Abstract
Oxidation state changes under reaction conditions are very common in heterogeneous catalysis. However, due to the limitation of experiment and computational methods, the relation between oxidation state and catalytic activity is not clear. Herein, we obtain the most stable structures of palladium oxide films with different oxidation states on palladium metal surfaces using density functional theory calculations and a state-of-the-art optimization method, namely the particle swarm optimization. These structures clearly show the process of palladium oxide film formation on metallic surfaces. Using CO oxidation as a model reaction, we find that the activities increase first and then decrease with the increase of oxidation states, peaking at Pd4O3. Our findings offer an understanding of the phase transformation and the activity of non-stoichiometric phases.
Similar content being viewed by others
References
Reuter K, Scheffler M. Phys Rev B, 2001, 65: 035406
Wang HF, Kavanagh R, Guo YL, Guo Y, Lu G, Hu P. J Catal, 2012, 296: 110–119
Tao FF, Shan JJ, Nguyen L, Wang Z, Zhang S, Zhang L, Wu Z, Huang W, Zeng S, Hu P. Nat Commun, 2015, 6: 7798
Hu W, Lan J, Guo Y, Cao XM, Hu P. ACS Catal, 2016, 6: 5508–5519
Yang M, Yuan H, Wang H, Hu P. Sci China Chem, 2018, 61: 457–467
Wang Z, Liu X, Rooney DW, Hu P. Surf Sci, 2015, 640: 181–189
Tyo EC, Yin C, Di Vece M, Qian Q, Kwon G, Lee S, Lee B, DeBartolo JE, Seifert S, Winans RE, Si R, Ricks B, Goergen S, Rutter M, Zugic B, Flytzani-Stephanopoulos M, Wang ZW, Palmer RE, Neurock M, Vajda S. ACS Catal, 2012, 2012: 2409–2423
Wang J, Wang H, Hu P. Sci China Chem, 2018, 61: 336–343
Duchesne PN, Chen G, Zhao X, Zheng N, Zhang P. J Phys Chem C, 2014, 118: 28861–28867
Chen D, Chen C, Baiyee ZM, Shao Z, Ciucci F. Chem Rev, 2015, 115: 9869–9921
Over H, Muhler M. Prog Surf Sci, 2003, 72: 3–17
Over H, Kim YD, Seitsonen AP, Wendt S, Lundgren E, Schmid M, Varga P, Morgante A, Ertl G. Science, 2000, 287: 1474–1476
Soon A, Todorova M, Delley B, Stampfl C. Phys Rev B, 2006, 73: 165424
Lundgren E, Kresse G, Klein C, Borg M, Andersen JN, De Santis M, Gauthier Y, Konvicka C, Schmid M, Varga P. Phys Rev Lett, 2002, 88: 246103
Chueh WC, Falter C, Abbott M, Scipio D, Furler P, Haile SM, Steinfeld A. Science, 2010, 330: 1797–1801
Zhang S, Shan J, Zhu Y, Frenkel AI, Patlolla A, Huang W, Yoon SJ, Wang L, Yoshida H, Takeda S, Tao FF. J Am Chem Soc, 2013, 135: 8283–8293
Wang JB, Tsai DH, Huang TJ. J Catal, 2002, 208: 370–380
Wang Z, Cao XM, Zhu J, Hu P. J Catal, 2014, 311: 469–480
Falsig H, Hvolbaek B, Kristensen IS, Jiang T, Bligaard T, Christensen CH, Nørskov JK. Angew Chem Int Ed, 2008, 47: 4835–4839
Chen Y, Vlachos DG. Ind Eng Chem Res, 2012, 51: 12244–12252
Gong XQ, Raval R, Hu P. Phys Rev Lett, 2004, 93: 106104
