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The electrochemical reduction of nitrogen to ammonia is a promising way to produce ammonia at mild condition. The design and preparation of an efficient catalyst with high ammonia selectivity is critical for the real applications. In this work, a series of transition metal (TM = Sc, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Y, Zr, Nb, Mo, Tc, Ru, Rh, Pd, Ag, and Cd) atoms supported by gt-C3N4 (TM/gt-C3N4) are investigated as electrocatalysts for the nitrogen reduction reaction (NRR) based on density functional calculations. It is found that Mo/gt-C3N4 with a limiting potential of -0.82 V is the best catalyst for standing-on adsorbed N2 cases. While for lying-on adsorbed N2 cases, V/gt-C3N4 with a limiting potential of -0.79 V is better than other materials. It is believed that this work provides several promising candidates for the non-noble metal electrocatalysts for NRR at mild condition.
Smil, V. Detonator of the population explosion. Nature 1999, 400, 415.
Anantharaman, B.; Hazarika, S.; Ahmad, T.; Nagvekar, M.; Ariyapadi, S.; Gualy, R. Coal gasification technology for ammonia plants. In Proceedings of the Nitrogen & Syngas 2012 Conference, Houston, TX, USA, 2012, pp 1–10.
Erisman, J. W.; Sutton, M. A.; Galloway, J.; Klimont, Z.; Winiwarter, W. How a century of ammonia synthesis changed the world. Nat. Geosci. 2008, 1, 636–639.
Back, S.; Jung, Y. On the mechanism of electrochemical ammonia synthesis on the Ru catalyst. Phys. Chem. Chem. Phys. 2016, 18, 9161–9166.
Burgess, B. K.; Lowe, D. J. Mechanism of molybdenum nitrogenase. Chem. Rev. 1996, 96, 2983–3012.
Jacobsen, C. J. H.; Dahl, S.; Hansen, P. L.; Törnqvist, E.; Jensen, L.; Topsøe, H.; Prip, D. V.; Møenshaug, P. B.; Chorkendorff, I. Structure sensitivity of supported ruthenium catalysts for ammonia synthesis. J. Mol. Catal. A-Chem. 2000, 163, 19–26.
Ertl, G. Primary steps in catalytic synthesis of ammonia. J. Vac. Sci. Technol. A 1983, 1, 1247–1253.
Aparicio, L. M.; Dumesic, J. A. Ammonia synthesis kinetics: Surface chemistry, rate expressions, and kinetic analysis. Top. Catal. 1994, 1, 233–252.
Boudart, M. Ammonia synthesis: The bellwether reaction in heterogeneous catalysis. Top. Catal. 1994, 1, 405–414.
Shi, M. M.; Bao, D.; Wulan, B. R.; Li, Y. H.; Zhang, Y. F.; Yan, J. M.; Jiang, Q. Au sub-nanoclusters on TiO2 toward highly efficient and selective electrocatalyst for N2 conversion to NH3 at ambient conditions. Adv. Mater. 2017, 29, 1606550.
Kamiya, K.; Tatebe, T.; Yamamura, S.; Iwase, K.; Harada, T.; Nakanishi, S. Selective reduction of nitrate by a local cell catalyst composed of metal-doped covalent triazine frameworks. ACS Catal. 2018, 8, 2693–2698.
Li, S. J.; Bao, D.; Shi, M. M.; Wulan, B. R.; Yan, J. M.; Jiang, Q. Amorphizing of Au nanoparticles by CeOx–RGO Hybrid support towards highly efficient electrocatalyst for N2 reduction under ambient conditions. Adv. Mater. 2017, 29, 1700001.
Zhang, Y.; Qiu, W. B.; Ma, Y. J.; Luo, Y. L.; Tian, Z. Q.; Cui, G. W.; Xie, F. Y.; Chen, L.; Li, T. S.; Sun, X. P. High-performance electrohydrogenation of N2 to NH3 catalyzed by multishelled hollow Cr2O3 microspheres under ambient conditions. ACS Catal. 2018, 8, 8540–8544.
