Rational design and fabrication of metal–organic framework (MOF)-derived ordered hierarchical macro-/meso-/microporous N-doped carbon materials featured with the atomically dispersed metal atoms can effectively enhance their catalytic performance. Herein we develop a template-assisted strategy, namely the confined growth and pyrolysis of single-crystalline zeolite imidazolate framework-8 (ZIF-8) in three-dimensional ordered template voids, to create hierarchical porosity in MOFs-derived N-doped carbon materials. The as-synthesized single-atom Zn on N-doped hierarchically ordered porous carbon polyhedrons (Zn-N-HOPCPs) show integrated Lewis acid (single-atom Zn) and base sites (pyridinic N), high surface area (1128 m²·g⁻¹), large pore volume (0.90 cm³·g⁻¹), periodically interconnected open windows (~55 nm), highly accessible micro/mesopore channels (0.55, 0.8, 1.2, and 4 nm), and abundant Zn content (5.8 wt%). The hierarchical nanoarchitecture (macro-/meso-/micropores) significantly facilitates mass transfer for bulky-molecule-involved reactions and exposes inside active sites, resulting in satisfactory CO₂ photoconversion under mild conditions. The strategy presented here sheds light on the design and fabrication of various hierarchically ordered porous carbon decorated with atomically dispersed metal atoms for other important applications.

合理设计和制造金属-有机骨架（MOF）衍生的有序分层的大/中/微孔N掺杂碳材料，这些材料具有原子分散的金属原子，可以有效地提高其催化性能。本文中，我们开发了一种模板辅助策略，即在三维有序模板空隙中单晶沸石咪唑盐骨架8（ZIF-8）的密闭生长和热解，以在MOF衍生的N掺杂碳材料中创建分层孔隙率。N掺杂的分级有序碳多孔多面体（Zn-N-HOPCPs）上合成的单原子Zn显示出集成的路易斯酸（单原子Zn）和碱基位点（吡啶N），具有高表面积（1128 m ² · g ^-1），大孔体积（0.90 cm ³ ·g^-1），周期性互连的开放窗口（〜55 nm），高度可访问的微/中孔通道（0.55、0.8、1.2和4 nm）和丰富的Zn含量（5.8 wt％）。分层的纳米结构（大孔/中孔/微孔）极大地促进了大分子参与的反应的质量转移并暴露在活性位点内部，从而在温和条件下产生了令人满意的CO ₂光转化。本文提出的策略为设计和制造各种以原子分散的金属原子装饰的分层有序的多孔碳为其他重要应用提供了启示。