Z. Zhao, T. Liu, Y. Wu, C. Lan, W. Jiang, L. Zhu, Y. Wang, D. Yang, Z. Shao, Nature 2022, 612, 673.
- 20J. Yu, B.-Q. Li, C.-X. Zhao, Q. Zhang, Energy Environ. Sci. 2020, 13, 3253.
- 21Q. Tang, L. Bai, C. Zhang, R. Meng, L. Wang, C. Geng, Y. Guo, F. Wang, Y. Liu, G. Song, G. Ling, H. Sun, Z. Weng, Q.-H. Yang, Sci. Bull. 2023, 68, 3172.
- 22J. Lu, Q. Lu, Y. Guo, X. Chen, Z. Yin, Y. Cao, Y. Guo, J. Zhang, H. Wang, Y. Wang, X. Zheng, K. I. Ozoemena, Y. Deng, Energy Storage Mater. 2024, 65, 103093.
- 23W. Zhou, B. Li, X. Liu, J. Jiang, S. Bo, C. Yang, Q. An, Y. Zhang, M. A. Soldatov, H. Wang, S. Wei, Q. Liu, Nat. Commun. 2024, 15, 6650.
- 24H. Niu, L. Huang, Y. Qin, R. Qi, B. Mei, D. Wu, F.-M. Li, B. You, Q. Li, Y. Yao, Z. Wang, T. Yao, S. Ding, W. Guo, Y. Chen, Y. Su, F. Song, B. Y. Xia, J. Am. Chem. Soc. 2024, 146, 22650.
- 25Y. Luo, K. Li, Y. Chen, J. Feng, L. Wang, Y. Jiang, L. Li, G. Yu, J. Feng, Adv. Mater. 2023, 35, 2300624.
- 26Y. Dong, Y. Wang, Z. Tian, K. Jiang, Y. Li, Y. Lin, C. W. Oloman, E. L. Gyenge, J. Su, L. Chen, The Innovation 2021, 2, 100161.
- 27S. Wu, X. Liu, H. Mao, J. Zhu, G. Zhou, J. Chi, Z. Wu, L. Wang, Adv. Energy Mater. 2024, 14, 2400183.
- 28S. Kim, S. Ji, H. Yang, H. Son, H. Choi, J. Kang, O. L. Li, Appl. Catal. B 2022, 310, 121361.
- 29D. H. Suh, S. K. Park, P. Nakhanivej, Y. Kim, S. M. Hwang, H. S. Park, J. Power Sources 2017, 372, 31.
- 30S. K. Kaiser, Z. Chen, D. Faust Akl, S. Mitchell, J. Pérez-Ramírez, Chem. Rev. 2020, 120, 11703.
- 31L. Yan, P. Li, Q. Zhu, A. Kumar, K. Sun, S. Tian, X. Sun, Chem 2023, 9, 280.
- 32S. Yin, L. Chen, J. Yang, X. Cheng, H. Zeng, Y. Hong, H. Huang, X. Kuai, Y. Lin, R. Huang, Y. Jiang, S. Sun, Nat. Commun. 2024, 15, 7489.
- 33M. Tong, F. Sun, G. Xing, C. Tian, L. Wang, H. Fu, Angew. Chem., Int. Ed. 2023, 62, 202314933.
- 34W. Zheng, R. Zhu, H. Wu, T. Ma, H. Zhou, M. Zhou, C. He, X. Liu, S. Li, C. Cheng, Angew. Chem., Int. Ed. 2022, 61, 202208667.
- 35X. Li, L. Liu, X. Ren, J. Gao, Y. Huang, B. Liu, Sci. Adv. 2020, 6, eabb6833.
- 36T. Sun, S. Mitchell, J. Li, P. Lyu, X. Wu, J. Pérez-Ramírez, J. Lu, Adv. Mater. 2020, 33, 2003075.
- 37H. Wang, T. Yang, J. Wang, Z. Zhou, Z. Pei, S. Zhao, Chem 2024, 10, 48.
- 38Y. Zhu, Y. Jiang, H. Li, D. Zhang, L. Tao, X.-Z. Fu, M. Liu, S. Wang, Angew. Chem.,Int. Ed. 2024, 63, 202319370.
