Advanced Design of Metal Nanoclusters and Single Atoms Embedded in C1N1‐Derived Carbon Materials for ORR, HER, and OER

Advanced Functional MaterialsVolume 33, Issue 21 2300405 Research Article Advanced Design of Metal Nanoclusters and Single Atoms Embedded in C1N1-Derived Carbon Materials for ORR, HER, and OER Javier Quílez-Bermejo, Corresponding Author Javier Quílez-Bermejo [email protected] orcid.org/0000-0003-2808-1036 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, France Departamento de Química Inorgánica and Instituto de Materiales, Universidad de Alicante, Ap. 99, 03080 Alicante, Spain E-mail: [email protected]; [email protected]Search for more papers by this authorSergio García-Dalí, Sergio García-Dalí orcid.org/0000-0002-0042-0430 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, France Departamento de Ciencia de los Materiales e Ingenieria Metalúrgica, Universidad de Oviedo, 33004 Oviedo, SpainSearch for more papers by this authorAyoub Daouli, Ayoub Daouli orcid.org/0000-0002-4402-5467 Laboratoire de Physique et Chimie Théoriques (LPCT), Université de Lorraine, UMR 7019 CNRS, F-54000 Nancy, FranceSearch for more papers by this authorAndrea Zitolo, Andrea Zitolo orcid.org/0000-0002-2187-6699 Synchrotron SOLEIL, L'orme des Merisiers, BP 48 Saint Aubin, 91192 Gif-sur-Yvette, FranceSearch for more papers by this authorRafael L.S. Canevesi, Rafael L.S. Canevesi orcid.org/0000-0001-9076-1265 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, FranceSearch for more papers by this authorMélanie Emo, Mélanie Emo orcid.org/0000-0003-3599-6824 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), 54011 Nancy, FranceSearch for more papers by this authorMaría T. Izquierdo, María T. Izquierdo orcid.org/0000-0002-2408-2528 Instituto de Carboquímica (ICB-CSIC), Miguel Luesma Castán 4, E-50018 Zaragoza, SpainSearch for more papers by this authorMichael Badawi, Michael Badawi orcid.org/0000-0002-3504-4180 Laboratoire de Physique et Chimie Théoriques (LPCT), Université de Lorraine, UMR 7019 CNRS, F-54000 Nancy, FranceSearch for more papers by this authorAlain Celzard, Alain Celzard orcid.org/0000-0003-0073-9545 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, France Institut Universitaire de France (IUF), F-88000 Épinal, FranceSearch for more papers by this authorVanessa Fierro, Corresponding Author Vanessa Fierro [email protected] orcid.org/0000-0001-7081-3697 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, France E-mail: [email protected]; [email protected]Search for more papers by this author Javier Quílez-Bermejo, Corresponding Author Javier Quílez-Bermejo [email protected] orcid.org/0000-0003-2808-1036 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, France Departamento de Química Inorgánica and Instituto de Materiales, Universidad de Alicante, Ap. 99, 03080 Alicante, Spain E-mail: [email protected]; [email protected]Search for more papers by this authorSergio García-Dalí, Sergio García-Dalí orcid.org/0000-0002-0042-0430 