Enhanced Catalytic Performance via Ultrasonication-Plasma Synergy in PtGaPCoOx Catalysts Under Mild Conditions

Wail Al Zoubi , Yujun Sheng , Mohammad R. Thalji , Bassem Assfour , Stefano Leoni , Abdullah Al Mahmud , Jee-Hyun Kang , Abdul Wahab Allaf , Young Gun Ko

SusMat ›› 2025, Vol. 5 ›› Issue (5) : e70029

PDF
SusMat ›› 2025, Vol. 5 ›› Issue (5) : e70029 DOI: 10.1002/sus2.70029
RESEARCH ARTICLE

Enhanced Catalytic Performance via Ultrasonication-Plasma Synergy in PtGaPCoOx Catalysts Under Mild Conditions

Author information +
History +
PDF

Abstract

The synergistic effect of bi-component support catalysts via facile synthesis remains a pivotal challenge in catalysis, particularly under mild conditions. Therefore, this study reports an ultrasonication-plasma strategy to produce a PtGaPCoCoO@TiOx site catalyst encapsulated within a high-entropy alloy framework. This approach harnesses instantaneous high-temperature plasma generated using an electrical field and ultrasonication under ambient conditions in H2O. This study also elucidates the origin of the bifunctional effect in high-loading, ultra-stable, and ultra-fine PtGaPCoCoO catalysts, which are coated with a reducible TiOx layer, thereby achieving optimal catalytic activity and hydrogen evolution reaction (HER) performance. PtGaPCo intimacy in PtGaPCoCoO@TiOx is tuned and distributed on the porous titania coating based on strong metal–support interactions by leveraging the instantaneous high-energy input from plasma discharge and ultrasonication under ambient conditions in H2O. PtGaPCoCoO@TiOx exhibits remarkable selectivity and durability in the hydrogenation of 3-nitrophenylacetylene, even after 25 cycles with high conversion rates, significantly outperforming comparative catalysts lacking the ultrasonication plasma treatment and other reported catalysts. Furthermore, the catalyst exhibits exceptional HER activity, demonstrated by an overpotential of 187 mV at a current density of 10 mA cm−2 and a Tafel slope of 152 mV dec−1. This enhancement can be attributed to an increased electron density on the Pt surface within the PtGaPCo alloy. These findings highlight the potential of achieving synergistic chemical interactions among active metal sites in stable, industry-applicable catalysts.

Keywords

bi-components / catalysts / hydrogen evolution / metals / plasma / ultrasonic

Cite this article

Download citation ▾
Wail Al Zoubi, Yujun Sheng, Mohammad R. Thalji, Bassem Assfour, Stefano Leoni, Abdullah Al Mahmud, Jee-Hyun Kang, Abdul Wahab Allaf, Young Gun Ko. Enhanced Catalytic Performance via Ultrasonication-Plasma Synergy in PtGaPCoOx Catalysts Under Mild Conditions. SusMat, 2025, 5(5): e70029 DOI:10.1002/sus2.70029

登录浏览全文

4963

注册一个新账户 忘记密码

References

[1]

J. Zhang, Z. Gao, S. Wang, et al., “Origin of Synergistic Effects in Bicomponent Cobalt Oxide-Platinum Catalysts for Selective Hydrogenation Reaction,” Nature Communications 10, no. 1 (2019): 4166.

[2]

W. Al Zoubi, Y. Sheng, I. Hussain, et al., “Synthesis and machine learning prediction of high entropy multi-pronciple element nanoparticles,” Small 21, no. 22 (2025): 2501444.

[3]

N. M. Briggs, L. Barrett, E. C. Wegener, et al., “Identification of Active Sites on Supported Metal Catalysts With Carbon Nanotube Hydrogen Highways,” Nature Communications 9, no. 1 (2018): 3827.

[4]

T. N. Phaahlamohlaka, D. O. Kumi, M. W. Dlamini, et al., “Effects of Co and Ru Intimacy in Fischer-Tropsch Catalysts Using Hollow Carbon Sphere Supports: Assessment of the Hydrogen Spillover Processes,” ACS Catalysis 7, no. 3 (2017): 1568-1578.

