Pt, PtSn 촉매를 제조한 후, 재분산 연구를 위해 수소분위기에서 소결시킨 후 여러 온도에서 산소처리를 적용하여 백 금주석입자의 재분산 정도를 확인하고, 프로판 탈수소 반응실험으로 촉매의 활성을 측정하여 촉매의 물리적, 화학적 상태 변화와 활성의 관계를 이해하고자 하였다. 재분산 처리에 따른 촉매 활성 금속의 상태 및 촉매 입자 간 상호작용 등을 보기 위해 X-선 회절분석(XRD), CO-화학흡착(CO-pulse chemisorption), 수소 승온환원(H2-TPR) 분석을 실시하 였다. 산소 재분산 처리 조건에 따라 백금의 분산도 및 입자 크기, 촉매의 결정상 및 환원 거동이 달라지는 것을 확인 하였다. 촉매를 재분산 처리하였을 시 500℃에서 산소 처리한 촉매가 가장 높은 전환율과 활성회복률을 보였다. 500 ℃ 로 산소 처리한 촉매가 백금의 분산도도 비교적 높게 나타나고, 평균 입자 크기가 작아지는 것을 XRD와 CO-화학흡 착 결과로부터 확인하여 백금주석입자가 재분산되는 것을 알 수 있었다. 이러한 산소처리에 의한 재분산으로 인해 촉 매활성이 회복된다는 것을 알 수 있었고, 백금보다 백금주석 촉매의 활성회복률이 더 높았다.

Redispersion of Pt-Sn particles in Pt, PtSn catalyst which have been sintered by high temperature hydrogen reduction was investigated using oxygen treatment with various temperatures. The aim of this study was to understand the relationship between the catalytic activity for propane dehydrogenation reaction and the change in the physicochemical properties of the catalyst. X-ray diffraction analysis (XRD), CO pulse chemisorption, and H2 temperature programmed reduction (H2-TPR) were performed to investigate the state of active metal and interactions between particles of redispersed catalyst. It was confirmed that the dispersion and particle size of platinum, the crystal phase of the catalyst, and the reduction behavior were changed according to the oxygen treatment. As for the catalytic activity in propane dehydrogeantion, sintered PtSn catalyst treated with oxygen at 500℃ showed best activity and recovery of initial activity. It was confirm that catalyst after oxygen treatment at 500℃ showed high dispersion of Pt and decreased particle size as the results of CO pulse chemisorption and XRD of catalyst, and thus the redispersion of PtSn particles in sintered catalyst was occurred. Catalytic activity was recovered due to redispersion using oxygen treatment, and the activity recovery of the PtSn catalyst was higher than that of Pt catalyst.

