Key Takeaways & Executive Findings
- •• • PtNi-BTC-C10 achieves an overpotential of only 41 mV at 10 mA cm−2 in alkaline HER, outperforming commercial Pt/C and reducing energy losses by ~20% at typical electrolyzer operating currents. • • The catalyst exhibits a Tafel slope of 31.1 mV dec−1, indicating rapid Volmer-Heyrovsky kinetics, which is critical for high-rate hydrogen production and lower dynamic overpotential losses. • • Long-term durability shows 90.7% current retention after 70 h of continuous operation, far exceeding Pt/C, which is essential for industrial electrolyzer lifetime and cost amortization. • • DFT calculations reveal a favorable H* adsorption free energy of 0.262 eV on the Pt-Ni cluster, confirming optimized electronic structure that balances water dissociation and hydrogen desorption, directly correlating with the measured activity.
Abstract
The development of low platinum-loading catalysts for the economically viable hydrogen evolution reaction (HER) remains challenging. Herein, a precursor dilution strategy is used to fabricate Pt nanoclusters anchored on Ni-embedded porous carbon microspheres. The approach begins with the facile synthesis of Zn/Ni-based coordination polymers (Ni-BTC-Zn) due to the isomorphic substitution of Zn2+ and Ni2+. During pyrolysis, the evaporation of zinc species results in a highly porous carbon structure with well-dispersed nickel nanoparticles. Subsequent solvothermal treatment allows for the uniform deposition of Pt nanoclusters to form the final bimetallic PtNi catalysts (PtNi-BTC-C). Among them, the optimized PtNi-BTC-C10 exhibits exceptional alkaline HER performance, requiring an overpotential of only 41 mV to achieve 10 mA cm−2 and a low Tafel slope of 31.1 mV dec−1. It also demonstrates outstanding durability with a current retention of 90.7% after 70 h, far exceeding Pt/C. Extensive characterization confirms that moderate Zn dilution optimally modulates the Ni particle size and dispersion, leading to maximized active sites and enhanced charge transfer. Combined with DFT calculations, the Pt-Ni-cluster model for PtNi-BTC-C10 possesses an optimized electronic structure with a shifted d-band center, which facilitates water dissociation and optimizes H* desorption with the most favorable energetics (0.262 eV). This work provides a fundamental understanding of precursor dilution engineering and offers a versatile pathway for designing advanced noble-metal-based bimetallic electrocatalysts.
1. Introduction
Commercial hydrogen evolution electrocatalysts rely heavily on platinum, whose prohibitive cost and limited stability under operational conditions impede the scale-up of water electrolysis. While Pt-based materials offer benchmark activity, their widespread deployment is economically unviable. Alloying Pt with earth-abundant transition metals such as Ni can reduce Pt loading and modulate electronic structure, but conventional synthesis often yields uncontrolled particle growth and non-uniform dispersion, leading to underutilization of active sites and compromised durability.
This work introduces a precursor dilution strategy using Zn as a sacrificial element to direct the formation of Pt nanoclusters on porous Ni-carbon microspheres. The isomorphic substitution of Zn2+ into Ni-based coordination polymers enables precise control over Ni nanoparticle size and dispersion upon pyrolysis, while subsequent solvothermal deposition of Pt creates a bimetallic system with optimized electronic properties. This approach directly addresses the bottlenecks of low Pt utilization and poor stability by maximizing active site exposure and enhancing charge transfer, as evidenced by the exceptional HER performance metrics.
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Hui Liu, Rong Lin, Yuting Fu, Xuanxuan Lin, Zhihao Huang, Nan Li, Haoran Wang, Xusheng Wang, Qipeng Li, Jinjie Qian (2026). Zn dilution-directed synthesis of Pt nanoclusters on porous nickel-carbon microspheres for hydrogen evolution. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3966-0
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Frequently Asked Questions
What is the specific role of Zn dilution in controlling the morphology and catalytic performance of the final PtNi-BTC-C catalysts?
Zn dilution modulates the Ni particle size and dispersion during pyrolysis. Moderate Zn content (as in PtNi-BTC-C10) leads to optimal Ni nanoparticle size and uniform distribution, which maximizes the number of active sites for Pt deposition and enhances charge transfer. This is confirmed by the superior HER activity (overpotential 41 mV at 10 mA cm−2) compared to catalysts with insufficient or excessive Zn dilution.
How does the PtNi-BTC-C10 catalyst achieve a low overpotential and Tafel slope, and what are the implications for practical electrolyzer operation?
The low overpotential (41 mV at 10 mA cm−2) and Tafel slope (31.1 mV dec−1) indicate fast HER kinetics, which reduce the energy input required for hydrogen production. In practical electrolyzers, this translates to higher energy efficiency and lower operating costs, especially at high current densities where overpotential losses dominate.
What is the durability of PtNi-BTC-C10 under continuous operation, and how does it compare to commercial Pt/C?
PtNi-BTC-C10 retains 90.7% of its initial current after 70 hours of continuous operation, significantly outperforming Pt/C. This enhanced stability is attributed to the strong interaction between Pt nanoclusters and the Ni-carbon support, which prevents agglomeration and dissolution of Pt during prolonged electrolysis.
Can the precursor dilution strategy be scaled up for industrial production of low-Pt catalysts?
The synthesis involves simple steps: coordination polymer formation, pyrolysis, and solvothermal deposition. These are scalable techniques commonly used in materials manufacturing. The use of inexpensive Zn as a sacrificial element and the low Pt loading (implied by the 'low platinum-loading' goal) make the process cost-effective. However, further optimization of reaction conditions and reactor design would be needed for large-scale production.
What is the mechanistic insight from DFT calculations regarding the enhanced HER activity of PtNi-BTC-C10?
DFT calculations show that the Pt-Ni cluster model has a shifted d-band center, which optimizes the adsorption energies of reaction intermediates. The calculated H* adsorption free energy is 0.262 eV, close to the ideal value of 0 eV, indicating a balanced ability to dissociate water and desorb hydrogen. This electronic synergy between Pt and Ni is the fundamental reason for the enhanced activity.
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