Abstract
The ability of a material to perform surface catalysis depends on the electronic structure features at the surface. Recent experiments on Fe2O3, one of the most studied water oxidation catalysts show that surface states may originate from adsorbed reaction intermediates that are cardinal for catalysis. Our recent theoretical DFT+U calculations confirm this hypothesis. In this paper, in order to account for more accurate electronic structure of the surface, we perform a one-shot GW calculation from a DFT+U wavefunction. We find that G0W0 overestimates the energy position of surface states, but provides good qualitative features of the surface’s electronic structure.
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Li Y, Chan SH, Sun Q (2015) Nanoscale 7:8663
Medford AJ, Vojvodic A, Hummelshøj JS, Voss J, Abild-Pedersen F, Studt F, Bligaard T, Nilsson A, Nørskov JK (2015) J Catal 328:36
Mao Y, Chen J, Wang H, Hu P (2015) Chin J Catal 36:1596
Zaffran J, Toroker MC (2016) Chem Phys Chem 17:1630
Zaffran J, Toroker MC (2016) Chem Sel 1:911
Man IC, Su H-Y, Calle-Vallejo F, Hansen HA, Martínez JI, Inoglu NG, Kitchin J, Jaramillo TF, Nørskov JK, Rossmeisl J (2011) Chem Cat Chem 3:1159
Rossmeisl J, Qu ZW, Zhu H, Kroes GJ, Nørskov JK (2007) J Electroanal Chem 607:83
Negreiros FR, Pedroza LS, Dalpian GM (2016) J Phys Chem C 120:11918
von Rudorff GF, Jakobsen R, Rosso KM, Blumberger J (2016) J Phys Chem Lett 7:1155
Tamirat AG, Rick J, Dubale AA, Su W-N, Hwang B-J (2016) Nanoscale Horiz 1:243
Young KMH, Klahr BM, Zandi O, Hamann TW (2013) Catal Sci Technol 3:1660
Klahr B, Hamann T (2014) J Phys Chem C 118:10393
Klahr B, Gimenez S, Fabregat-Santiago F, Bisquert J, Hamann TW (2012) Energy Environ Sci 5:7626
Cummings CY, Marken F, Peter LM, Upul Wijayantha KG, Tahir AA (2011) J Am Chem Soc 134:1228
Peter L (2013) J Solid State Electrochem 17:315
Barroso M, Mesa CA, Pendlebury SR, Cowan AJ, Hisatomi T, Sivula K, Grätzel M, Klug DR, Durrant JR (2012) Proc Natl Acad Sci USA 109:15640
Le Formal F, Pendlebury SR, Cornuz M, Tilley SD, Grätzel M, Durrant JR (2014) J Am Chem Soc 136:2564
Barroso M, Pendlebury SR, Cowan AJ, Durrant JR (2013) Chem Sci 4:2724
Le Formal F, Sivula K, Grätzel M (2012) J Phys Chem C 116:26707
Neufeld O, Yatom N, Caspary Toroker M (2015) ACS Catal 5:7237
Neufeld O, Toroker MC (2015) PCCP 17:24129
Trainor TP, Chaka AM, Eng PJ, Newville M, Waychunas GA, Catalano JG, Brown GE Jr (2004) Surf Sci 573:204
Hellman A, Pala RGS (2011) J Phys Chem C 115:12901
Liao P, Keith JA, Carter EA (2012) J Am Chem Soc 134:13296
Nguyen M-T, Piccinin S, Seriani N, Gebauer R (2015) ACS Catal 5:715
Nguyen M-T, Seriani N, Piccinin S, Gebauer R (2014) J Chem Phys 140:64703
Yatom N, Neufeld O, Caspary Toroker M (2015) J Phys Chem C 119:24789
Iandolo B, Hellman A (2014) Angew Chem 126:13622
Klahr B, Gimenez S, Fabregat-Santiago F, Hamann T, Bisquert J (2012) J Am Chem Soc 134:4294
Pendlebury SR, Barroso M, Cowan AJ, Sivula K, Tang J, Grätzel M, Klug D, Durrant JR (2011) Chem Commun 47:716
Cummings CY, Marken F, Peter LM, Tahir AA, Wijayantha KU (2012) Chem Commun 48:2027