- 39B. Wang, M. Wang, Z. Fan, C. Ma, S. Xi, L. Y. Chang, M. Zhang, N. Ling, Z. Mi, S. Chen, W. R. Leow, J. Zhang, D. Wang, Y. Lum, Nat. Commun. 2024, 15, 1719.
- 40J. Su, C. B. Musgrave, Y. Song, L. Huang, Y. Liu, G. Li, Y. Xin, P. Xiong, M. M.-J. Li, H. Wu, M. Zhu, H. M. Chen, J. Zhang, H. Shen, B. Z. Tang, M. Robert, W. A. Goddard, R. Ye, Nat. Catal. 2023, 6, 818.
- 41G. Chen, R. Lu, C. Li, J. Yu, X. Li, L. Ni, Q. Zhang, G. Zhu, S. Liu, J. Zhang, U. I. Kramm, Y. Zhao, G. Wu, J. Xie, X. Feng, Adv. Mater. 2023, 35, 2300907.
- 42Y. Wu, J. Yang, Z. Wang, C.-X. Huang, Y. Zhang, Q. Zhang, C. Chen, J. Du, X. Zhou, Y. Zhang, H. Zhou, L. Wang, X. Zheng, L. Gu, L.-M. Yang, Angew.Chem.,Int. Ed. 2021, 60, 22722.
- 43H.-S. Qian, S.-H. Yu, J.-Y. Gong, L.-B. Luo, L.-f. Fei, Langmuir 2006, 22, 3830.
- 44X. Wang, M.-Q. Zhang, R. Kou, L.-L. Lu, Y. Zhao, X.-W. Xu, G.-M. Liu, Y.-M. Zheng, S.-H. Yu, Adv. Funct. Mater. 2016, 26, 5086.
- 45L. Wang, Z. Zeng, W. Gao, T. Maxson, D. Raciti, M. Giroux, X. Pan, C. Wang, J. Greeley, Science 2019, 363, 870.
- 46Y. Wang, X. Li, M. Zhang, Y. Zhou, D. Rao, C. Zhong, J. Zhang, X. Han, W. Hu, Y. Zhang, K. Zaghib, Y. Wang, Y. Deng, Adv. Mater. 2020, 32, 2000231.
- 47Y. Yao, S. Hu, W. Chen, Z.-Q. Huang, W. Wei, T. Yao, R. Liu, K. Zang, X. Wang, G. Wu, W. Yuan, T. Yuan, B. Zhu, W. Liu, Z. Li, D. He, Z. Xue, Y. Wang, X. Zheng, J. Dong, C.-R. Chang, Y. Chen, X. Hong, J. Luo, S. Wei, W.-X. Li, P. Strasser, Y. Wu, Y. Li, Nat. Catal. 2019, 2, 304.
- 48Z.-Y. Wu, P. Zhu, D. A. Cullen, Y. Hu, Q.-Q. Yan, S.-C. Shen, F.-Y. Chen, H. Yu, M. Shakouri, J. D. Arregui-Mena, A. Ziabari, A. R. Paterson, H.-W. Liang, H. Wang, Nat. Synth. 2022, 1, 658.
- 49J. Wang, Y. Yao, C. Zhang, Q. Sun, D. Cheng, X. Huang, J. Feng, J. Wan, J. Zou, C. Liu, C. Yu, Adv. Sci. 2021, 8, 2100120.
- 50J. Chen, Y. Cheng, Q. Zhang, C. Luo, H.-Y. Li, Y. Wu, H. Zhang, X. Wang, H. Liu, X. He, J. Han, D.-L. Peng, M. Liu, M.-S. Wang, Adv. Funct. Mater. 2021, 31, 2007158.
- 51K. Yuan, S. Sfaelou, M. Qiu, D. Lützenkirchen-Hecht, X. Zhuang, Y. Chen, C. Yuan, X. Feng, U. Scherf, ACS Energy Lett. 2018, 3, 252.
- 52M. Zhao, H. Liu, H. Zhang, W. Chen, H. Sun, Z. Wang, B. Zhang, L. Song, Y. Yang, C. Ma, Y. Han, W. Huang, Energy Environ. Sci. 2021, 14, 6455.
