ACS Publications. Most Trusted. Most Cited. Most Read
Revealing the Impact of Pulsed Laser-Produced Single-Pd Nanoparticles on a Bimetallic NiCo2O4 Electrocatalyst for Energy-Saving Hydrogen Production via Hybrid Water Electrolysis

OR SEARCH CITATIONS

My Activity
Publications

Figure 1Loading Img
Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Catal. 2024, 14, 5, 3320-3335
    Research Article

    Revealing the Impact of Pulsed Laser-Produced Single-Pd Nanoparticles on a Bimetallic NiCo2O4 Electrocatalyst for Energy-Saving Hydrogen Production via Hybrid Water Electrolysis
    Click to copy article linkArticle link copied!

    • Raja Arumugam Senthil
      Raja Arumugam Senthil
      Department of Chemistry (BK21 FOUR), Research Institute of Natural Sciences, Gyeongsang National University, Jinju 52828, Republic of Korea
      More by Raja Arumugam Senthil
    • Sieon Jung
      Sieon Jung
      Department of Chemistry (BK21 FOUR), Research Institute of Natural Sciences, Gyeongsang National University, Jinju 52828, Republic of Korea
      More by Sieon Jung
    • Ahreum Min
      Ahreum Min
      Core-Facility Center for Photochemistry & Nanomaterials, Gyeongsang National University, Jinju 52828, Republic of Korea
      More by Ahreum Min
    • Anuj Kumar
      Anuj Kumar
      Nano-Technology Research Laboratory, Department of Chemistry, GLA University, Mathura281406, Uttar Pradesh, India
      More by Anuj Kumar
      Orcidhttps://orcid.org/0000-0001-9374-6677
    • Cheol Joo Moon
      Cheol Joo Moon
      Core-Facility Center for Photochemistry & Nanomaterials, Gyeongsang National University, Jinju 52828, Republic of Korea
      More by Cheol Joo Moon
    • Monika Singh
      Monika Singh
      Nano-Technology Research Laboratory, Department of Chemistry, GLA University, Mathura281406, Uttar Pradesh, India
      More by Monika Singh
    • Myong Yong Choi*
      Myong Yong Choi
      Department of Chemistry (BK21 FOUR), Research Institute of Natural Sciences, Gyeongsang National University, Jinju 52828, Republic of Korea
      Core-Facility Center for Photochemistry & Nanomaterials, Gyeongsang National University, Jinju 52828, Republic of Korea
      *Email: [email protected]
      More by Myong Yong Choi
      Orcidhttps://orcid.org/0000-0001-5729-5418
    Other Access OptionsSupporting Information (1)

    ACS Catalysis

    Cite this: ACS Catal. 2024, 14, 5, 3320–3335
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acscatal.3c05051
    Published February 16, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

    Abstract

    Click to copy section linkSection link copied!
    Abstract Image

    Nowadays, the assembling of hybrid water electrolysis using a hydrazine oxidation reaction (HzOR) instead of a slow anodic oxygen evolution reaction (OER) has been established as a favorable technology for efficient hydrogen (H2) production. Nevertheless, it is still critical to develop highly effective bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and HzOR. In this work, we propose a facile approach for the design and synthesis of single-Pd-nanoparticles-decorated bimetallic NiCo2O4 nanoplates as a bifunctional electrocatalyst for both HER and HzOR. Initially, the NiCo2O4 nanoplates are synthesized by a combination of hydrothermal reaction and high-temperature calcination. Subsequently, single-Pd nanoparticles with varying proportions are decorated on NiCo2O4 nanoplates via facile pulsed laser irradiation (PLI), leading to the formation of Pd/NiCo2O4 composites. The optimized Pd/NiCo2O4 composite shows a remarkable electrocatalytic ability with a low overpotential of 294 mV for the HER and an ultrasmall working potential of −6 mV (vs RHE) for the HzOR at 10 mA cm–2 in a 1 M KOH electrolyte. Thus, an overall hydrazine splitting (OHzS) electrolyzer with the Pd/NiCo2O4∥Pd/NiCo2O4 system presents the current densities of 10 and 100 mA cm–2 at respective low cell voltages of 0.35 and 0.94 V. Notably, in situ/operando Raman spectroscopy confirms the surface formation of α-Co(OH)2 during the HER and γ-NiOOH during the HzOR. Furthermore, the density function theory (DFT) calculations demonstrate that the decoration of Pd onto NiCo2O4 facilitates the optimization of both the hydrogen adsorption free energy (ΔGH*) and enhancement of hydrazine dehydrogenation kinetics. This work introduces a facile strategy for fabricating bifunctional electrocatalysts, potentially useful in energy-saving H2 production.

    Copyright © 2024 American Chemical Society

    Subjects

    what are subjects

    Keywords

    what are keywords

    Read this article

    To access this article, please review the available access options below.

