Chromium Oxynitride Electrocatalysts for Electrochemical Synthesis of Ammonia Under Ambient Conditions
Yao Yao
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
Search for more papers by this authorQi Feng
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Search for more papers by this authorShangqian Zhu
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
Search for more papers by this authorJiadong Li
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
Search for more papers by this authorYuze Yao
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
Search for more papers by this authorYajun Wang
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Search for more papers by this authorQi Wang
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Search for more papers by this authorMeng Gu
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Search for more papers by this authorCorresponding Author
Haijiang Wang
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
E-mail: [email protected], [email protected], [email protected]Search for more papers by this authorCorresponding Author
Hui Li
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
E-mail: [email protected], [email protected], [email protected]Search for more papers by this authorXiao-Zi Yuan
National Research Council Canada, Vancouver, BC, V6T 1W5 Canada
Search for more papers by this authorCorresponding Author
Minhua Shao
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
E-mail: [email protected], [email protected], [email protected]Search for more papers by this authorYao Yao
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
Search for more papers by this authorQi Feng
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Search for more papers by this authorShangqian Zhu
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
Search for more papers by this authorJiadong Li
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
Search for more papers by this authorYuze Yao
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
Search for more papers by this authorYajun Wang
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Search for more papers by this authorQi Wang
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Search for more papers by this authorMeng Gu
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
Search for more papers by this authorCorresponding Author
Haijiang Wang
Department of Mechanical and Energy Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
E-mail: [email protected], [email protected], [email protected]Search for more papers by this authorCorresponding Author
Hui Li
Department of Materials Science and Engineering, Southern University of Science and Technology, 1088 Xueyuan Blvd, Nanshan District, Shenzhen, Guangdong, 518055 China
E-mail: [email protected], [email protected], [email protected]Search for more papers by this authorXiao-Zi Yuan
National Research Council Canada, Vancouver, BC, V6T 1W5 Canada
Search for more papers by this authorCorresponding Author
Minhua Shao
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong
E-mail: [email protected], [email protected], [email protected]Search for more papers by this authorAbstract
The electrochemical synthesis of ammonia via nitrogen reduction reaction (NRR) has received much attention as a more environmentally friendly and less energy consuming technology than the conventional Haber–Bosch process. The catalytic activities of all NRR electrocatalysts reported so far, however, are very low under ambient conditions. In this study, partially oxidized chromium nitride (chromium oxynitride) nanoparticles are synthesized and their NRR activities are evaluated in a proton exchange membrane electrolyzer under ambient conditions. The highest ammonia formation rate of 8.9 × 10−11 mol s−1 cm−2 and 15.56 µg h−1 mg−1cat are achieved at a cell voltage of 2.0 V. The highest Faradaic efficiency of 6.7% is achieved at a cell voltage of 1.8 V. The findings demonstrate that metal nitride–based materials can be promising electrocatalysts toward NRR and could guide rational design of more advanced catalysts for various reactions.
Conflict of Interest
The authors declare no conflict of interest.
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References
- 1T. Lipman, N. Shah, Ammonia as an Alternative Energy Storage Medium for Hydrogen Fuel Cells: Scientific and Technical Review for Near-Term Stationary Power Demonstration Projects, Final Report. UC Berkeley Transportation Sustainability Research Center 2007.
- 2Z. J. Schiffer, K. Manthiram, Joule 2017, 1, 10.
- 3A. Varotto, Rasing the standards: Enhanced catalytic performance for globle ammonia production, 2015.
- 4A. J. Medford, M. C. Hatzell, ACS Catal. 2017, 7, 2624.
- 5Y. H. Lu, Y. Yang, T. F. Zhang, Z. Ge, H. C. Chang, P. S. Xiao, Y. Y. Xie, L. Hua, Q. Y. Li, H. Y. Li, M. Bo, N. J. Guan, Y. F. Ma, Y. S. Chen, ACS Nano 2016, 10, 10507.
- 6T. Oshikiri, K. Ueno, H. Misawa, Angew. Chem., Int. Ed. 2016, 55, 3942.
- 7Z. W. Seh, J. Kibsgaard, C. F. Dickens, I. B. Chorkendorff, J. K. Norskov, T. F. Jaramillo, Science 2017, 355, eaad4998.
- 8S. Giddey, S. P. S. Badwal, A. Kulkarni, Int. J. Hydrogen Energy 2013, 38, 14576.