[5]

W. Karim, C. Spreafico, A. Kleibert, et al., “Catalyst Support Effects on Hydrogen Spillover,” Nature 541, no. 7635 (2017): 68-71.

[6]

Z. Li, M. Zhang, X. Dong, et al., “Strong Electronic Interaction of Indium Oxide With Palladium Single Atoms Induced by Quenching Toward Enhanced Hydrogenation of Nitrobenzene,” Applied Catalysis B: Environmental 313 (2022): 121462.

[7]

Z. Wu, B. C. Bukowski, Z. Li, et al., “Changes in Catalytic and Adsorptive Properties of 2 Nm Pt3Mn Nanoparticles by Subsurface Atoms,” Journal of the American Chemical Society 140, no. 44 (2018): 14870-14877.

[8]

W. Cai, R. Mu, S. Zha, et al., “Subsurface Catalysis-Mediated Selectivity of Dehydrogenation Reaction,” Science Advances 4, no. 8 (2018): 541.

[9]

Y. Wang, H. Li, S. Di, et al., “Constructing Long-Cycling Crystalline C3N4-Based Carbonaceous Anodes for Sodium-Ion Battery via Nconfiguration Control,” Carbon Energy 6, no. 1 (2023): 388.

[10]

W. Al Zoubi, A. W. Allaf, B. Assfour, and Y. G. Ko, “Concurrent Oxidation-Reduction Reactions in a Single System Using a Low-Plasma Phenomenon: Excellent Catalytic Performance and Stability in the Hydrogenation Reaction,” ACS Appl Mater Interfaces 14, no. 5 (2022): 6740-6753.

[11]

K. Kusada, M. Mukoyoshi, D. Wu, and H. Kitagawa, “Chemical Synthesis, Characterization, and Properties of Multielement Nanoparticles,” Angewandte Chemie International Edition 61, no. 48 (2022): 20229616.

[12]

M. Cui, C. Yang, S. Hwang, et al., “Multi-principal Elemental Intermetallic Nanoparticles Synthesized via a Disorder-to-Order Transition,” Science Advances 8, no. 4 (2022): eabm4322.

[13]

Y. S. Yoon, P. Basumatary, M. E. Kilic, et al., “Novel GaPtMnP Alloy Based Anodic Electrocatalyst With Excellent Catalytic Features for Direct Ethanol Fuel Cells,” Advanced Functional Materials 32, no. 27 (2022): 2111272.

[14]

M. Bertram, C. Prossl, M. Ronovsky, et al., “Cobalt Oxide-Supported Pt Electrocatalysts: Intimate Correlation Between Particle Size, Electronic Metal-Support Interaction and Stability,” Journal of Physical Chemistry Letters 11, no. 19 (2020): 8365-8371.

[15]

Y. Tong, P. Chen, T. Zhou, et al., “A Bifunctional Hybrid Electrocatalyst for Oxygen Reduction and Evolution: Cobalt Oxide Nanoparticles Strongly Coupled to B,N-Decorated Graphene,” Angewandte Chemie International Edition 56, no. 25 (2017): 7121-7125.

[16]

Z. Yan, L. Zhao, Y. Liang, et al., “Two-in-one Shell Configurationfor Bimetal Selenides Toward Fast Sodium Storage Withinbroadened Voltage Windows,” Carbon Energy 4, no. 4 (2022): 586-597.

[17]

B. P. Vinayan and .R. S. Platinum-TM, “(Co) Alloy Nanoparticles Dispersed Nitrogen Doped (Reduced Graphene Oxide-Multiwalled Carbon Nanotube) Hybrid Structure Cathode Electrocatalysts for High Performance PEMFC Applications,” NanoScale 5, no. 11 (2013): 5019-5118.

[18]

M. Melchionna, S. Marchesan, M. Prato, and P. Fornasiero, “Carbon Nanotubes and Catalysis: The Many Facets of a Successful Marriage,” Catalysis Science and Technology 5, no. 8 (2015): 3859-3875.

[19]

K. Deng, Y. Xu, D. Yang, et al., “Pt-Ni-P Nanocages With Surface Porosity as Efficient Bifunctional Electrocatalysts for Oxygen Reduction and Methanol Oxidation,” Journal of Materials Chemistry A 7, no. 16 (2019): 9791-9797.

