Abstract

Metal isolated single atomic sites catalysts have attracted intensive attention in recent years owing to their maximized atom utilization and unique structure. Despite the success of single atom catalyst synthesis, directly anchoring metal single atoms on three-dimensional (3D) macro support, which is promising to achieve the heterogenization of homogeneous catalysis, remains a challenge and a blank in this field. Herein, we successfully fabricate metal single atoms (Pd, Pt, Ru, Au) on porous carbon nitride/reduced graphene oxide (C₃N₄/rGO) foam as highly efficient catalysts with convenient recyclability. C₃N₄/rGO foam features two-dimensional microstructures with abundant N chelating sites for the stabilization of metal single atoms and vertically-aligned hierarchical mesostructure that benefits the mass diffusion. The obtained Pd₁/C₃N₄/rGO monolith catalyst exhibits much enhanced activity over its nanoparticle counterpart for Suzuki-Miyaura reaction. Moreover, the Pd₁/C₃N₄/rGO monolith catalyst can be readily assembled in a flow reactor to achieve the highly efficient continuous production of 4-nitro-1,1′-biphenyl through Suzuki-Miyaura coupling.

中文翻译：

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在C 3 N 4 / rGO上制备Pd分离的单原子位点，以实现均相催化的均相

摘要

近年来，金属分离的单原子位催化剂由于其最大的原子利用率和独特的结构而备受关注。尽管单原子催化剂合成成功，但是将金属单原子直接锚定在三维（3D）宏观载体上，有望实现均相催化的异质化，仍然是该领域的挑战和空白。在这里，我们成功地在多孔氮化碳/还原氧化石墨烯（C ₃ N ₄ / rGO）泡沫上制备了金属单原子（Pd，Pt，Ru，Au），作为具有便捷可回收性的高效催化剂。C ₃ N ₄/ rGO泡沫具有二维微观结构，具有丰富的N螯合位点以稳定金属单原子，并且垂直排列的分层介观结构有利于质量扩散。所获得的Pd ₁ / C ₃ N ₄ / rGO整体催化剂与铃木-宫浦反应的纳米粒子相比，具有更大的活性。此外，Pd ₁ / C ₃ N ₄ / rGO整体催化剂可以很容易地在流动反应器中组装，以通过Suzuki-Miyaura偶联高效连续地生产4-硝基-1,1'-联苯。