- 9C. X. Guo, A. Vasileff, S. Qiao, Energy Environ. Sci. 2017, 11, 45.
- 10S. Licht, B. C. Cui, B. H. Wang, F. F. Li, J. Lau, S. Z. Liu, Science 2014, 345, 637.
- 11V. Kyriakou, I. Garagounis, E. Vasileiou, A. Vourros, M. Stoukides, Catal. Today 2017, 286, 2.
- 12A. R. Singh, B. A. Rohr, J. A. Schwalbe, M. Cargnello, K. Chan, T. F. Jaramillo, I. Chorkendorff, J. K. Norskov, ACS Catal. 2017, 7, 706.
- 13R. Lan, J. T. S. Irvine, S. W. Tao, Sci. Rep. 2013, 3, 1145.
- 14K. Kugler, M. Luhn, J. A. Schramm, K. Rahimi, M. Wessling, Phys. Chem. Chem. Phys. 2015, 17, 3768.
- 15N. Jared, A. Jacob, W. Junhua, Y. Yushan, X. Bingjun, J. Electrochem. Soc. 2017, 164, F1712.
- 16H. M. Liu, S. H. Han, Y. Zhao, Y. Y. Zhu, X. L. Tian, J. H. Zeng, J. X. Jiang, B. Y Xia, Y. Chen, J. Mater. Chem. A 2018, 6, 3211.
- 17M. M. Shi, D. Bao, B. R. Wulan, Y. H. Li, Y. F. Zhang, J. M. Yan, Q. Jiang, Adv. Mater. 2017, 29, 1606550.
- 18D. Bao, Q. Zhang, F. L. Meng, H. X. Zhong, M. M. Shi, Y. Zhang, J. M. Yan, Q. Jiang, X. B. Zhang, Adv. Mater. 2017, 29, 1604799.
- 19S. J. Li, D. Bao, M. M. Shi, B. R. Wulan, J. M. Yan, Q. Jiang, Adv. Mater. 2017, 29, 1700001.
- 20E. Skulason, T. Bligaard, S. Gudmundsdottir, F. Studt, J. Rossmeisl, F. Abild-Pedersen, T. Vegge, H. Jonsson, J. K. Norskov, Phys. Chem. Chem. Phys. 2012, 14, 1235.
- 21J. H. Montoya, C. Tsai, A. Vojvodic, J. K. Norskov, ChemSusChem 2015, 8, 2180.
- 22S. M. Chen, S. Perathoner, C. Ampelli, C. Mebrahtu, D. S. Su, G. Centi, Angew. Chem., Int. Ed. 2017, 56, 2699.
- 23X. R. Zhao, F. X. Yin, N. Liu, G. R. Li, T. X. Fan, B. H. Chen, J. Mater. Sci. 2017, 52, 10175.
- 24K. Kim, C. Y. Yoo, J. N. Kim, H. C. Yoon, J. I. Han, J. Electrochem. Soc. 2016, 163, F1523.
- 25D. S. Yang, T. Chen, Z. J. Wang, J. Mater. Chem. A 2017, 5, 18967.
- 26Y. Abghoui, E. Skulason, J. Phys. Chem. C 2017, 121, 6141.
- 27Y. Abghoui, A. L. Garden, V. F. Hlynsson, S. Björgvinsdóttir, H. Ólafsdóttir, E. Skúlason, Phys. Chem. Chem. Phys. 2015, 17, 4909.
- 28A. Ishihara, K. Lee, S. Doi, S. Mitsushima, N. Kamiya, M. Hara, K. Domen, K. Fukuda, K. Ota, Electrochem. Solid-State Lett. 2005, 8, 201.
- 29L. Shen, S. Xu, N. Sun, T. Cheng, Q. Cui, Mater. Lett. 2008, 62, 1469.
- 30T. Suzuki, J. Inoue, H. Saito, M. Hirai, H. Suematsu, W. H. Jiang, K. Yatsui, Thin Solid Films 2006, 515, 2161.
- 31L. Castaldi, D. Kurapov, A. Reiter, V. Shklover, J. Patscheider, J. Appl. Phys. 2011, 109, 053720.
- 32A. Lippitz, T. Hübert, Surf. Coat. Technol. 2005, 200, 250.
- 33P. Wilhartitz, S. Dreer, P. Ramminger, Thin Solid Films 2004, 447–448, 289.