Surface engineering of Pd-based nanoparticles by gas treatment for oxygen reduction reaction

A. Anto Jeffery; Sang-Young Lee; Jiho Min; Youngjin Kim; Seunghyun Lee; Jin Hee Lee; Namgee Jung; Sung Jong Yoo

Korean Journal of Chemical Engineering, Vol.37, No.8, 1360-1364, August, 2020

DOI10.1007/s11814-020-0586-2 Export Citation

Surface engineering of Pd-based nanoparticles by gas treatment for oxygen reduction reaction

A. Anto Jeffery¹, Sang-Young Lee², Jiho Min¹, Youngjin Kim¹, Seunghyun Lee¹, Jin Hee Lee³, Namgee Jung^{1, †}, and Sung Jong Yoo^{4, 5, †}

¹Graduate School of Energy Science and Technology (GEST), Chungnam National University, 99 Daehak-ro, Yuseong-gu, Daejeon 34134, Korea
²The Environment Technology Institute, Research Division, Coway R&D Center, 1 Guanak-ro, Gwanak-gu, Seoul 08826, Korea
³Center for Environment & Sustainable Resources, Korea Research Institute of Chemical Technology, Daejeon 34114, Korea
⁴Center for Hydrogen·Fuel Cell Research, Korea Institute of Science and Technology (KIST), Seoul 02792, Korea
⁵Division of Energy & Environment Technology, KIST School, University of Science and Technology (UST), Seoul 02792, Korea

E-mail:,

In many catalyst systems, including fuel cell applications, control of the catalyst surface composition is important for improving activity since catalytic reactions occur only at the surface. However, it is very difficult to modify the surface composition without changing the morphology of metal nanoparticles. Herein, carbon-supported Pd3Au1 nanoparticles with uniform size and distribution are fabricated by tert-butylamine reduction method. Pd or Au surface segregation is induced by simply heating as-prepared Pd3Au1 nanoparticles under CO or Ar atmosphere, respectively. Especially, CO-induced Pd surface segregation allows the alloy nanoparticles to have a Pd-rich surface, which is attributed to the strong CO binding energy of Pd. To demonstrate the change in surface composition of Pd3Au1 alloy catalyst with the annealing gas species, the oxygen reduction reaction performance is investigated and consequently, Pd3Au1 catalyst with the highest number of surface Pd atoms indicates excellent catalytic activity. Therefore, the present work provides insights into the development of metal-based alloys with optimum structures and surface compositions for various catalytic systems.

Keywords:CO-induced Surface Segregation;Surface Composition;Metal Alloy;Catalyst;Oxygen Reduction Reaction

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[2] Lee SY, Jung N, Shin DY, Park HY, Ahn D, Kim HJ, Jang JH, Lim DH, Yoo SJ, Appl. Catal. B: Environ., 206, 666 (2017)

[3] Sharma M, Jung N, Yoo SJ, Chem. Mater., 30, 2 (2018)

[4] Gasteiger HA, Kocha SS, Sompalli B, Wagner FT, Appl. Catal. B: Environ., 56(1-2), 9 (2005)

[5] Sung H, Sharma M, Jang J, Lee SY, Choi MG, Lee K, Jung N, Nanoscale, 11, 5038 (2019)

[6] Sharma M, Jang JH, Shin DY, Kwon JA, Lim DH, Choi D, et al., Energy Environ. Sci., 12, 2200 (2019)

[7] Erikson H, Sarapuu A, Tammeveski K, Jose SG, Feliu JM, Electrochem. Commun., 13, 734 (2011)

[8] Arjona N, Guerra-Balcazar M, Ortiz-Frade L, Osorio-Monreal G, Alvarez-Contreras L, Ledesma-Garciab J, Arriaga LG, J. Mater. Chem. A, 1, 15524 (2013)

[9] Zhang L, Chang Q, Chen H, Shao M, Nano Energy, 29, 198 (2016)

[10] Lee SY, Jung N, Cho J, Park HY, Ryu J, Jang I, Kim HJ, et al., ACS Catal., 4, 2402 (2014)

[11] Han S, Chae GS, Lee JS, Korean J. Chem. Eng., 33(6), 1799 (2016)

[12] Liu Z, Fu G, Li J, Liu Z, Xu L, Sun D, Tang Y, Nano Res., 11, 4686 (2018)

[13] Ramos-Sanchez G, Yee-Madeira H, Solorza-Feria O, Int. J. Hydrog. Energy, 33(13), 3596 (2008)

[14] Ye HQ, Li YM, Chen JH, Sheng JL, Fu XZ, Sun R, Wong CP, J. Mater. Sci., 53(23), 15871 (2018)

[15] Gao F, Goodman DW, Chem. Soc. Rev., 41, 8009 (2012)

[16] Liu P, Nørskov JK, Phys. Chem. Chem. Phys., 3, 3814 (2001)

[17] Strasser P, Koh S, Anniyev T, Greeley J, More K, Yu C, Liu Z, et al., Nat. Chem., 2, 454 (2010)

[18] Singh AK, Xu Q, ChemCatChem., 5, 652 (2013)

[19] Kumar VS, Kummari S, Goud KY, Satyanarayana M, Gobi KV, Int. J. Hydrog. Energy, 45(1), 1018 (2020)

[20] Chen LY, Chen N, Hou Y, Wang ZC, Lv SH, Fujita T, Jiang JH, Hirata A, Chen MW, ACS Catal., 3, 1220 (2013)

[21] Erikson H, Sarapuu A, Kozlova J, Matisen L, Sammelselg V, Tammeveski K, Electrocatalysis, 6, 77 (2015)

[22] Kumar VS, Kummari S, Goud KY, Satyanarayana M, Gobi KV, Int. J. Hydrog. Energy, 45(1), 1018 (2020)

[23] Paalanen P, Weckhuysen BM, Sankar M, Catal. Sci. Technol., 3, 2869 (2013)

[24] Yin Z, Chi M, Zhu Q, Ma D, Sun J, Bao X, J. Mater. Chem. A, 1, 9157 (2013)

[25] Jiao W, Chen C, You W, Chen G, Xue S, Zhang J, Liu J, Feng Y, Wang P, Wang Y, Wen H, Che R, Appl. Catal. B: Environ., 262, 118298 (2020)

[26] Kumikov VK, Khokonov KB, J. Appl. Phys., 54, 1346 (1983)

[27] Mezey LZ, Giber J, Appl. Phys. A-Mater. Sci. Process., 35, 87 (1984)

[28] Zhang J, Jin H, Sullivan MB, Lim FCH, Wu P, Phys. Chem. Chem. Phys., 11, 1441 (2009)

[29] Greeley J, Mavrikakis M, Catal. Today, 111(1-2), 52 (2006)

[30] Patterson A, Phys. Rev., 56, 978 (1939)

[31] Nascente PAP, De castro SGC, Landers R, Kleiman GG, Phys. Rev. B, 43, 4659 (1991)

[32] Hoshi N, Kida K, Nakamura M, Nakada M, Osada K, J. Phys. Chem. B, 110(25), 12480 (2006)