Abstract
In an effort to determine the active state of supported palladium for the direct formation of H2O2 from H2 and O2, the catalytic behavior of Pd0/SiO2, PdO/SiO2 and partially reduced PdO/SiO2 was determined. The results obtained in an ethanol slurry, with chloride ions and H2SO4 being present, showed that the PdO/SiO2 catalyst was almost completely inactive for the formation of H2O2 at 10 °C. The Pd0/SiO2 catalyst exhibited the highest activity for H2O2 formation, and the PdO/SiO2 material, reduced under very mild conditions, exhibited an intermediate activity. The state of Pd on the three catalysts was characterized by XRD, TEM and XPS methods. Only Pd0 (the metal phase) and PdO were observed on Pd0/SiO2 and PdO/SiO2, respectively. As expected, with the partially reduced PdO/SiO2 catalyst, both Pd0 and PdO phases were evident. The TEM results revealed that the Pd0 particles decorated the larger PdO particles. The results reported here support the role of metallic palladium, rather than the oxide, as the active phase for the direct formation of H2O2.
Similar content being viewed by others
References
Hess WT (1995) In: Kroschwitz JI, Howe-Grant M (eds) Kirk-Othmer encyclopedia of chemical technology, vol 13, 4th edn. Wiley, New York, p 961
(2005) Chemical & Engineering News 83(42) 13 (October 17)
Krishan VV, Dokoutchaev AG, Thompson ME (2000) J Catal 196:366
Burch R, Ellis PR (2003) Appl Catal B Environ 42:203
Landon P, Collier PJ, Carley AF, Chadwick D, Papworth AJ, Burrows A, Kielyd CJ, Hutchings GJ (2003) Phys Chem Chem Phys 5:1917
Liu Q, Lunsford JH (2006) J Catal 239:237
Choudhary VR, Jana P (2007) J Catal 246:434
Liu Q, Bauer JC, Schaak RE, Lunsford JH (2008) Angew Chem Int Ed 47:6221
Choudhary VR, Samanta C (2006) J Catal 238:28
Liu Q, Lunsford JH (2006) Appl Catal A Gen 314:94
Choudhary VR, Gaikwad AG, Sansare SD (2002) Catal Lett 83:235
Choudhary VR, Sansare SD, Gaikwad AG (2002) Catal Lett 84:81
Gosser LW (1989) US Patent 4,889,705 to DuPont
Choudhary VR, Samanta C, Jana P (2007) Appl Catal A Gen 332:70
Samanta C (2008) Appl Catal A Gen 350:133
Blanco-Brieva G, Cano-Serrano E, Campos-Martin JM, Fierro JLG (2004) Chem Commun 1184
Burato C, Campestrini S, Han Y-F, Canton P, Centomo P, Canu P, Corain B (2009) Appl Catal A Gen 358:224
Melada S, Rioda R, Menegazzo F, Pinna F, Strukul G (2006) J Catal 239:422
Datye AK, Bravo J, Nelson TR, Atanasova P, Lyubovsky M, Pfefferle L (2000) Appl Catal A Gen 198:179
Chinta S, Lunsford JH (2004) J Catal 225:249
Cohen IR, Purcell TC, Altshuller AP (1967) Environ Sci Technol 1:247
Wagner CD, Riggs WM, Davis LE, Moulder JF, Muilenberg GE (1978) Handbook of X-ray photoelectron spectroscopy. Physical Electronics Division, Perkin-Elmer Corp, Eden Prairie, MN
Penner S, Wang D, Jenewein B, Gabasch H, Klötzer B, Knop-Gericke A, Schlögl R, Hayek K (2006) J Chem Phys 125:094703
Penner S, Bera P, Pedersen S, Ngo LT, Harris JJW, Campbell CT (2006) J Phys Chem B 110:24577
Ketteler G, Ogeltree DF, Bluhm H, Liu H, Hebenstreit ELD, Salmeron M (2005) J Am Chem Soc 127:18269
Gaikwad AG, Sansare SD, Choudhary VR (2002) J Mol Catal A Chem 181:143
Samanta C, Choudhary VR (2007) Appl Catal A Gen 330:23
Choudhary VR, Jana P (2007) Appl Catal A Gen 329:79
Samanta C, Choudhary VR (2007) Appl Catal A Gen 326:28
Samanta C, Choudhary VR (2007) Catal Commun 8:73
Pospelova TA, Kobozev NI (1961) Rus J Phys Chem Trans 35:262
Lunsford JH (2003) J Catal 216:455
Dissanayake DP, Lunsford JH (2003) J Catal 214:113
Gao F, Wang Y, Cai Y, Goodman DW (2009) J Phys Chem C 113:174
Acknowledgments
We gratefully acknowledge financial support from DuPont, the National Science Foundation (DMR-0545201) and the Robert A. Welch Foundation (Grant No. A-1583).
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Liu, Q., Gath, K.K., Bauer, J.C. et al. The Active Phase in the Direct Synthesis of H2O2 from H2 and O2 over Pd/SiO2 Catalyst in a H2SO4/Ethanol System. Catal Lett 132, 342–348 (2009). https://doi.org/10.1007/s10562-009-0104-y
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10562-009-0104-y