Coordination Tailoring of Pt Single‐Atom Catalysts at Room Temperature and Their Exceptional Performance in Hydrogen Evolution Reaction
ABSTRACT Single‐atom catalysts (SACs) have garnered interest in designing their ligand environments, facilitating the modification of single catalytic sites toward high activity and selectivity. Despite various synthetic approaches, it remains challenging to achieve a catalytically favorable coordin...
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| Main Authors: | , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Wiley
2025-05-01
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| Series: | Carbon Energy |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/cey2.720 |
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| Summary: | ABSTRACT Single‐atom catalysts (SACs) have garnered interest in designing their ligand environments, facilitating the modification of single catalytic sites toward high activity and selectivity. Despite various synthetic approaches, it remains challenging to achieve a catalytically favorable coordination structure simultaneously with the feasible formation of SACs at low temperatures. Here, a new type of coordination structure for Pt SACs is introduced to offer a highly efficient hydrogen evolution reaction (HER) catalyst, where Pt SACs are readily fabricated by atomically confining PtCl2 on chemically driven NO2 sites in two‐dimensional nitrogen‐doped carbon nanosheets at room temperature. The resultant Pt SACs form the NO2–Pt–Cl2 coordination structure with an atomic dispersion, as revealed by X‐ray spectroscopy and transmission electron microscopy investigations. Moreover, our first‐principles density functional theory (DFT) calculations show strong interactions in the coordination by computing the binding energy and charge density difference between PtCl2 and NO2. Pt SACs, established on the NO2‐functionalized carbon support, demonstrate the onset potential of 25 mV, Tafel slope of 40 mV dec−1, and high specific activity of 1.35 A mgPt−1. Importantly, the Pt SACs also exhibit long‐term stability up to 110 h, which is a significant advance in the field of single‐atom Pt catalysts. The newly developed coordination structure of Pt SACs features a single Pt active center, providing hydrogen binding ability comparable to that of Pt(111), enhanced long‐term durability due to strong metal‐support interactions, and the advantage of room‐temperature fabrication. |
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| ISSN: | 2637-9368 |