Wang, L.; Xia, M. K.; Wang, H.; Huang, K. F.; Qian, C. X.; Maravelias, C. T.; Ozin, G. A. Greening ammonia toward the solar ammonia refinery. Joule 2018, 2, 1055–1074.
Nazemi, M.; Panikkanvalappil, S. R.; El-Sayed M. A. Enhancing the rate of electrochemical nitrogen reduction reaction for ammonia synthesis under ambient conditions using hollow gold nanocages. Nano Energy 2018, 49, 316–323.
Zhang, L.; Ji, X. Q.; Ren, X.; Luo, Y. L.; Shi, X. F.; Asiri, A. M.; Zheng, B. Z.; Sun, X. P. Efficient electrochemical N2 reduction to NH3 on MoN nanosheets array under ambient conditions. ACS Sustainable Chem. Eng. 2018, 6, 9550–9554.
Chen, J. G.; Crooks, R. M.; Seefeldt, L. C.; Bren, K. L.; Morris Bullock, R.; Darensbourg, M. Y.; Holland, P. L.; Hoffman, B.; Janik, M. J.; Jones, A. K. et al. Beyond fossil fuel–driven nitrogen transformations. Science 2018, 360, 873.
Dahl, S.; Logadottir, A.; Egeberg, R. C.; Larsen, J. H.; Chorkendorff, I.; Törnqvist, E.; Nørskov, J. K. Role of steps in N2 activation on Ru(0001). Phys. Rev. Lett. 1999, 83, 1814–1817.
Dahl, S.; Törnqvist, E.; Chorkendorff, I. Dissociative adsorption of N2 on Ru(0001): A surface reaction totally dominated by steps. J. Catal. 2000, 192, 381–390.
Murakami, T.; Nishikiori, T.; Nohira, T.; Ito, Y. Electrolytic synthesis of ammonia in molten salts under atmospheric pressure. J. Am. Chem. Soc. 2003, 125, 334–335.
Dahl, S.; Sehested, J.; Jacobsen, C. J. H.; Törnqvist, E.; Chorkendorff, I. Surface science based microkinetic analysis of ammonia synthesis over ruthenium catalysts. J. Catal. 2000, 192, 391–399.
Kojima, R.; Aika, K. I. Molybdenum nitride and carbide catalysts for ammonia synthesis. Appl. Catal. A-Gen. 2001, 219, 141–147.
Rod, T. H.; Logadottir, A.; Nørskov, J. K. Ammonia synthesis at low temperatures. J. Chem. Phys. 2000, 112, 5343–5347.
Hinnemann, B.; Nørskov, J. K. Modeling a central ligand in the nitrogenase FeMo cofactor. J. Am. Chem. Soc. 2003, 125, 1466–1467.
Logadottir, A.; Rod, T. H.; Nørskov, J. K.; Hammer, B.; Dahl, S.; Jacobsen, C. J. H. The Brønsted–Evans–Polanyi relation and the volcano plot for ammonia synthesis over transition metal catalysts. J. Catal. 2001, 197, 229–231.
Logadóttir, Á.; Nørskov, J. K. Ammonia synthesis over a Ru(0001) surface studied by density functional calculations. J. Catal. 2003, 220, 273–279.
Hellman, A.; Honkala, K.; Remediakis, I. N.; Logadóttir, Á.; Carlsson, A.; Dahl, S.; Christensen, C. H.; Nørskov, J. K. Ammonia synthesis and decomposition on a Ru-based catalyst modeled by first-principles. Surf. Sci. 2009, 603, 1731–1739.
Hellman, A.; Baerends, E. J.; Biczysko, M.; Bligaard, T.; Christensen, C. H.; Clary, D. C.; Dahl, S.; Van Harrevelt, R.; Honkala, K.; Jónsson, H. et al. Predicting catalysis: Understanding ammonia synthesis from first-principles calculations. J. Phys. Chem. B 2006, 110, 17719–17735.
