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<p>Efficient separation of carbon monoxide (CO) from nitrogen (N₂) is vital for recycling steel industry by-product gases and advancing carbon-neutral chemical production. However, current Cu(I)-based π-complexation adsorbents suffer from excessive binding strength and low working capacity. Here we report thermally-dispersed open metal sites (OMS) with two-coordinated Cu(I) units, ( ≡ C–O)CuCl, anchored onto zeolite imidazolate frameworks (ZIFs) derived oxygen-containing porous carbons (ZPC), where the Cu···CO interaction strength is precisely moderated. The optimized adsorbent, 15Cu(I)/ZPC-1, with 15 mmol g⁻¹ Cu(I) dispersed in 10–30 Å pores, delivers a high CO working capacity of 3.21 mmol g⁻¹ (0.1–1 bar, 298 K), the highest among reported recyclable Cu(I)-based adsorbents. The analyses reveal that a low-symmetric trigonal ( ≡ C–O)CuCl···CO coordination geometry weakens π-backbonding, enhances working capacity. Process simulations predict that 15Cu(I)/ZPC-1 enables high productivity and low energy consumption. This work establishes OMS regulation in porous carbon as an effective strategy for efficient CO/N₂ separation.</p>

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Two-coordinate Cu(I) sites in ZIF-derived porous carbon enable high CO working capacity for CO/N₂ separation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年7月14日

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  • Congli Li,
  • Qingmin Hu,
  • Bin Zheng,
  • Zhengxing Lv,
  • Jiahui Yang,
  • Xuling Guo,
  • Zhitong Zhao,
  • Lei Tang,
  • Rufeng Tian,
  • Qi Shi,
  • Zhe Gao,
  • Jinxiang Dong,
  • Yue-Biao Zhang

摘要

Efficient separation of carbon monoxide (CO) from nitrogen (N₂) is vital for recycling steel industry by-product gases and advancing carbon-neutral chemical production. However, current Cu(I)-based π-complexation adsorbents suffer from excessive binding strength and low working capacity. Here we report thermally-dispersed open metal sites (OMS) with two-coordinated Cu(I) units, ( ≡ C–O)CuCl, anchored onto zeolite imidazolate frameworks (ZIFs) derived oxygen-containing porous carbons (ZPC), where the Cu···CO interaction strength is precisely moderated. The optimized adsorbent, 15Cu(I)/ZPC-1, with 15 mmol g⁻¹ Cu(I) dispersed in 10–30 Å pores, delivers a high CO working capacity of 3.21 mmol g⁻¹ (0.1–1 bar, 298 K), the highest among reported recyclable Cu(I)-based adsorbents. The analyses reveal that a low-symmetric trigonal ( ≡ C–O)CuCl···CO coordination geometry weakens π-backbonding, enhances working capacity. Process simulations predict that 15Cu(I)/ZPC-1 enables high productivity and low energy consumption. This work establishes OMS regulation in porous carbon as an effective strategy for efficient CO/N₂ separation.