Interaction between Pd and Cu nanoparticles in bimetallic CuPdx nanoparticles and its impact on oxidation of 1,2-propanediol to aliphatic acids

doi:10.1016/j.cjche.2020.02.005

Chinese Journal of Chemical Engineering ›› 2020, Vol. 28 ›› Issue (4): 1085-1094.DOI: 10.1016/j.cjche.2020.02.005

• Catalysis, Kinetics and Reaction Engineering • Previous Articles Next Articles

Interaction between Pd and Cu nanoparticles in bimetallic CuPd_x nanoparticles and its impact on oxidation of 1,2-propanediol to aliphatic acids

Wei Tao, Aili Wang, Hengbo Yin

Faculty of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212000, China

Received:2019-09-03 Revised:2020-01-28 Online:2020-07-27 Published:2020-04-28
Contact: Aili Wang, Hengbo Yin
Supported by:
This work was financially supported by the Funding of Jiangsu Science and Technology Department, China (FZ20180919). We also sincerely thank Dr. Kangmin Chen for his helpful support on TEM and HRTEM analyses.

Interaction between Pd and Cu nanoparticles in bimetallic CuPd_x nanoparticles and its impact on oxidation of 1,2-propanediol to aliphatic acids

Wei Tao, Aili Wang, Hengbo Yin

Faculty of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212000, China

通讯作者: Aili Wang, Hengbo Yin
基金资助:
This work was financially supported by the Funding of Jiangsu Science and Technology Department, China (FZ20180919). We also sincerely thank Dr. Kangmin Chen for his helpful support on TEM and HRTEM analyses.

Abstract

Abstract: Bimetallic CuPd x nanoparticles synthesized by the wet chemical reduction method were used as the catalysts in the catalytic oxidation of 1,2-propanediol with gaseous oxygen to aliphatic acids. The palladium and copper nanoparticles in the bimetallic CuPd_x nanoparticles had an alloying trend. The catalytic activity of the palladium nanoparticles in the bimetallic CuPd_x nanoparticles was enhanced by the interaction between the palladium and copper nanoparticles. When the bimetallic CuPd₇ nanoparticles catalyzed the oxidation of 1,2-propanediol in an alkaline aqueous solution at 100 ℃ for 3 h, lactic, formic, and acetic acids were dominantly produced with the total selectivity of above 99% at the 1,2-propanediol conversion of 85.9%. The simulation of the reaction kinetic equation on the CuPd₇ catalyst showed that the reaction activation energy was 29.4 kJ·mol^-1, indicating that the bimetallic CuPd₇ nanoparticles had a high catalytic activity in the oxidation reaction between 1,2-propanediol and gaseous oxygen.

Key words: Bimetallic CuPdCuPd_x nanoparticles, 1,2-Propanediol, Aliphatic acids

摘要： Bimetallic CuPd x nanoparticles synthesized by the wet chemical reduction method were used as the catalysts in the catalytic oxidation of 1,2-propanediol with gaseous oxygen to aliphatic acids. The palladium and copper nanoparticles in the bimetallic CuPd_x nanoparticles had an alloying trend. The catalytic activity of the palladium nanoparticles in the bimetallic CuPd_x nanoparticles was enhanced by the interaction between the palladium and copper nanoparticles. When the bimetallic CuPd₇ nanoparticles catalyzed the oxidation of 1,2-propanediol in an alkaline aqueous solution at 100 ℃ for 3 h, lactic, formic, and acetic acids were dominantly produced with the total selectivity of above 99% at the 1,2-propanediol conversion of 85.9%. The simulation of the reaction kinetic equation on the CuPd₇ catalyst showed that the reaction activation energy was 29.4 kJ·mol^-1, indicating that the bimetallic CuPd₇ nanoparticles had a high catalytic activity in the oxidation reaction between 1,2-propanediol and gaseous oxygen.

关键词: Bimetallic CuPdCuPd_x nanoparticles, 1,2-Propanediol, Aliphatic acids

Wei Tao, Aili Wang, Hengbo Yin. Interaction between Pd and Cu nanoparticles in bimetallic CuPd_x nanoparticles and its impact on oxidation of 1,2-propanediol to aliphatic acids[J]. Chinese Journal of Chemical Engineering, 2020, 28(4): 1085-1094.