Liu, C. W.; Li, Q. Y.; Zhang, J.; Jin, Y. G.; MacFarlane, D. R.; Sun, C. H. Theoretical evaluation of possible 2D boron monolayer in N2 electrochemical conversion into ammonia. J. Phys. Chem. C 2018, 122, 25268–25273.
Choi, C.; Back, S.; Kim, N. Y.; Lim, J.; Kim, Y. H.; Jung, Y. Suppression of hydrogen evolution reaction in electrochemical N2 reduction using single-atom catalysts: A computational guideline. ACS Catal. 2018, 8, 7517–7525.
Zhao, J. X.; Chen, Z. F. Single Mo atom supported on defective boron nitride monolayer as an efficient electrocatalyst for nitrogen fixation: A computational study. J. Am. Chem. Soc. 2017, 139, 12480–12487.
Ling, C. Y.; Ouyang, Y. X.; Li, Q.; Bai, X. W.; Mao, X.; Du, A. J.; Wang, J. L. A general two-step strategy-based high-throughput screening of single atom catalysts for nitrogen fixation. Small Methods 2018, 1800376, DOI: 10.1002/smtd.201800376.
Ling, C. Y.; Bai, X. W.; Ouyang, Y. X.; Du, A. J.; Wang, J. L. Single molybdenum atom anchored on N-doped carbon as a promising electrocatalyst for nitrogen reduction into ammonia at ambient conditions. J. Phys. Chem. C 2018, 122, 16842–16847.
Ling, C. Y.; Niu, X. H.; Li, Q.; Du, A. J.; Wang, J. L. Metal-free single atom catalyst for N2 fixation driven by visible light. J. Am. Chem. Soc. 2018, 140, 14161–14168.
Liang, S. X.; Hao, C.; Shi, Y. T. The power of single-atom catalysis. ChemCatChem 2015, 7, 2559–2567.
Li, X. F.; Li, Q. K.; Cheng, J.; Liu, L. L.; Yan, Q.; Wu, Y. C.; Zhang, X. H.; Wang, Z. Y.; Qiu, Q.; Luo, Y. Conversion of dinitrogen to ammonia by FeN3-embedded graphene. J. Am. Chem. Soc. 2016, 138, 8706–8709.
Le, Y. Q.; Gu, J.; Tian, W. Q. Nitrogen-fixation catalyst based on graphene: Every part counts. Chem. Commun. 2014, 50, 13319–13322.
Dong, G. P.; Zhang, Y. H.; Pan, Q. W.; Qiu, J. R. A fantastic graphitic carbon nitride (g-C3N4) material: Electronic structure, photocatalytic and photoelectronic properties. J. Photochem. Photobiol. C-Photochem. Rev. 2014, 20, 33–50.
Ghosh, D.; Periyasamy, G.; Pandey, B.; Pati, S. K. Computational studies on magnetism and the optical properties of transition metal embedded graphitic carbon nitride sheets. J. Mater. Chem. C 2014, 2, 7943–7951.
Gao, D. Q.; Xu, Q.; Zhang, J.; Yang, Z. L.; Si, M. S.; Yan, Z. J.; Xue, D. S. Defect-related ferromagnetism in ultrathin metal-free g-C3N4 nanosheets. Nanoscale 2014, 6, 2577–2581.
Xu, K.; Li, X. L.; Chen, P. Z.; Zhou, D.; Wu, C. Z.; Guo, Y. Q.; Zhang, L. D; Zhao, J. Y.; Wu, X. J.; Xie, Y. Hydrogen dangling bonds induce ferromagnetism in two-dimensional metal-free graphitic-C3N4 nanosheets. Chem. Sci. 2015, 6, 283–287.
Choudhuri, I.; Bhattacharyya, G.; Kumar, S.; Pathak, B. Metal-free half-metallicity in a high energy phase C-doped gh-C3N4 system: A high Curie temperature planar system. J. Mater. Chem. C 2016, 4, 11530–11539.
Zhang, Y.; Wang, Z.; Cao, J. X. Prediction of magnetic anisotropy of 5d transition metal-doped g-C3N4. J. Mater. Chem. C 2014, 2, 8817–8821.