    Get instant access

    Purchase Access

    Read this article for 48 hours. Check out below using your ACS ID or as a guest.

    Recommended

    Access through Your Institution

    You may have access to this article through your institution.

    Your institution does not have access to this content. Add or change your institution or let them know you’d like them to include access.

    Supporting Information

    Click to copy section linkSection link copied!

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.3c05051.

    • Characterization techniques; electrochemical examinations; computational measurements; optical images of the samples (Figure S1); reaction vials (Figures S2 and S3); EDS spectrum (Figure S4); HR-TEM images (Figure S5); TEM-EDS mapping images (Figure S6); CV curves to determine TOF values (Figure S7); CV curves to calculate Cdl values (Figure S8); Cdl plots (Figure S9); ICP-OES results (Table S1); and comparison of the bifunctional activity of the Pd/NiCo2O4-2 composite (Table S2) (PDF)

    Terms & Conditions

    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    Click to copy section linkSection link copied!
    Citation Statements
    Explore this article's citation statements on scite.ai
    powered by  Scite

    This article is cited by 30 publications.

    1. Surajit Mondal, Supriti Dutta, Vishwadeepa Hazra, Swapan K. Pati, Sayan Bhattacharyya. Decoding the Hume–Rothery Rule in a Bifunctional Tetra-metallic Alloy for Alkaline Water Electrolysis. Nano Letters 2025, 25 (4) , 1296-1304. https://doi.org/10.1021/acs.nanolett.4c04412
    2. Siyu Chen, Li Jiang, Shuting Xu, Yumeng Yang, Guoying Wei. MOF-199-Derived C–Cu@Pd/Nanoporous Materials as Efficient Electrocatalysts for the Hydrogen Evolution Reaction. Crystal Growth & Design 2024, 24 (21) , 8748-8757. https://doi.org/10.1021/acs.cgd.4c00472
    3. Hao-Yu Wang, Sixiang Zhai, Hao Wang, Fengxiao Yan, Jin-Tao Ren, Lei Wang, Minglei Sun, Zhong-Yong Yuan. Taking Advantage of Potential Coincidence Region: Insights into Gas Production Behavior in Advanced Self-Activated Hydrazine-Assisted Alkaline Seawater Electrolysis. ACS Nano 2024, 18 (30) , 19682-19693. https://doi.org/10.1021/acsnano.4c04831
    4. Hyogyun Roh, Sehun Oh, Changhyun Lim, Kijung Yong. Recent Progress and Challenges in Hybrid Water Electrolysis through Economic Evaluation. ACS Materials Letters 2024, 6 (7) , 3080-3089. https://doi.org/10.1021/acsmaterialslett.4c00676
    5. Akash Prabhu Sundar Rajan, Raja Arumugam Senthil, Cheol Joo Moon, Anuj Kumar, Ahreum Min, Mohd Ubaidullah, Myong Yong Choi. Self‐Powered Hydrogen Production via Laser‐Coordinated NiCoPt Alloy Catalysts in an Integrated Zn‐Hydrazine Battery with Hydrazine Splitting. Small Methods 2025, 9 (3) https://doi.org/10.1002/smtd.202401709
    6. Cheol Joo Moon, Velusamy Maheskumar, Ahreum Min, Anuj Kumar, Seongbo Lee, Raja Arumugam Senthil, Mohd Ubaidullah, Myong Yong Choi. Laser‐Regulated Iridium‐Diffused Nitrogen–Carbon Sites for Enhanced Hydrazine‐Assisted Alkaline Seawater Splitting and Zinc–Hydrazine Batteries. Small 2025, 21 (8) https://doi.org/10.1002/smll.202408569
    7. Jinrui Hu, Xuan Wang, Yi Zhou, Meihan Liu, Caikang Wang, Meng Li, Heng Liu, Hao Li, Yawen Tang, Gengtao Fu. Asymmetric Rh–O–Co bridge sites enable superior bifunctional catalysis for hydrazine-assisted hydrogen production. Chemical Science 2025, 16 (4) , 1837-1848. https://doi.org/10.1039/D4SC07442D
    8. Kuan Deng, Xuesong Liu, Peng Liu, Xingbin Lv, Wen Tian, Junyi Ji. Enhanced Adsorption Kinetics and Capacity of a Stable CeF 3 @Ni 3 N Heterostructure for Methanol Electro‐Reforming Coupled with Hydrogen Production. Angewandte Chemie 2025, 137 (4) https://doi.org/10.1002/ange.202416763
