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Open AccessDOI: 10.1007/s40820-025-01654-yOriginal Research

Transition Metal Carbonitride MXenes Anchored with Pt Sub-Nanometer Clusters to Achieve High-Performance Hydrogen Evolution Reaction at All pH Range

Zhihao Lei¹,Sajjad Ali¹,CI Sathish¹,Muhammad Ibrar Ahmed¹,Jiangtao Qu¹,Rongkun Zheng¹,Shibo Xi¹,Xiaojiang Yu¹,M. B. H. Breese¹,Chao Liu¹,Jizhen Zhang¹,Shuai Qi¹,Xinwei Guan¹,Vibin Perumalsamy¹,Mohammed Fawaz¹,Jae-Hun Yang¹,Mohamed Bououdina¹,Kazunari Domen¹,Ajayan Vinu¹,Liang Qiao¹,Jiabao Yi¹

Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia

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Transition Metal Carbonitride MXenes Anchored with Pt Sub-Nanometer Clusters to Achieve High-Performance Hydrogen Evolution Reaction at All pH Range
Graphical Abstract / Figure
Published In
Nano-Micro Letters
Published:January 31, 2025Edition:Vol. 17, Issue 123 • pp. 1-15Citation:Zhihao Lei et al. (2025), Nano-Micro Letters
Impact FactorPeer-Reviewed Core
Source JournalNano-Micro Letters
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Keywords & Index Terms:MXeneHydrogen evolution reactionDensity functional theoryElectrocatalysis

Key Takeaways & Executive Findings

  • • Two-dimensional mono- and few-layered Ti3CNTx MXene nanosheets with extremely high nitrogen content were synthesized. • Better performance for hydrogen evolution reaction (HER) than Pt/C catalyst in acidic, neutral and alkaline solutions. • Exceptional performance of HER in both acidic and alkaline solutions. • A large current density (>500 mA cm−2) has been achieved for HER.
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Abstract

Transition metal carbides, known as MXenes, particularly Ti3C2Tx, have been extensively explored as promising materials for electrochemical reactions. However, transition metal carbonitride MXenes with high nitrogen content for electrochemical reactions are rarely reported. In this work, transition metal carbonitride MXenes incorporated with Pt-based electrocatalysts, ranging from single atoms to sub-nanometer dimensions, are explored for hydrogen evolution reaction (HER). The fabricated Pt clusters/MXene catalyst exhibits superior HER performance compared to the single-atom-incorporated MXene and commercial Pt/C catalyst in both acidic and alkaline electrolytes. The optimized sample shows low overpotentials of 28, 65, and 154 mV at current densities of 10, 100, and 500 mA cm−2, a small Tafel slope of 29 mV dec−1, a high mass activity of 1203 mA mgPt−1 and an excellent turnover frequency of 6.1 s−1 in the acidic electrolyte. Density functional theory calculations indicate that this high performance can be attributed to the enhanced active sites, increased surface functional groups, faster charge transfer dynamics, and stronger electronic interaction between Pt and MXene, resulting in optimized hydrogen absorption/desorption toward better HER. This work demonstrates that MXenes with a high content of nitrogen may be promising candidates for various catalytic reactions by incorporating single atoms or clusters.

1. Introduction

The persistent and intensifying climate issues, the ever-growing depletion of fossil fuels, and the massive greenhouse gas emissions demand the development of green and clean energy to maintain a healthy and sustainable living environment. Hydrogen energy, which can be obtained from water, is one of the most promising candidates. In contrast, the efficiency of hydrogen production remains very low, and the associated cost is still pretty high. Therefore, searching for suitable catalysts to achieve a high hydrogen production rate is in demand.

Currently, platinum (Pt) is the benchmark catalyst for the hydrogen evolution reaction (HER). Traditional Pt-based catalysts have limited atom utilization efficiency, as only a small fraction of Pt atoms is actively involved in catalysis. Moreover, the scarcity and high cost of Pt limit its viability as a long-term and sustainable choice. To realize both high efficiency and maximum atom utilization, rational catalyst design strategies like reducing the dosage and size of Pt are considered promising ways to overcome the dilemma. However, when Pt is downsized to sub-nanometer clusters or single atoms, it is extremely important to search for suitable substrates to accommodate them with strong interactions to avoid surface diffusion and coarsening under applied bias. This could improve the intrinsic activity and stability of the active site, which is a key factor in HER performance.

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Cite This Research Paper
Zhihao Lei, Sajjad Ali, CI Sathish, Muhammad Ibrar Ahmed, Jiangtao Qu, Rongkun Zheng, Shibo Xi, Xiaojiang Yu, M. B. H. Breese, Chao Liu, Jizhen Zhang, Shuai Qi, Xinwei Guan, Vibin Perumalsamy, Mohammed Fawaz, Jae-Hun Yang, Mohamed Bououdina, Kazunari Domen, Ajayan Vinu, Liang Qiao, Jiabao Yi (2025). Transition Metal Carbonitride MXenes Anchored with Pt Sub-Nanometer Clusters to Achieve High-Performance Hydrogen Evolution Reaction at All pH Range. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01654-y
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Frequently Asked Questions

What is the main achievement of this research?

The research demonstrates that transition metal carbonitride MXenes (Ti3CNTx) with high nitrogen content, when anchored with Pt sub-nanometer clusters, exhibit superior hydrogen evolution reaction (HER) performance compared to commercial Pt/C catalysts across acidic, neutral, and alkaline conditions, achieving low overpotentials and high current densities.

How does the Pt clusters/MXene catalyst compare to single-atom catalysts?

The Pt clusters/MXene catalyst outperforms the single-atom-incorporated MXene and commercial Pt/C in both acidic and alkaline electrolytes, showing lower overpotentials, smaller Tafel slope, higher mass activity, and excellent turnover frequency.

What are the key factors contributing to the high HER performance?

Density functional theory calculations attribute the high performance to enhanced active sites, increased surface functional groups, faster charge transfer dynamics, and stronger electronic interaction between Pt and MXene, leading to optimized hydrogen absorption/desorption.

What is the significance of high nitrogen content in MXenes?

High nitrogen content in MXenes is rarely reported and is shown to be beneficial for catalytic reactions, as it enhances the material's properties for HER, making these MXenes promising candidates for various catalytic applications.

What are the potential applications of this research?

The findings suggest that nitrogen-rich MXenes with Pt clusters could be used as efficient and cost-effective electrocatalysts for hydrogen production, contributing to sustainable energy technologies.

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