[20]

B. You, X. Liu, X. Liu, and Y. Sun, “Efficient H2 Evolution Coupled With Oxidative Refining of Alcohols via a Hierarchically Porous Nickel Bifunctional Electrocatalyst,” ACS Catalysis 7, no. 7 (2017): 4564-4570.

[21]

Y. Ren, C. H. Q. Chang, N. Li, J. Yang, and S. Hu, “Boosting Chemoselective Reduction of 4-nitrostyrene via Photoinduced Energetic Electrons From in Situ Formed Cu Nanoparticles on Carbon Dots,” Green Chemistry 23, no. 8 (2021): 2938-2943.

[22]

Y. Tan, X. Y. Liu, L. Li, L. Kang, A. Wang, and T. Zhang, “Effects of Divalent Metal Ions of Hydrotalcites on Catalytic Behavior of Supported Gold Nanocatalysts for Chemoselective Hydrogenation of 3-Nitrostyrene,” Journal of Catalysis 364 (2018): 174-182.

[23]

Y. Ji, T. Fan, and Y. Luo, “First-Principles Study on the Mechanism of Photocatalytic Reduction of Nitrobenzene on the Rutile TiO2(110) Surface,” Physical Chemistry Chemical Physics 22, no. 3 (2020): 1187.

[24]

R. Gao, L. Pan, H. Wang, et al., “Breaking Trade-off Between Selectivity and Activity of Nickel-Based Hydrogenation Catalysts by Tuning Both Steric Effect and D-Band Center,” Advancement of Science 9, no. 10 (2019): 1900054.

[25]

Y. Sheng, Y. Liu, L. Yin, et al., “Rh Promotional Effects on Pt-Rh Alloy Catalysts for Chemoselective Hydrogenation of Nitrobenzene to p-Aminophenol,” Chemical Engineering Journal 452 (2023): 139448.

[26]

Z. Li, X. Dong, S. Ji, et al., “Strong Electronic Interaction of Indium Oxide With Palladium Single Atoms Induced by Quenching Toward Enhanced Hydrogenation of Nitrobenzene,” Applied Catalysis B: Environment and Energy 313 (2022): 121462.

[27]

A. Han, J. Zhang, W. Sun, et al., “Isolating Contiguous Pt Atoms and Forming Pt-Zn Intermetallic Nanoparticles to Regulate Selectivity in 4-Nitrophenylacetylene Hydrogenation,” Nature Communications 10, no. 1 (2019): 3787.

[28]

J. Guo, F. Feng, S. Zhao, et al., “High FeLS(C) Electrochemicalactivity of an Iron Hexacyanoferrate Cathode Boosts Superiorsodium Ion Storage,” Carbon Energy 5, no. 5 (2023): 314.

[29]

J. Zhang, X. Qu, Y. Han, et al., “Engineering PtRu Bimetallic Nanoparticles With Adjustable Alloying Degree for Methanol Electro-Oxidation: Enhanced Catalytic Performance,” Applied Catalysis B: Environmental 263 (2020): 118345.

[30]

F. Bao, E. Keppainen, I. Dorbandt, et al., “Understanding the Hydrogen Evolution Reaction Kinetics of Electrodeposited Nickel-Moly-Molybdenum in Acidic, Near-Neutral, and Alkaline Conditions,” ChemElectroChem 8, no. 1 (2021): 195-208.

[31]

H. Du, R. M. Kong, X. Guo, F. Qu, and J. Li, “Recent Progress in Transition Metal Phosphides With Enhanced Electrocatalysis for Hydrogen Evolution,” Nanoscale 10, no. 46 (2018): 21617-21624.

[32]

M. R. Kandel, U. N. Pan, D. R. Paudel, P. P. Dhakal, N. H. Kim, and J. H. Lee, “Hybridized Bimetallic Phosphides of Ni-Mo, Co-Mo, and Co-Ni in a Single Ultrathin-3D-Nanosheets for Efficient HER and OER in Alkaline media,” Composites Part B: Engineering 239 (2022): 109992.