    9. Kuan Deng, Xuesong Liu, Peng Liu, Xingbin Lv, Wen Tian, Junyi Ji. Enhanced Adsorption Kinetics and Capacity of a Stable CeF 3 @Ni 3 N Heterostructure for Methanol Electro‐Reforming Coupled with Hydrogen Production. Angewandte Chemie International Edition 2025, 64 (4) https://doi.org/10.1002/anie.202416763
    10. Xueyi Lu, Lulu Jia, Minchen Hou, Xuemin Wu, Chang Ni, Gaofei Xiao, Renzhi Ma, Xia Lu. Tunable heteroassembly of 2D CoNi LDH and Ti 3 C 2 nanosheets with enhanced electrocatalytic activity for oxygen evolution. Nanoscale 2025, 17 (2) , 1080-1091. https://doi.org/10.1039/D4NR03679D
    11. Premnath Kumar, Andreina García, Supareak Praserthdam, Piyasan Praserthdam. Self-assembled 3D-flowers of CoS2-MoS2@NGA grown on graphene aerogel: As an emerging reliable electrocatalyst for hydrogen production in alkaline and acidic medium. Journal of Alloys and Compounds 2025, 1010 , 177618. https://doi.org/10.1016/j.jallcom.2024.177618
    12. Rui Bai, Yuelong Liu, Yicheng Zhang, Yingtang Zhou, Haibo Zhang, Yan Zhao, Xue Zhao. Surface crystallized supramolecular to achieve highly dispersed ultrafine nano-palladium in-situ deposition to promote thermal/electrocatalytic reduction. Journal of Colloid and Interface Science 2025, 677 , 1-11. https://doi.org/10.1016/j.jcis.2024.07.222
    13. Xingxing Zhu, Zhengtong Ji, Wubin Wan, Yongfu Zhu, Xingyou Lang, Qing Jiang. Vacancy-rich heterogeneous MnCo2O4.5@NiS electrocatalyst for highly efficient overall water splitting. Journal of Colloid and Interface Science 2025, 678 , 878-884. https://doi.org/10.1016/j.jcis.2024.09.005
    14. Xianyou Luo, Bokai Cao, Muhammad Fayaz, Wende Lai, Baodong Du, Heng Zheng, Xunhui Xiong, Yong Chen. Enhancing effects of edge-N in Pt-based carbon support on hydrogen evolution reaction. Surfaces and Interfaces 2025, 56 , 105499. https://doi.org/10.1016/j.surfin.2024.105499
    15. Ming-Lei Sun, Hao-Yu Wang, Yi Feng, Jin-Tao Ren, Lei Wang, Zhong-Yong Yuan. Electrodegradation of nitrogenous pollutants in sewage: from reaction fundamentals to energy valorization applications. Chemical Society Reviews 2024, 53 (24) , 11908-11966. https://doi.org/10.1039/D4CS00517A
    16. Junhao Wu, Xiao Zhang, Sijia Ren, Xinhui Lu, Jiaxin Yang, Kui Li. Employing a MoO 2 @NiO heterojunction as a highly selective and efficient electrochemical ethanol-to-acetaldehyde conversion catalyst. CrystEngComm 2024, 26 (47) , 6701-6706. https://doi.org/10.1039/D4CE01039F
    17. Neshanth Vadivel, Arun Prasad Murthy. Recent Developments in Membrane‐Free Hybrid Water Electrolysis for Low‐Cost Hydrogen Production Along with Value‐Added Products. Small 2024, 20 (52) https://doi.org/10.1002/smll.202407845
    18. Xueqing Gao, Yutong Chen, Yujun Wang, Luyao Zhao, Xingyuan Zhao, Juan Du, Haixia Wu, Aibing Chen. Next-Generation Green Hydrogen: Progress and Perspective from Electricity, Catalyst to Electrolyte in Electrocatalytic Water Splitting. Nano-Micro Letters 2024, 16 (1) https://doi.org/10.1007/s40820-024-01424-2
    19. Akash Prabhu Sundar Rajan, Raja Arumugam Senthil, Cheol Joo Moon, Anuj Kumar, Ahreum Min, Mohd Ubaidullah, Myong Yong Choi. Insights into dual-functional catalytic activity of laser-driven CoGaIr-LDH nanosheets in water electrolysis for green hydrogen production via in-situ Raman and theoretical analyses. Chemical Engineering Journal 2024, 502 , 157848. https://doi.org/10.1016/j.cej.2024.157848
    20. Eunseo Lee, Younghee So, Sungwook Mhin. Laser-driven synthesis of functional materials for advanced energy applications: A short review. Journal of Crystal Growth 2024, 648 , 127925. https://doi.org/10.1016/j.jcrysgro.2024.127925
    21. Ahreum Min, Velusamy Maheskumar, Dong Hyeon Lee, Anuj Kumar, Cheol Joo Moon, Raja Arumugam Senthil, Myong Yong Choi. Assembly of low-voltage driven co-production of hydrogen and sulfur via Ru nanoclusters on metal-sulfur coordination: Insights from DFT calculations. Journal of Energy Chemistry 2024, 99 , 541-552. https://doi.org/10.1016/j.jechem.2024.08.002
