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<p>While solar evaporation efficiency fundamentally depends on photothermal conversion dynamics, conventional materials face an irreconcilable compromise between broadband absorption and rapid energy transfer. Here, we resolve this dilemma through high-entropy single-atom porous carbon sponge (HESAs@PCS), where five transition metals are atomically dispersed in a nitrogen-doped carbon matrix via hierarchically pore-confined spatial proximity. Synchrotron XAFS and DFT theoretical calculation reveal compressed M–N bonds in Fe/Co/Ni/Cu and elongated Mn–N environments, driving space interactions among proximal metals and gradient d-p orbital hybridization. Systematic evaluation of 12 control samples spanning unitary, ternary, and quaternary analogs also confirms that multi-metal synergy within hierarchically porous directly correlates with optical absorption intensification and energy transfer via metal-N bonds as bridges. The optimized HESAs@PCS evaporator achieves a record evaporation rate of 2.36 kg m<sup>−2</sup> h<sup>−1</sup> under 1 sun irradiation, outperforming state-of-the-art single-metal analogs by 10.3% in seawater desalination. This work deciphers hierarchically pore-mediated spatially interactions and d-p orbital coupling tailoring, offering a blueprint for advanced solar-driven systems.</p>

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Orbital coupling modulation in hierarchical pore-confined high-entropy single atoms for efficient solar photothermal conversion

  • 期刊论文

  • 发表日期：

    2026年3月9日

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  • Chong Wang,
  • Shan Hu,
  • Tong Liu,
  • Wei Wang,
  • Liangjun Xia,
  • Yang Wang,
  • Yuanfu Ren,
  • Huabin Zhang,
  • Jiacheng Ma,
  • Weilin Xu,
  • Wenhuan Huang

摘要

While solar evaporation efficiency fundamentally depends on photothermal conversion dynamics, conventional materials face an irreconcilable compromise between broadband absorption and rapid energy transfer. Here, we resolve this dilemma through high-entropy single-atom porous carbon sponge (HESAs@PCS), where five transition metals are atomically dispersed in a nitrogen-doped carbon matrix via hierarchically pore-confined spatial proximity. Synchrotron XAFS and DFT theoretical calculation reveal compressed M–N bonds in Fe/Co/Ni/Cu and elongated Mn–N environments, driving space interactions among proximal metals and gradient d-p orbital hybridization. Systematic evaluation of 12 control samples spanning unitary, ternary, and quaternary analogs also confirms that multi-metal synergy within hierarchically porous directly correlates with optical absorption intensification and energy transfer via metal-N bonds as bridges. The optimized HESAs@PCS evaporator achieves a record evaporation rate of 2.36 kg m−2 h−1 under 1 sun irradiation, outperforming state-of-the-art single-metal analogs by 10.3% in seawater desalination. This work deciphers hierarchically pore-mediated spatially interactions and d-p orbital coupling tailoring, offering a blueprint for advanced solar-driven systems.