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, France Departamento de Ciencia de los Materiales e Ingenieria Metalúrgica, Universidad de Oviedo, 33004 Oviedo, SpainSearch for more papers by this authorAyoub Daouli, Ayoub Daouli orcid.org/0000-0002-4402-5467 Laboratoire de Physique et Chimie Théoriques (LPCT), Université de Lorraine, UMR 7019 CNRS, F-54000 Nancy, FranceSearch for more papers by this authorAndrea Zitolo, Andrea Zitolo orcid.org/0000-0002-2187-6699 Synchrotron SOLEIL, L'orme des Merisiers, BP 48 Saint Aubin, 91192 Gif-sur-Yvette, FranceSearch for more papers by this authorRafael L.S. Canevesi, Rafael L.S. Canevesi orcid.org/0000-0001-9076-1265 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, FranceSearch for more papers by this authorMélanie Emo, Mélanie Emo orcid.org/0000-0003-3599-6824 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), 54011 Nancy, FranceSearch for more papers by this authorMaría T. Izquierdo, María T. Izquierdo orcid.org/0000-0002-2408-2528 Instituto de Carboquímica (ICB-CSIC), Miguel Luesma Castán 4, E-50018 Zaragoza, SpainSearch for more papers by this authorMichael Badawi, Michael Badawi orcid.org/0000-0002-3504-4180 Laboratoire de Physique et Chimie Théoriques (LPCT), Université de Lorraine, UMR 7019 CNRS, F-54000 Nancy, FranceSearch for more papers by this authorAlain Celzard, Alain Celzard orcid.org/0000-0003-0073-9545 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, France Institut Universitaire de France (IUF), F-88000 Épinal, FranceSearch for more papers by this authorVanessa Fierro, Corresponding Author Vanessa Fierro [email protected] orcid.org/0000-0001-7081-3697 Université de Lorraine, Centre National de la Recherche Scientifique (CNRS), Institut Jean Lamour (IJL), F-88000 Épinal, France E-mail: [email protected]; [email protected]Search for more papers by this author First published: 20 February 2023 https://doi.org/10.1002/adfm.202300405Citations: 3Read the full textAboutPDF ToolsRequest permissionExport citationAdd to favoritesTrack citation ShareShare Give accessShare full text accessShare full-text accessPlease review our Terms and Conditions of Use and check box below to share full-text version of article.I have read and accept the Wiley Online Library Terms and Conditions of UseShareable LinkUse the link below to share a full-text version of this article with your friends and colleagues. Learn more.Copy URL Share a linkShare onEmailFacebookTwitterLinkedInRedditWechat Abstract Single atoms and nanoclusters of Fe, Ni, Co, Cu, and Mn are systematically designed and embedded in a well-defined C1N1-type material that has internal cavities of ≈0.6 nm based on four N atoms. These N atoms serve as perfect anchoring points for the nucleation of small nanoclusters of different metal natures through the creation of metal-nitrogen (TM-N4) bonds. After pyrolysis at 800 °C, TM@CNx-type structures are obtained, where TM is the transition metal and x < 1. Fe@CNx and Co@CNx are the most promising