Dotan H, Sivula K, Grätzel M, Rothschild A, Warren SC (2011) Energy Environ Sci 4:958
Dudarev SL, Botton GA, Savrasov SY, Humphreys CJ, Sutton AP (1998) Phys Rev B 57:1505
Zhou F, Cococcioni M, Marianetti CA, Morgan D, Ceder G (2004) Phys Rev B 70:235121
Anisimov VI, Aryasetiawan F, Lichtenstein AI (1997) J Phys 9:767
Rollmann G, Rohrbach A, Entel P, Hafner J (2004) Phys Rev B 69:165107
Wang L, Maxisch T, Ceder G (2006) Phys Rev B 73:195107
Toroker MC (2014) J Phys Chem C 118:23162
Neufeld O, Toroker MC (2015) J Phys Chem C 119:5836
Yatom N, Toroker M (2015) Molecules 20:19668
Yatom N, Toroker MC (2016) PCCP 18:16098
Neufeld O, Toroker MC (2016) J Chem Theory Comput 12:1572
Liao P, Carter EA (2011) PCCP 13:15189
Aryasetiawan F, Gunnarsson O (1998) Rep Prog Phys 61:237
Körzdörfer T, Marom N (2012) Phys Rev B 86:041110
Kresse G, Hafner J (1993) Phys Rev B 47:558
Kresse G, Furthmüller J (1996) Comp Mater Sci 6:15
Perdew JP, Burke K, Ernzerhof M (1997) Phys Rev Lett 78:1396
Mosey NJ, Liao P, Carter EA (2008) J Chem Phys 129:014103
Kresse G, Joubert D (1999) Phys Rev B 59:1758
Blöchl PE (1994) Phys Rev B 50:17953
Lehmann G, Taut M (1972) Physica Status solidi (b) 54:469
Nocedal J, Wright SJ (2006) Conjugate gradient methods. In: Numerical optimization. Springer, New York
Rohrbach A, Hafner J, Kresse G (2004) Phys Rev B 70:125426
Chambers SA, Yi SI (1999) Surf Sci 439:L785
Thevuthasan S, Kim YJ, Yi SI, Chambers SA, Morais J, Denecke R, Fadley CS, Liu P, Kendelewicz T, Brown GE Jr (1999) Surf Sci 425:276
Wang XG, Weiss W, Shaikhutdinov SK, Ritter M, Petersen M, Wagner F, Schlögl R, Scheffler M (1998) Phys Rev Lett 81:1038
Shaikhutdinov SK, Weiss W (1999) Surf Sci 432:L627
Greene ME, Chiaramonti AN, Christensen ST, Cao LX, Bedzyk MJ, Hersam MC (2005) Adv Mater 17:1765
Lemire C, Bertarione S, Zecchina A, Scarano D, Chaka A, Shaikhutdinov S, Freund HJ (2005) Phys Rev Lett 94:166101
Lad RJ, Henrich VE (1988) Surf Sci 193:81
Valdés Á, Qu ZW, Kroes GJ, Rossmeisl J, Nørskov JK (2008) J Phys Chem C 112:9872
Chen J, Selloni A (2012) J Phys Chem Lett 3:2808
Momma K, Izumi F (2008) J Appl Crystallogr 41:653
Merchant P, Collins R, Kershaw R, Dwight K, Wold A (1979) J Solid State Chem 27:307
Zimmermann R, Steiner P, Claessen R, Reinert F, Hüfner S, Blaha P, Dufek P (1999) J Phys 11:1657
Huang P, Carter EA (2008) Ann Rev Phys Chem 59:261
Acknowledgments
This research was supported by the Nancy and Stephen Grand Technion Energy Program, the I-CORE Program of the Planning and Budgeting Committee, and The Israel Science Foundation (Grant No. 152/11). N. Y. acknowledges excellence scholarships by the Department of Materials Science and Engineering at the Technion and by the Russell Barrie Nanotechnology Institute (RBNI) at the Technion.
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Yatom, N., Toroker, M.C. Electronic Structure of Catalysis Intermediates by the G0W0 Approximation. Catal Lett 146, 2009–2014 (2016). https://doi.org/10.1007/s10562-016-1825-3
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DOI: https://doi.org/10.1007/s10562-016-1825-3