A DFT Study on Palladium-Based Bimetallic Catalysts for Direct Synthesis of Hydrogen Peroxide: Core-Shell Approach for Enhanced Selectivity

Mawan Nugraha; Meng-Che Tsai; Susiani Susiani; Suratni Suratni; Wei-Nien Su; Bing Joe Hwang

doi:10.22146/ijc.104066

A DFT Study on Palladium-Based Bimetallic Catalysts for Direct Synthesis of Hydrogen Peroxide: Core-Shell Approach for Enhanced Selectivity

https://doi.org/10.22146/ijc.104066

Mawan Nugraha^(1*), Meng-Che Tsai⁽²⁾, Susiani Susiani⁽³⁾, Suratni Suratni⁽⁴⁾, Wei-Nien Su⁽⁵⁾, Bing Joe Hwang⁽⁶⁾

(1) Department of Industrial Engineering, Politeknik Negeri Media Kreatif, Jl. Srengseng Sawah, Jagakarsa, Jakarta 12640, Indonesia
(2) Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, No. 43, Sec. 4, Keelung Rd., Da'an Dist., Taipei City 106335, Taiwan
(3) Department of Industrial Engineering, Politeknik Negeri Media Kreatif, Jl. Srengseng Sawah, Jagakarsa, Jakarta 12640, Indonesia
(4) Department of Publishing, Politeknik Negeri Media Kreatif, Jl. Srengsengsawah, Jagakarsa, Jakarta 12640, Indonesia
(5) Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, No. 43, Sec. 4, Keelung Rd., Da'an Dist., Taipei City 106335, Taiwan
(6) Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, No. 43, Sec. 4, Keelung Rd., Da'an Dist., Taipei City 106335, Taiwan; Department of Chemical Engineering, Graduate Institute of Applied Science and Technology, National Taiwan University of Science and Technology, No. 43, Sec. 4, Keelung Rd., Da'an Dist., Taipei City 106335, Taiwan; National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan
(*) Corresponding Author

Abstract

Pd-Au alloy is one of the most researched catalysts for directly synthesizing hydrogen peroxide (DSHP). To overcome the limitations of natural resources, one challenge is to design an alternative catalyst composed of abundant, cheap elements that can be prepared via a cleaner process and exhibit better selectivity than Pd-Au. Using DFT-based analysis, we investigated Pd-based core-shell catalysts, where Pd is the shell and the core is selected from the Ag, Cd, Pt, Au, Hg, Ni, Cu, and Zn group. The descriptors of selectivity (OOH versus O adsorption energies) and reaction rate (O₂ versus O adsorption energies) were used to search for a better catalyst. Strong OOH and weaker O adsorption energy characterize the better catalytic selectivity. The stronger adsorption energy of OOH compared to O, the better formation of H₂O₂. The stronger O adsorption energy compared to OOH, the more likely the formation of H₂O is to occur instead of H₂O₂. We also studied the geometric descriptor, represented by surface elasticity and distortion, by calculating the root-mean-square dislocation when the surface adsorbs O species. We have identified a promising new catalyst, Ni₆@Pd₃₂, for the direct synthesis of H₂O₂.

Keywords

palladium-based; bimetallic catalysts; hydrogen peroxide direct synthesis; DFT study

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DOI: https://doi.org/10.22146/ijc.104066