for oxygen reduction reaction and hydrogen evolution reaction, respectively, with a Pt-like performance, and Ni@CNx is the most active for oxygen evolution reaction (OER) with an EOER of 1.59 V versus RHE, far outperforming the commercial IrO2 (EOER = 1.72 V). This systematic and benchmarking study can serve as a basis for the future design of advanced multi-functional electrocatalysts by modulating and combining the metallic nature of nanoclusters and single atoms. 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 Filename Description adfm202300405-sup-0001-SuppMat.pdf3.3 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 1V. Masson-Delmotte, P. Zhai, H. O. P€ortner, D. Roberts, J. Skea, P. R. Shukla, A. Pirani, W. Moufouma-Okia, C. Péan, R. Pidcock, S. Connors, J. B. R. Matthews, Y. Chen, X. Zhou, M. I. Gomis, E. Lonnoy, T. Maycock, M. Tignor, T. Waterfield, Summary for Policymakers, IPCC, Cambridge University Press, Cambridge, UK and New York, NY, USA, 2018. 2 Paris Agreement to the United Nations Framework Convention on Climate Change, 2015, T.I.A.S., 16. 3J. Quílez-Bermejo, E. Morallón, D. Cazorla-Amorós, Carbon 2020, 165, 434. 4X. Li, L. Zhao, J. Yu, X. Liu, X. Zhang, H. Liu, W. Zhou, Nano-Micro Lett. 2020, 12, 131. 5M. Winter, R. J. Brodd, Chem. Rev. 2004, 104, 4245. 6Y. Sahai, J. Ma, Fundamentals of Electrochemical Energy Devices, World Scientific Publishing Co Pte Ltd, Singapore, 2021. 7L. Li, P. Wang, Q. Shao, X. Huang, Adv. Mater. 2021, 33, 2004243. 8J. Zhu, L. Hu, P. Zhao, L. Y. S. Lee, K.-Y. Wong, Chem. Rev. 2020, 120, 851. 9A. Morozan, B. Jousselme, S. Palacín, Energy Environ. Sci. 2011, 4, 1238. 10J. Wang, J. Kim, S. Choi, H. Wang, J. Lim, Small Methods 2020, 4, 2000621. 11Y. Wang, D. Wang, Y. Li, Adv. Mater. 2021, 33, 2008151. 12J. Cai, R. Javed, D. Ye, H. Zhao, J. Zhang, J. Mater. Chem. A 2020, 8, 22467. 13T. Sun, S. Mitchel, J. Li, P. Lyu, X. Wu, J. Pérez-Ramírez, J. Lu, Adv. Mater. 2021, 33, 2003075. 14C. Zhu, S. Fu, Q. Shi, D. Du, Y. Lin, Angew. Chem., Int. Ed. 2017, 56, 13944. 15B. W. Zhang, Y. X. Wang, S. L. Chou, H. K. Liu, S. X. Dou, Small Methods 2019, 3, 1800497. 16T. Sharifi, E. Gracia-Espino, A. Chen, G. Hu, T. Wagberg, Adv. Energy Mater. 2020, 10, 1902084. 17J. Kossmann, T. Heil, M. Antonietti, N. López-Salas, ChemSusChem 2020, 13, 6643. 18J. Kossmann, D. Piankova, N. V. Tarakina, J. Heske, T. D. Kühne, J. Schmidt, M. Antonietti, N. López-Salas, Carbon 2021, 172, 497. 19N. López-Salas, J. Kossmann, M. Antonietti, Acc. Mater. Res. 2020, 1, 117. 20H. Wang, W. Wang, Y. Y. Xu, S. Dong, J. Xiao, F. Wang, H. Liu, B. Y. Xia, ACS Appl. Mater. Interfaces 2017, 9, 10610. 21Y. Wang, Q. Li, L.-C. Zhang, Y. Wu, H. Chen, T. Li, M. Xu, S.-J. Bao, J. Mater. Chem. A 2021, 9, 7137. 22K. Hu, L. Tao, D. Liu, J. Huo, S. Wang, ACS Appl. Mater. Interfaces 2016, 8, 19379. 23J. Quílez-Bermejo, M. Melle-Franco, E. San-Fabián, E. Morallón, D. Cazorla-Amorós, J. Mater. Chem. A 2019, 7, 24239. 