Direct synthesis of graphene with well‐defined nanoscale pores over large areas can transform the fabrication of nanoporous atomically thin membranes (NATMs) and greatly enhance their potential for practical applications. However, scalable bottom‐up synthesis of continuous sheets of nanoporous graphene that maintain integrity over large areas has not been demonstrated. Here, it is shown that a simple reduction in temperature during chemical vapor deposition (CVD) on Cu induces in‐situ formation of nanoscale defects (≤2–3 nm) in the graphene lattice, enabling direct and scalable synthesis of nanoporous monolayer graphene. By solution‐casting of hierarchically porous polyether sulfone supports on the as‐grown nanoporous CVD graphene, large‐area (>5 cm²) NATMs for dialysis applications are demonstrated. The synthesized NATMs show size‐selective diffusive transport and effective separation of small molecules and salts from a model protein, with ≈2–100× increase in permeance along with selectivity better than or comparable to state‐of‐the‐art commercially available polymeric dialysis membranes. The membranes constitute the largest fully functional NATMs fabricated via bottom‐up nanopore formation, and can be easily scaled up to larger sizes permitted by CVD synthesis. The results highlight synergistic benefits in blending traditional membrane casting with bottom‐up pore creation during graphene CVD for advancing NATMs toward practical applications.

中文翻译：

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直接合成具有纳米级孔隙率的石墨烯可轻松制备大面积的原子薄膜

在大面积上具有明确定义的纳米级孔的石墨烯的直接合成可以改变纳米多孔原子薄膜（NATM）的制造方式，并极大地增强其在实际应用中的潜力。但是，尚未证明可扩展的自底向上合成方法，该方法可在大面积上保持完整性的纳米多孔石墨烯连续片材的合成。在此表明，在铜上进行化学气相沉积（CVD）期间温度的简单降低会诱导石墨烯晶格中原位形成纳米级缺陷（≤2-3nm），从而可以直接且可扩展地合成纳米多孔单层石墨烯。通过在逐步生长的纳米多孔CVD石墨烯上浇铸分级多孔聚醚砜载体，大面积（> 5 cm ²）展示了用于透析应用的NATM。合成的NATM表现出大小选择性扩散运输以及从模型蛋白中有效分离小分子和盐的作用，渗透率增加了≈2–100倍，选择性也优于或与最新的市售聚合物透析相当膜。该膜构成了通过自下而上的纳米孔形成而制造的最大的全功能NATM，并且可以轻松按比例放大至CVD合成所允许的更大尺寸。结果突出显示了在将传统膜浇铸与石墨烯CVD期间自下而上的孔生成混合在一起的协同优势，从而将NATM推向了实际应用。