    22. Hao‐Yu Wang, Fengxiao Yan, Hao Wang, Sixiang Zhai, Jin‐Tao Ren, Lei Wang, Minglei Sun, Zhong‐Yong Yuan. The Combination of Electronic Structure and Lattice Strain Engineering for Multi‐Powered Hydrazine‐Assisted Seawater Electrolysis System at High Current Densities. Advanced Energy Materials 2024, 14 (42) https://doi.org/10.1002/aenm.202402611
    23. Kotesh Kumar Mandari, Younghwan Im, Misook Kang. NiCo-LDH sheets and Ag3PO4 nanoparticles decorated on graphitic carbon nitride for efficient oxygen evolution reaction. Journal of Alloys and Compounds 2024, 1004 , 175860. https://doi.org/10.1016/j.jallcom.2024.175860
    24. Sagyntay Sarsenov, Raja Arumugam Senthil, Ahreum Min, Anuj Kumar, Cheol Joo Moon, Juhyeon Park, Myong Yong Choi. Deciphering the Electronic Coupling Dynamics of Laser‐induced Ru/Cu Electrocatalyst for Dual‐Side Hydrogen Production and Formic Acid Co‐synthesis via DFT Analysis. Small 2024, 57 https://doi.org/10.1002/smll.202403999
    25. Ehtisham Umar, Muhammad Arslan Sunny, Haseebul Hassan, M. Waqas Iqbal, Rimsha Anwar, Norah Salem Alsaiari, Mohamed Ouladsmane, N. A. Ismayilova, Ehsan Elahi, Yazen M. Alawaideh. Hybrid Design Using Metal–Organic Framework MIL-101(Cr) with Melaminium Bis (Hydrogenoxalate) (MOX) for Hybrid Supercapacitors and Hydrogen Evolution Reactions. Journal of Inorganic and Organometallic Polymers and Materials 2024, 7 https://doi.org/10.1007/s10904-024-03413-9
    26. Premnath Kumar, Andreina García, Supareak Praserthdam, Piyasan Praserthdam. A comprehensive review and perspective of recent research developments, and accomplishments on structural-based catalysts; 1D, 2D, and 3D nanostructured electrocatalysts for hydrogen energy production. International Journal of Hydrogen Energy 2024, 88 , 638-657. https://doi.org/10.1016/j.ijhydene.2024.09.265
    27. Donglian Li, Xuerong Xu, Junzheng Jiang, Hao Dong, Hao Li, Xiang Peng, Paul K. Chu. Coupled electrocatalytic hydrogen production. Materials Science and Engineering: R: Reports 2024, 160 , 100829. https://doi.org/10.1016/j.mser.2024.100829
    28. Nezar H. Khdary, Asmaa R. M. El-Gohary, Ahmed Galal, Ahmed M. Alhassan, Sami D. Alzahrain. Cu-P@silica-CNT-based catalyst for effective electrolytic water splitting in an alkaline medium with hydrazine assistance. RSC Advances 2024, 14 (35) , 25830-25843. https://doi.org/10.1039/D4RA03998J
    29. Talshyn Begildayeva, Jayaraman Theerthagiri, Wanwisa Limphirat, Ahreum Min, Soorathep Kheawhom, Myong Yong Choi. Deciphering Indirect Nitrite Reduction to Ammonia in High‐Entropy Electrocatalysts Using In Situ Raman and X‐ray Absorption Spectroscopies. Small 2024, 20 (29) https://doi.org/10.1002/smll.202400538
    30. Ruihong Guo, Yujuan Zhang, Xiutang Zhang, Hong Yang, Tuoping Hu. Synthesis of Co0·52Cu0·48/Cu@S–C arrays for the enhanced performance of hydrazine-assisted hydrogen production. International Journal of Hydrogen Energy 2024, 68 , 472-480. https://doi.org/10.1016/j.ijhydene.2024.04.180
    31. Xingxing Zhu, Zhengtong Ji, Wubin Wan, YongFu Zhu, Qing Jiang. Vacancy-Rich Heterogeneous Mnco2o4.5@Nis Electrocatalysts for Highly Efficient Overall Water Splitting. 2024https://doi.org/10.2139/ssrn.4848432
    Download PDF
    Go to ACS Catalysis
    Get e-Alerts
    Get e-Alerts

    ACS Catalysis

    Cite this: ACS Catal. 2024, 14, 5, 3320–3335
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acscatal.3c05051
    Published February 16, 2024
    Copyright © 2024 American Chemical Society
    Request reuse permissions

    Article Views

    1785

    Altmetric

    -

    Citations

    30
    Learn about these metrics

    Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.

    Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.

    The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.