24J. Li, P. Prslja, T. Shinagawa, A. J. Fernández, F. Krumeich, K. Artyushkova, P. Atanassov, A. Zitolo, Y. Zhou, R. García-Muelas, N. Lopez, J. Pérez-Ramírez, F. Jaouen, ACS Catal. 2019, 9, 10426. 25D. Karapinar, N. T. Huan, N. R. Sahraie, J. Li, D. Wakerley, N. Touati, S. Zanna, D. Taverna, L. H. G. Tizei, A. Zitolo, F. Jaouen, V. Mougel, M. Fontecave, Angew. Chem., Int. Ed. 2019, 58, 15098. 26H. Dierkes, R. Dronskowski, J. Inorg. Gen. Chem. 2014, 640, 3148. 27X. Wan, W. Chen, J. Yang, M. Liu, X. Liu, J. Shui, ChemElectroChem 2019, 6, 304. 28A. Dessalle, J. Quílez-Bermejo, V. Fierro, F. Xu, A. Celzard, Carbon 2023, 203, 237. 29Y. Wang, L. Wang, Y. Xie, M. Tong, C. Tian, H. Fu, ACS Sustainable Chem. Eng. 2022, 10, 3346. 30Y. Qin, Z. Ou, C. Xu, Q. Lan, R. Jin, X. Xu, C. Guo, H. Li, Y. Si, Chem. Eng. J. 2022, 440, 135850. 31J. Quílez-Bermejo, E. Morallón, C. Amorós, Chem. Commun. 2018, 54, 4441. 32J. Quílez-Bermejo, S. Pérez-Rodríguez, R. L. S. Canevesi, D. Torres, E. Morallón, D. Cazorla-Amorós, A. Celzard, V. Fierro, Carbon 2022, 196, 708. 33J. Li, M. T. Sougrati, A. Zitolo, J. M. Ablett, I. C. Oguz, T. Mineva, I. Matanovic, P. Atanassov, Y. Huang, I. Zenyuk, A. Di Cicco, K. Kumar, L. Dubau, F. Maillard, G. Drazic, F. Jaouen, Nat. Catal. 2021, 4, 10. 34Y. Yang, K. Mao, S. Gao, H. Huang, G. Xia, Z. Lin, P. Jian, C. Wang, H. Wang, Q. Chen, Adv. Mater. 2018, 30, 1801732. 35H. Shang, W. Sun, R. Sui, J. Pei, L. Zheng, J. Dong, Z. Jiang, D. Zhou, Z. Zhuang, W. Chen, J. Zhang, D. Wang, Y. Li, Nano Lett. 2020, 20, 5443. 36Z.-Y. Wu, X.-X. Xu, B.-C. Hu, H.-W. Liang, Y. Lin, L.-F. Chen, S.-H. Yu, Angew. Chem., Int. Ed. 2015, 54, 8179. 37Q. Li, W. Chen, H. Xiao, Y. Gong, Z. Li, L. Zheng, Z. Zheng, W. Yang, 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. 38Y. Guo, F. Liu, L. Feng, X. Wang, X. Zhang, J. Liang, Chem. Eng. J. 2022, 429, 132150. 39Y. Wang, L. Chen, Z. Mao, L. Peng, R. Xiang, X. Tang, J. Deng, Z. Wei, Q. Liao, Sci. Bull. 2019, 64, 1095. 40C. Shi, Y. Liu, R. Qi, J. Li, J. Zhu, R. Yu, S. Li, X. Hong, J. Wu, S. Xi, L. Zhou, L. Mai, Nano Energy 2021, 87, 106153. 41X. Song, N. Li, H. Zhang, L. Wang, Y. Yan, H. Wang, L. Wang, Z. Bian, ACS Appl. Mater. Interfaces 2020, 12, 17519. 42J. Chen, H. Li, C. Fan, Q. Meng, Y. Tang, X. Qiu, G. Fu, T. Ma, Adv. Mater. 2020, 32, 2003134. 43W. Wu, Y. Liu, D. Liu, W. Chen, Z. Song, X. Wang, Y. Zheng, N. Lu, C. Wang, J. Mao, Y. Li, Nano Res. 2021, 14, 998. 44L. Bai, C. Hou, X. Wen, J. Guan, ACS Appl. Energy Mater. 2019, 2, 4755. 45J. Quílez-Bermejo, K. Strutynski, M. Melle-Franco, E. Morallón, D. Cazorla-Amorós, ACS Appl. Mater. Interfaces 2020, 12, 54815. 46Z. W. She, J. Kibsgaard, C. F. Dickens, I. Chorkendorff, J. K. Norskov, T. F. Jaramillo, Science 2017, 355, 6321. 47J. K. Norskov, J. Rossmeisl, A. Logadottir, L. Lindqvist, J. R. Kitchin, T. Bligaard, H. Jonsson, J. Phys. Chem. B 2004, 108, 17886. 48X. Chen, R. Hu, Int. J. Hydrogen Energy 2019, 44, 15409. 49Y. J. Sa, S. O. Park, G. Y. Jung, T. J. Shin, H. Y. Jeong, S. K. Kwak, S. H. Joo, ACS Catal. 2019, 9, 83. 