Two-dimensional materials, such as layered compounds and nanosheets, have attracted interest for their characteristic structures and properties. If layered materials containing functional organic molecules are synthesized, designed nanosheets can be obtained by exfoliation. Here we show the design and synthesis of an amorphous organic layered material containing a conjugated-polymer network, its exfoliation into nanosheets, and their applications. Copolymerization of benzoquinone and pyrrole generates random stacks of the conjugated polymer layers through successive C-C bond formation and pericyclic reaction under mild conditions at 60 °C. The amorphous organic layered materials are efficiently exfoliated into nanosheets in 44.6% after 1 h. The nanosheets are used as a metal-free electrocatalyst for hydrogen evolution reaction with the overpotential 0.28 V (vs. RHE). The present approach may be applied to the design of functional nanosheets with graphene-like structures under mild conditions.

二维材料（例如层状化合物和纳米片）因其独特的结构和性能而引起了人们的兴趣。如果合成包含功能性有机分子的层状材料，则可以通过剥离获得设计的纳米片。在这里，我们展示了包含共轭聚合物网络的无定形有机层状材料的设计与合成，其剥离成纳米片及其应用。苯醌和吡咯的共聚反应通过在60°C的温和条件下连续的CC键形成和周环反应生成共轭聚合物层的无规堆叠。1小时后，非晶有机层状材料有效地剥落到纳米片中的比例为44.6％。纳米片被用作无金属的电催化剂，用于过电势为0.28 V（vs. RHE）的氢气析出反应。本方法可以应用于在温和条件下具有石墨烯样结构的功能纳米片的设计。