[33]

L. Yu, J. Zhang, Y. Dang, et al., “In Situ Growth of Ni2P-Cu3P Bimetallic Phosphide With Bicontinuous Structure on Self-Supported NiCuC Substrate as an Efficient Hydrogen Evolution Reaction Electrocatalyst,” ACS Catalysis 9, no. 8 (2019): 6919-6928.

[34]

X. Zhang, A. Wu, D. Wang, et al., “Fine-tune the Electronic Structure in Co-Mo Based Catalysts to Give Easily Coupled HER and OER Catalysts for Effective Water Splitting,” Applied Catalysis B: Environmental 328 (2023): 122474.

[35]

C. C. L. McCrory, S. Jung, J. C. Peters, and T. F. Jaramillo, “Benchmarking Heterogeneous Electrocatalysts for the Oxygen Evolution Reaction,” Journal of the American Chemical Society 135, no. 45 (2013): 16977-16987.

[36]

A. Manzoor, S. Pandey, D. Chakraborty, S. R. Phillpot, and S. Aidhy, “Entropy Contributions to Phase Stability in Binary Random Solid Solutions,” npj Computational Materials 4 (2018): 47.

[37]

Y. F. Ye, Q. Wang, J. Lu, C. T. Liu, and Y. Yang, “High-entropy Alloy: Challenges and Prospects,” Materials Today 19, no. 6 (2016): 349-362.

[38]

J. W. Yeh, S. K. Chen, S. J. Lin, et al., “Nanostructured High-entropy Alloys With Multiple Principal Elements: Novel Alloy Design Concepts and Outcomes,” Advanced Engineering Materials 6, no. 5 (2004): 299.

[39]

J. D. Chodera and D. L. Mobely, “Entropy-enthalpy Compensation: Role and Ramifications in Biomolecular Ligand Recognition and Design,” Annual Review of Biophysics 42, no. 1 (2013): 121-142.

[40]

X. Tang, G. B. Thompson, K. Ma, and C. R. Weinberger, “The Role of Entropy and Enthalpy in High Entropy Carbides,” Computation Materials Science 210 (2022): 111474.

[41]

W. Al Zoubi, B. Assfour, A. W. Allaf, S. Leoni, J. H. Kang, and Y. G. Ko, “Experimental and Theoretical Investigation of High-Entropy-Alloy/Support as a Catalyst for Reduction Reactions,” Journal of Energy Chemistry 81 (2023): 132-142.

[42]

W. Al Zoubi, R. A. K. Putri, M. R. Abukhadra, and Y. G. Ko, “Recent Experimental and Theoretical Advances in the Design and Science of High-Entropy Alloy Nanoparticles,” Nano Energy 110 (2023): 108362.

[43]

Y. Yao, Q. Dong, A. Brozena, et al., “High-Entropy Nanoparticles: Synthesis-Structure-Property Relationships and Data-Driven Discovery,” Science 376, no. 6589 (2022): 151.

[44]

W. Al Zoubi, A. Al Mahmud, and F. Hazmathulhaq, “Origin of the Synergistic Effects of Bimetallic Nanoparticles Coupled With a Metal Oxide Heterostructure for Accelerating Catalytic Performance,” SusMat 4, no. 3 (2024): 216.

[45]

W. Al Zoubi, S. Leoni, B. Assfor, et al., “Continuous Synthesis of Metal Oxde-supported High-entropy Alloy Nanoparticles With Remarkable Durability and Catalytic Activity in the Hydrogen Reduction,” InfoMat 7, no. 2 (2025): e212617.

[46]

W. Al Zoubi, Y. Sheng, I. Hussain, H. Seongjun, and N. Park, “Multi-Principal Element Nanoparticles: Synthesis Strategies and Machine Learning Prediction,” Coordination Chemistry Reviews 535 (2025): 216656.

[47]

A. Al Mahmud, A. H. Alshatteri, H. S. Alhasan, et al., “Copper-doped Strontium Metal-organic Frameworks: Dual Function Active Material for Supercapcitor and Oxygen Evolution Reaction,” Electrochimica Act 503 (2024): 144857.

RIGHTS & PERMISSIONS

2025 The Author(s). SusMat published by Sichuan University and John Wiley & Sons Australia, Ltd.

AI Summary AI Mindmap
PDF

75

Accesses

0

Citation

Detail

Sections
Recommended

AI思维导图

/