Ghosh, D.; Periyasamy, G.; Pati, S. K. Transition metal embedded two-dimensional C3N4-graphene nanocomposite: A multifunctional material. J. Phys. Chem. C 2014, 118, 15487–15494.
Singh, A. R.; Montoya, J. H.; Rohr, B. A.; Tsai, C.; Vojvodic, A.; Nørskov, J. K. Computational design of active site structures with improved transition-state scaling for ammonia synthesis. ACS Catal. 2018, 8, 4017–4024.
Skúlason, E.; Bligaard, T.; Gudmundsdóttir, S.; Studt, F.; Rossmeisl, J.; Abild-Pedersen, F.; Vegge, T.; Jónsson, H.; Nørskov, J. K. A theoretical evaluation of possible transition metal electro-catalysts for N2 reduction. Phys. Chem. Chem. Phys. 2012, 14, 1235–1245.
Montoya, J. H.; Tsai, C.; Vojvodic, A.; Nørskov, J. K. The challenge of electrochemical ammonia synthesis: A new perspective on the role of nitrogen scaling relations. ChemSusChem 2015, 8, 2180–2186.
Han, L. L.; Liu, X. J.; Chen, J. P.; Lin, R. Q.; Liu, H. X.; Lü, F.; Bak, S.; Liang, Z. X.; Zhao, S. Z.; Stavitski, E. et al. Atomically dispersed molybdenum catalysts for efficient ambient nitrogen fixation. Angew. Chem. , Int. Ed. 2019, 58, 2321–2325.
Kitchin, J. R.; Nørskov, J. K.; Barteau, M. A.; Chen, J. G. Modification of the surface electronic and chemical properties of Pt(111) by subsurface 3D transition metals. J. Chem. Phys. 2004, 120, 10240–10246.
Bond, G. C. Catalysis by Metals; Academic Press: London, 1962.
Ozaki, A.; Aika, K. Catalytic activation of dinitrogen. In Catalysis-Science and Technology. Anderson, J. R.; Boudart, M., Eds.; Springer-Verlag: Berlin, 1981; pp 87–158.
Kresse, G.; Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 1999, 59, 1758–1775.
Perdew, J. P.; Burke, K.; Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 1996, 77, 3865–3868.
Grimme, S. Semiempirical GGA-type density functional constructed with a long-range dispersion correction. J. Comput. Chem. 2006, 27, 1787–1799.
Nørskov, J. K.; Rossmeisl, J.; Logadottir, A.; Lindqvist, L.; Kitchin, J. R.; Bligaard, T.; Jónsson, H. Origin of the overpotential for oxygen reduction at a fuel-cell cathode. J. Phys. Chem. B 2004, 108, 17886–17892.
Vegge, T.; Rasmussen, T.; Leffers, T.; Pedersen, O. B.; Jacobsen, K. W. Atomistic simulations of cross-slip of jogged screw dislocations in copper. Philos. Mag. Lett. 2001, 81, 137–144.
Howalt, J. G.; Bligaard, T.; Rossmeisl, J.; Vegge, T. DFT based study of transition metal nano-clusters for electrochemical NH3 production. Phys. Chem. Chem. Phys. 2013, 15, 7785–7795.
Computational Chemistry Comparison and Benchmark Database. https://cccbdb.nist.gov/.
Rossmeisl, J.; Qu, Z. W.; Zhu, H.; Kroes, G. J.; Nørskov, J. K. Electrolysis of water on oxide surfaces. J. Electroanal. Chem. 2007, 607, 83–89.
Rossmeisl, J.; Logadottir, A.; Nørskov, J. K. Electrolysis of water on (oxidized) metal surfaces. Chem. Phys. 2005, 319, 178–184.
Peterson, A. A.; Abild-Pedersen, F.; Studt, F.; Rossmeisl, J.; Nørskov, J. K. How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels. Energy Environ. Sci. 2010, 3, 1311–1315.
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