References

[1] C. Gao, C. Ma, P. Xu, Biotechnological routes based on lactic acid production from biomass, Biotechnol. Adv. 29(2011) 930-939.
[2] J. Sikder, S. Chakraborty, P. Pal, E. Drioli, C. Bhattacharjee, Purification of lactic acid from microfutrate fermention broth by cross-flow nanofiltration, Biochem. Eng. J. 69(2012) 130-137.
[3] T. Tsujino, T. Ohigashi, S. Sugiyama, K. Kawashiro, H. Hayashi, Oxidation of propylene glycol and lactic acid to pyruvic acid in aqueous phase catalyzed by leadmodified palladium-on-carbon and related systems, J. Mol. Catal. 71(1992) 25-35.
[4] H.H.C.M. Pinxt, B.F.M. Kuster, G.B. Marin, Promoter effects in the Pt-catalysed oxidation of propylene glycol, Appl. Catal. A. 191(2000) 45-54.
[5] L. Prati, M. Rossi, Gold on carbon as a new catalyst for selective liquid phase oxidation of diols, J. Catal. 176(1998) 552-560.
[6] H. Ma, X. Nie, J. Cai, C. Chen, J. Gao, H. Miao, J. Xu, Au/Mg(OH)2:Highly efficient for selective oxidation of 1,2-propanediol to lactic acid with molecular oxygen, Sci. China Chem. 53(2010) 1497-1501.
[7] Y. Ryabenkova, Q. He, P.J. Miedziak, N.F. Dummer, S.H. Taylor, A.F. Carley, D.J. Morgan, N. Dimitratos, D.J. Willock, D. Bethell, D.W. Knight, D. Chadwick, C.J. Kiely, G.J. Hutchings, The selective oxidation of 1,2-propanediol to lactic acid using mild conditions and gold-based nanoparticulate catalysts, Catal. Today 203(2013) 139-145.
[8] M.M. Dimos, G.J. Blanchard, Electro-catalytic oxidation of 1,2-propanediol at nanoporous and planar soil Pt electrodes, J. Electroanal. Chem. 654(2011) 13-19.
[9] Y. Feng, H. Yin, A. Wang, W. Xue, Selectively catalytic oxidation of 1,2-propanediol to lactic, formic, and acetic acids over Ag nanoparticles under mild reaction conditions, J. Catal. 326(2015) 26-37.
[10] W. Xue, H. Yin, Z. Lu, A. Wang, S. Liu, L. Shen, Selective oxidation of 1,2-propanediol to carboxylic acids catalyzed by copper nanoparticles, J. Nanosci. Nanotechnol. 18(2018) 3362-3372.
[11] Y. Ryabenkova, P.J. Miedziak, N.F. Dummer, S.H. Taylor, D.J. N, Dimitratos, D. Willock, D. Bethell, W. Knight, G Hutchings.J., The selective oxidation of 1,2-propanediol by supported gold-based nanoparticulate catalysts, Top Catal 55(2012) 1283-1288.
[12] Y. Feng, H. Yin, D. Gao, A. Wang, L. Shen, M. Meng, Selective oxidation of 1,2-propanediol to lactic acid catalyzed by hydroxylapatite nanorod-supported Au/Pd bimetallic nanoparticles under atmospheric pressure, J. Catal. 316(2014) 67-77.
[13] Y. Feng, H. Yin, A. Wang, D. Gao, X. Zhu, L. Shen, M. Meng, Selective oxidation of 1,2-propanediol to lactic acid catalyzed by nanosized Mg(OH)2-supported bimetallic Au-Pd catalysts, Appl. Catal. A. 482(2014) 49-60.
[14] N. Dimitratos, J.A. Lopez-Sanchez, G. Brett, N. Dummer, S. Meenakshisundaram, J.M. Anthonykutty, G. Brett, A.F. Carley, S.H. Taylor, D.W. Knight, G.J. Hutchings, Selective formation of lactate by oxidation of 1,2-propanediol using gold palladium alloy supported nanocrystals, Green Chem. 11(2009) 1209-1216.
[15] W. Xue, H. Yin, Z. Lu, Y. Feng, A. Wang, S. Liu, L. Shen, X. Jia, Catalytic oxidation of 1,2-propanediol over bimetallic Cu@Au core/shell nanoparticles, Catal. Lett. 146(2016) 1139-1152.
[16] L. Shen, X. Zhou, C. Zhang, H. Yin, A. Wang, C. Wang, Functional characterization of bimetallic CuPd x nanoparticles in hydrothermal conversion of glycerol to lactic acid, J. Food Biochem. 43(2019), e12931.
[17] H.X. Yin, C. Zhang, H. Yin, D. Gao, L. Shen, A. Wang, Hydrothermal conversion of glycerol to lactic acid catalyzed by Cu/hydroxyapatite, Cu/MgO, and Cu/ZrO₂ and reaction kinetics, Chem. Eng. J. 288(2016) 332-343.
[18] A. Wang, M. Zhang, H. Yin, S. Liu, M. Liu, T. Hu, Direct reaction between silicon and methanol over Cu-based catalysts:Investigation of active species and regeneration of CuCl catalyst, RSC Adv. 8(2018) 19317-19325.
[19] W.-L. Dai, Q. Sun, J.-F. Deng, D. Wu, Y.-H. Sun, XPS studies of Cu/ZnO/Al₂O₃ ultra-fine catalysts derived by a novel gel oxalate co-precipitation for methanol synthesis by CO₂+H₂, Appl. Surf. Sci. 177(2001) 172-179.
[20] C.L. Aravinda, P. Bera, V. Jayaram, A.K. Sharma, S.M. Mayanna, Characterization of electrochemically deposited Cu-Ni black coatings, Mater. Res. Bull. 37(2002) 397-405.
[21] K.L. Deutsch, B.H. Shanks, Hydrodeoxygenation of lignin model compounds over a copper chromite catalyst, Appl. Catal. A. 447-448(2012) 144-150.
[22] K. Sun, W. Lu, F. Qiu, S. Liu, X. Xu, Direct synthesis of DME over bifunctional catalyst:Surface properties and catalytic performance, Appl. Catal. A. 252(2003) 243-249.

Interaction between Pd and Cu nanoparticles in bimetallic CuPd_x nanoparticles and its impact on oxidation of 1,2-propanediol to aliphatic acids

Interaction between Pd and Cu nanoparticles in bimetallic CuPd_x nanoparticles and its impact on oxidation of 1,2-propanediol to aliphatic acids

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