Abstract
Catalytic ethane dehydrogenation was studied with density functional theory (DFT) calculations to investigate the differing role of Sn in the bulk and surface of PtSn alloys on the activity, selectivity, and stability of the catalyst. Pristine Pt(111), a surface alloy of Pt3Sn/Pt(111) and a bulk alloy of Pt3Sn(111) were compared. Binding energies of adsorbates were weakened by Sn on both alloys. With few changes for binding geometries of adsorbates, the change in binding energies was mainly attributed to the changes in the electronic interaction due to the strain effect and/or the ligand effect from d-band theory on the alloys. Especially, the combination of ligand and strain effects on the bulk alloy made the binding energies of adsorbates generally weaker than on Pt but stronger than on the surface alloy. In the successive dehydrogenation of C2Hx species, the activity was expected in the order of Pt > Pt3Sn > Pt3Sn/Pt by comparing the activation energies for ethene formation. The selectivity toward ethene was predicted using two descriptors from which the best selectivity was expected on Pt3Sn/Pt. Sn in the bulk made the gap between the barriers for ethene desorption and further dehydrogenation comparable, whereas ethene desorption was much more favorable on Pt3Sn/Pt. The preference for ethene formation from ethyl was also weakened on Pt3Sn. Therefore, despite the higher Sn composition, worse selectivity was predicted for Sn-rich bulk alloy than the surface alloy, followed by Pt.
Similar content being viewed by others
References
Ridha T, Li Y, Gençer E, Siirola JJ, Miller JT, Ribeiro FH, Agrawal R (2018) Processes 6:139
Wang Q, Chen X, Jha AN, Rogers H (2014) Renew Sustain Energy Rev 30:1–28
Sattler JJHB, Ruiz-Martinez J, Santillan-Jimenez E, Weckhuysen BM (2014) Chem Rev 114:10613–10653
Amghizar I, Vandewalle LA, Van Geem KM, Marin GB (2017) Engineering 3:171–178
Sadrameli SM (2015) Fuel 140:102–115
Cavani F, Ballarini N, Cericola A (2007) Catal Today 127:113–131
Sadrameli SM (2016) Fuel 173:285–297
Lee DY, Elgowainy A (2018) Int J Hydrog Energy 43:20143–20160
Vora BV (2012) Top Catal 55:1297–1308
Galvita V, Siddiqi G, Sun P, Bell AT (2010) J Catal 271:209–219
Wu J, Peng Z, Bell AT (2014) J Catal 311:161–168
Wegener EC, Wu Z, Tseng HT, Gallagher JR, Ren Y, Diaz RE, Ribeiro FH, Miller JT (2018) Catal Today 299:146–153
Siddiqi G, Sun P, Galvita V, Bell AT (2010) J Catal 274:200–206
Xiao L, Ma F, Zhu YA, Sui ZJ, Zhou JH, Zhou XG, Chen D, Yuan WK (2019) Chem Eng J 377:120049
Yang ML, Zhu YA, Zhou XG, Sui ZJ, Chen D (2012) ACS Catal 2:1247–1258
Nykänen L, Honkala K (2011) J Phys Chem C 115:9578–9586
Nykänen L, Honkala K (2013) ACS Catal 3:3026–3030
Hansen MH, Nørskov JK, Bligaard T (2019) J Catal 374:161–170
Zhang Y, Zhou Y, Shi J, Zhou S, Sheng X, Zhang Z, Xiang S (2014) J Mol Catal A 381:138–147
Lee MH, Nagaraja BM, Lee KY, Jung KD (2014) Catal Today 232:53–62
Kim J, Fu J, Podkolzin SG, Koel BE (2010) J Phys Chem C 114:17238–17247
Liu Y, Li D, Stamenkovic VR, Soled S, Henao JD, Sun S (2011) ACS Catal 1:1719–1723
Somodi F, Peng Z, Getsoian AB, Bell AT (2011) J Phys Chem C 115:19084–19090
Crabb EM, Marshall R, Thompsett D (2000) J Electrochem Soc 147:4440–4447
Hook A, Massa JD, Celik FE (2016) J Phys Chem C 120:27307–27318
Chen Y, Vlachos DG (2010) J Phys Chem C 114:4973–4982
Yang ML, Zhu J, Zhu YA, Sui ZJ, Yu YD, Zhou XG, Chen D (2014) J Mol Catal A 395:329–336
Haubrich J, Becker C, Wandelt K (2009) Surf Sci 603:1476–1485
Peng G, Gerceker D, Kumbhalkar M, Dumesic JA, Mavrikakis M (2018) Catal Sci Technol 8:2159–2174
Hook A, Celik FE (2017) J Phys Chem C 121:17882–17892
Saerens S, Sabbe MK, Galvita VV, Redekop EA, Reyniers MF, Marin GB (2017) ACS Catal 7:7495–7508
Kresse G, Furthmüller J (1996) Comput Mater Sci 6:15–50
Kresse G, Furthmüller J (1996) Phys Rev B 54:11169–11186
Perdew JP, Wang Y (1992) Phys Rev B 45:13244–13249
Blöchl PE (1994) Phys Rev B 50:17953–17979
Kresse G, Joubert D (1999) Phys Rev B 59:1758–1775
Jiang L, Sun G, Sun S, Liu J, Tang S, Li H, Zhou B, Xin Q (2005) Electrochim Acta 50:5384–5389
Atrei A, Bardi U, Rovida G, Torrini M, Zanazzi E (1992) Phys Rev B 46:1649–1654
Neugebauer J, Scheffler M (1992) Phys Rev B 46:16067–16080
Monkhorst HJ, Pack JD (1976) Phys Rev B 13:5188–5192
Henkelman G, Uberuaga BP, Jónsson H (2000) J Chem Phys 113:9901–9904
Duan Z, Zhong J, Wang G (2010) J Chem Phys 133:114701
Viñes F, Lykhach Y, Staudt T, Lorenz MPA, Papp C, Steinrück HP, Libuda J, Neyman KM, Görling A (2010) Chem Eur J 16:6530–6539
Yang ML, Zhu YA, Fan C, Sui ZJ, Chen D, Zhou XG (2010) J Mol Catal A 321:42–49
Watwe RM, Cortright RD, Mavrikakis M, Nørskov JK, Dumesic JA (2001) J Chem Phys 114:4663–4668
Zhao ZJ, Moskaleva LV, Aleksandrov HA, Basaran D, Rösch N (2010) J Phys Chem C 114:12190–12201
Hammer B, Nørskov JK (1995) Surf Sci 343:211–220
Hammer B, Nørskov JK (1995) Nature 376:238–240
Xu Y, Ruban AV, Mavrikakis M (2004) J Am Chem Soc 126:4717–4725
Delbecq F, Sautet P (2003) J Catal 220:115–126
Kitchin JR, Nørskov JK, Barteau MA, Chen JG (2004) J Chem Phys 120:10240–10246
Tasbihi M, Feyzi F, Amlashi MA, Abdullah AZ, Mohamed AR (2007) Fuel Process Technol 88:883–889
Acknowledgements
This work used resources from the Rutgers Discovery Informatics Institute, which are supported by Rutgers and the State of New Jersey. The authors would like to thank Dr. Alec Hook for his leadership in the early stages of this project.
Funding
This work was funded by the National Science Foundation under Grant Number CBET-1705746.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no conflict of interest.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Electronic supplementary material
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Nam, J., Celik, F.E. Effect of Tin in the Bulk of Platinum–Tin Alloys for Ethane Dehydrogenation. Top Catal 63, 700–713 (2020). https://doi.org/10.1007/s11244-020-01297-w
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11244-020-01297-w