Key Takeaways & Executive Findings
- •• • Pt1-MoS2/hNCNC achieves an overpotential of 11 mV at 10 mA cm−2 and a mass activity of 5.6 A mgPt−1 at −20 mV in 0.5 M H2SO4, surpassing commercial Pt/C and enabling significant Pt loading reduction in PEMWE cathodes. • • In a PEMWE MEA with an ultralow Pt loading of 40 μg Pt cm−2, the catalyst delivers 0.5 A cm−2 at 1.55 V, 1.0 A cm−2 at 1.66 V, and 2.0 A cm−2 at 1.88 V, demonstrating industrial-level current densities at an order of magnitude lower Pt loading than commercial PEMWE. • • The MEA exhibits a mass activity of 31.3 A mgPt−1 at 1.7 V, exceeding the 25.0 A mgPt−1 of a commercial 20 wt% Pt/C-based MEA, which translates to higher Pt utilization efficiency and potential cost reduction. • • Durability testing at 1 A cm−2 shows a degradation rate of 40 μV h−1 over 500 h, outperforming Pt1/hNCNC (90 μV h−1) and commercial Pt/C (44 μV h−1), addressing the critical stability bottleneck for SACs in PEMWE.
Abstract
The activity and stability of single-atom catalysts (SACs) are intimately associated with the structure of supports. Herein, by employing a van der Waals (vdW) heterostructure support, we construct a highly active and durable Pt SAC for hydrogen evolution reaction (HER). The unique support consists of monolayer MoS2 attaching on hierarchical N-doped carbon nanocages (hNCNC), on which Pt presents as individual single atoms on the hNCNC and as island-like single-atom layers on the MoS2. The optimized Pt1-MoS2/hNCNC demonstrates low overpotential (11 mV at 10 mA cm−2) and high mass activity (5.6 A mgPt−1 at −20 mV) in 0.5 M H2SO4 solution, outperforming commercial Pt/C. Impressively, the Pt1-MoS2/hNCNC exhibits improved long-term stability in proton exchange membrane water electrolyzer relative to commercial Pt/C. The excellent HER performance is attributed to the regulated electronic structure, robust interaction of Pt atoms with MoS2/hNCNC and facilitated charge transfer. This study establishes an innovative strategy to develop a highly active and durable Pt SAC using vdW heterostructure supports.
1. Introduction
Proton exchange membrane water electrolysis (PEMWE) is a leading technology for renewable hydrogen production, but its reliance on noble metal catalysts, particularly Pt/C cathodes with typical loadings of 0.4–0.5 mg Pt cm−2, imposes prohibitive costs that hinder widespread deployment. Single-atom catalysts (SACs) offer a pathway to minimize Pt usage, yet their stability under industrial current densities remains inadequate. Prior Pt1/hNCNC catalysts, while achieving ultralow overpotentials, exhibited a voltage increase of 9 mV over 100 h, insufficient for long-term operation. The degradation stems from insufficient anchoring and electronic instability of Pt atoms on carbon supports.
This study introduces a van der Waals heterostructure support comprising monolayer MoS2 on hierarchical N-doped carbon nanocages (hNCNC) to anchor Pt single atoms. The heterostructure combines the high conductivity of hNCNC with the near-zero hydrogen adsorption free energy of MoS2, while the vdW interface regulates Pt electronic structure and strengthens metal-support interactions. The resulting Pt1-MoS2/hNCNC catalyst achieves an overpotential of 11 mV at 10 mA cm−2 and a mass activity of 5.6 A mgPt−1 at −20 mV in acid, and in a PEMWE MEA with 40 μg Pt cm−2, it delivers 1.0 A cm−2 at 1.66 V with a degradation rate of only 40 μV h−1 over 500 h, outperforming commercial Pt/C and addressing the stability bottleneck.
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HE Haohua, TIAN Jingyi, BAI Xue, MAO Chenghui, ZHANG Yan, ZHOU Changkai, PENG Xiang, YANG Lijun, WANG Xizhang, WU Qiang, HU Zheng (2025). Platinum single-atom catalysts anchored on van der Waals heterostructure support for durable hydrogen evolution. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3510-0
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Frequently Asked Questions
What is the degradation mechanism of Pt1-MoS2/hNCNC under prolonged PEMWE operation, and how does it compare to commercial Pt/C?
The Pt1-MoS2/hNCNC MEA exhibits a degradation rate of 40 μV h−1 over 500 h at 1 A cm−2, significantly lower than the 90 μV h−1 for Pt1/hNCNC and 44 μV h−1 for commercial Pt/C. The enhanced stability is attributed to the robust vdW heterostructure support, which prevents Pt agglomeration and dissolution through strong Pt-MoS2 interactions and efficient charge transfer, mitigating the typical degradation mechanisms of Ostwald ripening and carbon corrosion.
Can the Pt1-MoS2/hNCNC catalyst achieve cost parity with commercial Pt/C in PEMWE systems?
The MEA uses an ultralow Pt loading of 40 μg Pt cm−2, an order of magnitude lower than the 0.4–0.5 mg Pt cm−2 in commercial PEMWE. Combined with a mass activity of 31.3 A mgPt−1 at 1.7 V (vs. 25.0 A mgPt−1 for Pt/C), this reduces Pt consumption by ~90% while maintaining higher performance, directly lowering material costs. However, the synthesis cost of the vdW heterostructure support must be optimized for industrial-scale production to achieve overall cost parity.
What are the scalability challenges for synthesizing the Pt1-MoS2/hNCNC catalyst?
The synthesis involves precise control of monolayer MoS2 growth on hNCNC and atomic Pt deposition. While the current protocol yields high-performance catalysts, scaling up requires uniform MoS2 dispersion and Pt anchoring over large areas. The use of hNCNC as a conductive scaffold mitigates MoS2 restacking, but batch-to-batch reproducibility of the vdW heterostructure and Pt single-atom layers must be ensured. No pilot-scale data are reported, indicating a need for further engineering.
How does the vdW heterostructure support enhance the intrinsic activity of Pt single atoms?
The vdW heterostructure regulates the electronic structure of Pt atoms, as evidenced by the low overpotential of 11 mV at 10 mA cm−2 and high mass activity of 5.6 A mgPt−1 at −20 mV. The MoS2 component provides near-zero ΔGH* sites, while hNCNC ensures conductivity. Strong Pt-support interactions prevent agglomeration, and facilitated charge transfer at the heterointerface optimizes HER kinetics, as confirmed by the superior performance compared to Pt1/hNCNC.
What is the long-term durability of the Pt1-MoS2/hNCNC MEA under industrial current densities, and what are the failure modes?
At 1 A cm−2, the MEA maintains stable operation for 500 h with a degradation rate of 40 μV h−1. Failure modes are primarily attributed to Pt dissolution and migration, but the vdW heterostructure mitigates these by strong anchoring. Post-mortem analyses would be required to identify any MoS2 degradation or membrane contamination, but the reported stability exceeds that of commercial Pt/C (44 μV h−1) and Pt1/hNCNC (90 μV h−1), demonstrating robustness under industrial conditions.
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