50J. Yu, J. Li, C. Y. Xu, J. Liu, R. Chen, J. Zhu, R. Li, J. Wang, Carbon 2021, 185, 96. 51L. Cao, Q. Luo, W. Liu, Y. Lin, X. Liu, Y. Cao, W. Zhang, Y. Wu, J. Yang, T. Yao, S. Wei, Nat. Catal. 2019, 2, 134. 52C. Lei, Y. Wang, Y. Hou, P. Liu, J. Yang, T. Zhang, X. Zhuang, M. Chen, B. Yang, L. Lei, C. Yuan, M. Qiu, X. Feng, Energy Environ. Sci. 2019, 12, 149. 53S. Li, Q. Zhou, G. Yu, Z. Lei, Z. Liu, Q. Xu, W. Xu, R. Wu, Appl. Surf. Sci. 2020, 518, 146239. 54J. Jiang, L. Zhu, Y. Sun, Y. Chen, H. Chen, S. Han, H. Lin, J. Power Sources 2019, 426, 74. 55S. Chao, Q. Xia, G. Wang, X. Zhang, Int. J. Hydrogen Energy 2019, 44, 4707. 56J. Li, Y. Wang, T. Shou, H. Zhang, X. Sun, J. Tang, L. Zhang, A. M. Al-Enizi, Z. Yang, G. Zheng, J. Am. Chem. Soc. 2015, 137, 14305. 57M. A. Ahsan, A. R. P. Santiago, Y. Hong, N. Zhang, M. Cano, E. Rodriguez-Castellón, L. Echegoyen, S. T. Sreenivasan, J. C. Noveron, J. Am. Chem. Soc. 2020, 142, 14688. 58S. Cui, M. Qian, X. Liu, Z. Sun, P. Du, ChemSusChem 2016, 9, 2365. 59H. Zhang, Y. Liu, T. Chen, J. Zhang, J. Zhang, X. W. Lou, Adv. Mater. 2019, 31, 1904585. 60Y. Zheng, G. Zhang, P. Zhang, S. Chu, D. Wu, C. Sun, B. Qian, S. Chen, S. Tao, L. Song, Chem. Eng. J. 2022, 429, 132122. 61J. Xu, L. Shi, C. Liang, H. Wu, J. Lei, D. Liu, D. Qu, Z. Xie, J. Li, H. Tang, ChemElectroChem 2017, 4, 1148. 62Y. Pan, S. Liu, K. Sun, X. Chen, B. Wang, K. Wu, X. Cao, W. C. Cheong, R. Shen, A. Han, Z. Chen, L. Zheng, J. Luo, Y. Lin, Y. Liu, D. Wang, Q. Peng, Q. Zhang, C. Chen, Y. Li, Angew. Chem., Int. Ed. 2018, 57, 8641. 63S. Dilpazir, H. He, Z. Li, M. Wang, P. Lu, R. Liu, Z. Xie, D. Gao, G. Zhang, ACS Appl. Energy Mater. 2018, 1, 3283. 64Y. Gao, H. Zhao, D. Chen, C. Chen, F. Ciucci, Carbon 2015, 94, 1028. 65L. Yang, L. Shi, D. Wang, Y. Lv, D. Cao, Nano Energy 2018, 50, 691. 66Y. Li, Z.-S. Wu, P. Lu, X. Wang, W. Liu, Z. Liu, J. Ma, W. Ren, Z. Jiang, X. Bao, Adv. Sci. 2020, 7, 1903089. 67W. Zha, D. Liu, Z. Ma, Y. Wang, Y. Wei, X. Ma, L. Wang, Q. Zhang, B. Lou, R. Yuan, X. Fu, R. Sa, Appl. Surf. Sci. 2021, 564, 150331. 68A. Filipponi, A. Di Cicco, C. R. Natoli, Phys. Rev. B: Condens. Matter Mater. Phys. 1995, 52, 15135. 69A. Filipponi, A. Di Cicco, C. R. Natoli, Phys. Rev. B: Condens. Matter Mater. Phys. 1995, 52, 15122. 70L. Bouleau, S. Pérez-Rodríguez, J. Quílez-Bermejo, M. T. Izquierdo, F. Xu, V. Fierro, A. Celzard, Carbon 2022, 189, 349. 71L. J. Sham, W. Kohn, Phys. Rev. 1966, 145, 561. 72P. Hohenberg, W. Kohn, Phys. Rev. 1964, 136, B864. 73G. Kresse, J. Hafner, Phys. Rev. B 1993, 47, 558. 74G. Kresse, J. Furthmüller, Comput. Mater. Sci. 1996, 6, 15. 75J. P. Perdew, K. Burke, M. Ernzerhof, Phys. Rev. Lett. 1996, 77, 3865. 76W. Kohn, L. J. Sham, Phys. Rev. 1965, 140, A1133. 77S. Grimme, S. Ehrlich, L. Goerigk, J. Comput. Chem. 2011, 32, 1456. 78S. Grimme, J. Antony, S. Ehrlich, H. Krieg, J. Chem. Phys. 2010, 132, 154104. 79L. Wang, T. Maxisch, G. Ceder, Phys. Rev. B 2006, 73, 195107. Citing Literature Volume33, Issue21May 17, 20232300405 ReferencesRelatedInformation