Hong S, Karim A, Rahman TS, Jacobi K, Ertl G. J Catal, 2010, 276: 371–381
Weaver JF, Zhang F, Pan L, Li T, Asthagiri A. Acc Chem Res, 2015, 48: 1515–1523
Zhang F, Pan L, Li T, Diulus JT, Asthagiri A, Weaver JF. J Phys Chem C, 2014, 118: 28647–28661
Zhang F, Li T, Pan L, Asthagiri A, Weaver JF. Catal Sci Technol, 2014, 4: 3826–3834
Lu S, Wang Y, Liu H, Miao MS, Ma Y. Nat Commun, 2014, 5: 3666
Wang Y, Lv J, Zhu L, Ma Y. Comput Phys Commun, 2012, 183: 2063–2070
Kresse G, Furthmüller J. Phys Rev B, 1996, 54: 11169–11186
Kresse G, Furthmüller J. Comput Mater Sci, 1996, 6: 15–50
Kresse G, Hafner J. Phys Rev B, 1994, 49: 14251–14269
Kresse G, Hafner J. Phys Rev B, 1993, 47: 558–561
Perdew JP, Burke K, Ernzerhof M. Phys Rev Lett, 1996, 77: 3865–3868
Kresse G, Joubert D. Phys Rev B, 1999, 59: 1758–1775
Blöchl PE. Phys Rev B, 1994, 50: 17953–17979
Michaelides A, Liu ZP, Zhang CJ, Alavi A, King DA, Hu P. J Am Chem Soc, 2003, 125: 3704–3705
Liu ZP, Hu P. J Am Chem Soc, 2003, 125: 1958–1967
Alavi A, Hu P, Deutsch T, Silvestrelli PL, Hutter J. Phys Rev Lett, 1998, 80: 3650–3653
Wu H, Qian Y, Lu S, Kan E, Lu R, Deng K, Wang H, Ma Y. Phys Chem Chem Phys, 2015, 17: 15694–15700
Lausche AC, Medford AJ, Khan TS, Xu Y, Bligaard T, Abild-Pedersen F, Nørskov JK, Studt F. J Catal, 2013, 307: 275–282
Mehar V, Kim M, Shipilin M, van den Bossche M, Gustafson J, Merte LR, Hejral U, Grönbeck H, Lundgren E, Asthagiri A, Weaver JF. ACS Catal, 2018, 8: 8553–8567
Shipilin M, Gustafson J, Zhang C, Merte LR, Stierle A, Hejral U, Ruett U, Gutowski O, Skoglundh M, Carlsson PA, Lundgren E. J Phys Chem C, 2015, 119: 15469–15476
Gong XQ, Liu ZP, Raval R, Hu P. J Am Chem Soc, 2004, 126: 8–9
Jin M, Park JN, Shon JK, Kim JH, Li Z, Park YK, Kim JM. Catal Today, 2012, 185: 183–190
Duan Z, Henkelman G. ACS Catal, 2014, 4: 3435–3443
Engel T, Ertl G. J Chem Phys, 1978, 69: 1267–1281
Szanyi J, Kuhn WK, Goodman DW. J Phys Chem, 1994, 98: 2978–2981
Zhang CJ, Hu P. J Am Chem Soc, 2000, 122: 2134–2135
Wang HF, Kavanagh R, Guo YL, Guo Y, Lu GZ, Hu P. Angew Chem Int Ed, 2012, 51: 6657–6661
Acknowledgements
The authors gratefully acknowledge UK’s national high performance computing service ARCHER (for which access was obtained via the UKCP consortium) for computing time. This work was supported by the National Natural Science Foundation of China (21333003) and Queens University Belfast for a Ph.D. studentship.
Author information
Authors and Affiliations
Corresponding author
Electronic supplementary material
Rights and permissions
About this article
Cite this article
Wang, Z., Hu, P. Identifying the general trend of activity of non-stoichiometric metal oxide phases for CO oxidation on Pd(111). Sci. China Chem. 62, 784–789 (2019). https://doi.org/10.1007/s11426-018-9445-7
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11426-018-9445-7