Content of review 1, reviewed on July 30, 2025

The manuscript entitled "Stabilizing Pt-Fe dual-metal single atoms in zifs: a pathway to form heterogeneous catalysts" reports the design of stable, dual-atom catalysts (DACs), advancing materials science by establishing synthesis strategies using in situ STEM with atomic-level understanding. While the concept is intriguing, I recommend a major revision of the manuscript due to the following concerns:

  1. The resolution of Figures 2f-g, Figures 2a, and Figures 5a should be improved to ensure clearer visualization of the features presented

  2. For single-atom systems—whether monometallic or bimetallic—it is essential to provide complementary characterization evidence to confirm the truly isolated nature of the metal atoms. In this work, in addition to HADDF imaging, XAFS characterization is necessary to determine whether metal–metal bonds exist around the active metal centers. Only with such evidence can the material be convincingly identified as a bimetallic single-atom catalyst.

  3. Given the typical limitations of transmission electron microscopy under reactive environments, the claimed in situ high-resolution HAADF-STEM characterization requires further clarification. The methodology described appears more consistent with a quasi-in situ strategy, where samples are imaged after reaction rather than during it.

  4. It is recommended to provide quasi-in situ XRD characterization, as it can offer structural-level insights into the formation process of bimetallic single atoms. For instance, such analysis would be valuable in supporting the following statement from this work: “The observed stability of Pt-Fe hetero-pairs, contrasted with Fe SA aggregation into Fe3C nanoclusters in single-metal systems, highlights the critical role of metal-metal interactions in preventing evaporation and clustering.

  5. In Fig. 2, XPS peak splitting and fitting is not reasonable. The fitting appears to lack sufficient justification regarding the number and position of peaks.

  6. Compared to F-ZIF, PF-ZIF maintains stable Pt–Fe heteroatomic pairs even at 900 °C, exhibiting superior resistance to aggregation and evaporation. The authors attribute this to enhanced electronic coupling between the metal atoms and the N-doped carbon matrix. However, more evidence and a thorough discussion are needed to support the formation mechanism of the bimetallic single atoms.

Source

    © 2025 the Reviewer.

Content of review 2, reviewed on September 16, 2025

The author has revised the manuscript according to the comments. I recommend accepting the article.

Source

    © 2025 the Reviewer.

References

    Kai-Yuan, H., Yi-Dong, L., Yu-Ru, L., Ching-Wei, C., Chun-Hui, L., Ruei-Hong, C., Dun-Jie, J., Yan-Gu, L., Yu-Lun, C., Ming-Yen, L. 2025. Stabilizing Pt-Fe dual-metal single atoms in ZIFs: a pathway to form heterogeneous catalysts. Materials Horizons.