Arrangement of Ordered D–A Components in a Metal‐Organic Framework for Cocatalyst‐Free Photocatalytic Hydrogen Evolution with Efficient Proton Conduction

. A detailed mechanism study revealed that the energy bond defined by the D-A components assisted with metal centers is the key to efficiently generating photogenerated charge carriers, and 2 has an appropriate affinity to proton to reduce the energy barrier for hydrogen evolution. Besides, the enhanced proton transport kinetics based on the arrayed free carboxyl groups in the hydrogen-bonded network endows 2 with higher proton conductivity than 1, thus promoting the usage rate of active metal sites in 2 for enhanced hydrogen evolution reaction kinetics.