Dehydrogenation Catalyst Redispersion Propane Sintering Oxygen treatment PtSn

Bartholomew CH, Appl. Catal. A: Gen., 212, 17 (2001)
Argyle MD, Bartholomew CH, Catalysts, 5(1), 145 (2015)
Arteaga GJ, Anderson JA, Rohchester CH, J. Catal., 187(1), 219 (1999)
Hung CC, Yeh CY, Shih CC, Chang JR, Catalysts, 9(4), 362 (2019)
Arteaga GJ, Anderson JA, Becker SM, Rohchester CH, J. Mol. Catal. A-Chem., 145(1), 183 (1999)
Fiedorow RMJ, Wanke SE, J. Catal., 43, 34 (1976)
Fiedorow RMJ, Chahar BS, Wanke SE, J. Catal., 51, 193 (1978)
Lee TJ, Kim YG, J. Catal., 90, 279 (1984)
Li X, Pei C, Gong J, Chem., 7(7), 1755 (2021)
Sattler JJHB, Ruiz-Martinez J, Santillan-Jimenez E, Weckhuysen BM, Chem. Rev., 114, 10613 (2014)
Bhasin MM, McCain JH, Vora BV, Imai T, Pujadó PR, Appl. Catal. A: Gen., 221(1), 397 (2001)
Arteaga GJ, Anderson JA, Rohchester CH, J. Catal., 189(1), 195 (2000)
Arteaga GJ, Anderson JA, Rohchester CH, J. Catal., 184(1), 268 (1999)
Chong FK, Anderson JA, Becker SM, Rohchester CH, J. Catal., 190(1), 327 (2000)
Stagga SM, Querinib CA, Alvareza WE, Resasco DE, J. Catal., 168(1), 75 (1997)
Kim GH, Jung K, Kim W, Um B, Shin C, Oh K, Koh HL, Res. Chem. Intermed., 42, 351 (2016)
Choi YS, Oh K, Jung K, Kim W, Koh HL, Catalysts, 10, 898 (2020)
Tedeeva MA, Kustov AL, Pribytkov PV, Kapusttin GI, Leonov AV, Tkachenko OP, Tursunov OB, Evdokimenko N, Fuel, 313, 122698 (2022)
Liu Y, Zhang G, Wang J, Zhu J, Zhang X, Miller JT, Song C, Guo X, Chin. J. Catal., 42, 2225 (2021)
Sattler JJHB, Gonzalez-Jimenez ID, Luo L, Stears BA, Malek A, Barton DG, Kilos BA, Kaminsky MP, Angew. Chem.-Int. Edit.
Searles K, Siddiqi G, Safonova OV, Copéret C, Chem. Sci., 8(4), 2661 (2017)
Liu G, Zhao Z, Wu T, Zeng L, Gong J, ACS Catal., 6(8), 5207 (2016)
Wu Y, Han Z, Yam X, Lang W, Guo Y, Microporous Mesoporous Mater., 330, 111616 (2022)
Im JH, Choi MK, ACS. Catal., 6, 2819 (2016)
https://www.tkisrus.com/assets/pdf/brochures/en/tkis-star-en.pdf
Wang J, Chang X, Chen S, Sun G, Zhou X, Vovk E, Yang Y, Deng W, Zhao Z, Mu R, Pei C, Gong J, ACS. Catal., 11, 4401 (2021)
Anresa P, Gaune-Escarda M, Brosa JP, Hayerb E, J. Alloy. Compd., 280(1-2), 158 (1998)
Kuznetsov VI, Belyi AS, Yurchenko EN, Smolikov MD, Protasova MT, Zatolokina EV, Duplyakin VK, J. Catal., 99(1), 159 (1986)
Srinivasan R, Angelis RJD, Davis BH, Catal. Lett., 4, 303 (1990)
Tasbihi M, Feyzi F, Amlashi MA, Abdullah AZ, Mohamed AR, Fuel Process. Technol., 88, 883 (2007)
Llorca J, Delapiscina PR, Fierro JL, Sales J, Homs N, J. Catal., 156, 139 (1995)
Srinivasan R, Davis BH, Platin. Met. Rev., 36, 151 (1992)
Vu BK, Song MB, Ahn IY, Suh YW, Suh DJ, Kim W, Koh HL, Choi YG, Shin EW, Appl. Catal. A: Gen., 400, 25 (2011)
Vicerich MA, Benitez VM, Sanchez MA, Especel C, Epron F, Pieck CL, Can. J. Chem. Eng., 98(3), 749 (2020)
Kim SS, Choi SH, Lee SM, Hong SC, J. Ind. Eng. Chem., 18(1), 272 (2012)
He Z, Qian Q, Zhang Z, Meng Q, Zhou H, Jiang Z, Han B, Philos. Trans. R. Soc. Lond. Ser. A-Math. Phys. Eng. Sci., 373(2057), 20150006 (2015)
Mazzieri VA, Grau JM, Yori JC, Vera CR, Pieck CL, Appl. Catal. A: Gen., 354(1-2), 161 (2009)
Lee J, Jang EJ, Oh DG, Szanyi J, Kwak KH, J. Catal., 285, 204 (2020)
Bariås OA, Holmen A, Blekkan EA, J. Catal., 158, 1 (1996)