- 53S. Ibraheem, S. Chen, J. Li, Q. Wang, Z. Wei, J. Mater. Chem. A 2019, 7, 9497.
- 54H. Yang, W. Wang, X. Wu, M. S. Siddique, Z. Su, M. Liu, W. Yu, Appl. Catal., B 2022, 301, 120790.
- 55M. Mooste, E. Kibena-Põldsepp, V. Vassiljeva, A. Kikas, M. Käärik, J. Kozlova, V. Kisand, M. Külaviir, S. Cavaliere, J. Leis, A. Krumme, V. Sammelselg, S. Holdcroft, K. Tammeveski, ChemCatChem 2020, 12, 4568.
- 56R. Sibul, E. Kibena-Põldsepp, S. Ratso, M. Kook, M. T. Sougrati, M. Käärik, M. Merisalu, J. Aruväli, P. Paiste, A. Treshchalov, J. Leis, V. Kisand, V. Sammelselg, S. Holdcroft, F. Jaouen, K. Tammeveski, ChemElectroChem 2020, 7, 1739.
- 57J. Tian, Y. Zhu, X. Yao, L. Yang, C. Du, Z. Lv, M. Hou, S. Zhang, X. Ma, C. Cao, J. Mater. Chem. A 2023, 11, 5288.
- 58Q. Li, W. Chen, H. Xiao, Y. Gong, Z. Li, L. Zheng, X. Zheng, W. Yan, W.-C. Cheong, R. Shen, N. Fu, L. Gu, Z. Zhuang, C. Chen, D. Wang, Q. Peng, J. Li, Y. Li, Adv. Mater. 2018, 30, 1800588.
- 59J. Sun, H. Xue, L. Lu, M. Gao, N. Guo, T. Song, H. Dong, J. Zhang, L. Wu, Q. Wang, Appl. Catal. B 2022, 313, 121429.
- 60J. Barrio, A. Pedersen, S. C. Sarma, A. Bagger, M. Gong, S. Favero, C.-X. Zhao, R. Garcia-Serres, A. Y. Li, Q. Zhang, F. Jaouen, F. Maillard, A. Kucernak, I. E. L. Stephens, M.-M. Titirici, Adv. Mater. 2023, 35, 2211022.
- 61A. Mehmood, M. Gong, F. Jaouen, A. Roy, A. Zitolo, A. Khan, M.-T. Sougrati, M. Primbs, A. M. Bonastre, D. Fongalland, G. Drazic, P. Strasser, A. Kucernak, Nat. Catal. 2022, 5, 311.
- 62N. Zhang, T. Zhou, M. Chen, H. Feng, R. Yuan, C. a. Zhong, W. Yan, Y. Tian, X. Wu, W. Chu, C. Wu, Y. Xie, Energy Environ. Sci. 2020, 13, 111.
- 63J. Li, M. T. Sougrati, A. Zitolo, J. M. Ablett, I. C. Oğuz, T. Mineva, I. Matanovic, P. Atanassov, Y. Huang, I. Zenyuk, A. Di Cicco, K. Kumar, L. Dubau, F. Maillard, G. Dražić, F. Jaouen, Nat. Catal. 2021, 4, 10.
- 64J. Han, H. Bao, J.-Q. Wang, L. Zheng, S. Sun, Z. L. Wang, C. Sun, Appl. Catal. B 2021, 280, 119411.
- 65X. Hai, S. Xi, S. Mitchell, K. Harrath, H. Xu, D. F. Akl, D. Kong, J. Li, Z. Li, T. Sun, H. Yang, Y. Cui, C. Su, X. Zhao, J. Li, J. Pérez-Ramírez, J. Lu, Nat. Nanotechnol. 2022, 17, 174.
- 66X. Wan, X. Liu, Y. Li, R. Yu, L. Zheng, W. Yan, H. Wang, M. Xu, J. Shui, Nat. Catal. 2019, 2, 259.
- 67C. Chen, M. Sun, F. Zhang, H. Li, M. Sun, P. Fang, T. Song, W. Chen, J. Dong, B. Rosen, P. Chen, B. Huang, Y. Li, Energy Environ. Sci. 2023, 16, 1685.
