Ligand-Restricted Strategy for Synthesizing Highly Pairing Dual Atom Catalysts

Dual atom catalysts (DACs), characterized by high activity and metal utilization, as well as structural diversity with a large variety of catalytic sites, hold immense promise for energy conversion technologies, garnering substantial interest from both academia and industry. However, achieving precise control and manipulation of atomic dispersion, pairing ratios, and interatomic distances in DACs, which significantly affect their multifunctional catalytic properties, remains a significant challenge. Herein, we developed a ligand-restricted strategy for the precise synthesis of highly pairing DACs with tunable atomic distances. This was accomplished by coordinating diamine ligands with dual metal precursors, restricting the pairing and relative positions of two metal atoms on two-dimensional graphitic carbon nitride. The atomic pairing ratio exceeded 82%, with the chain length of diamine molecules effectively regulating the distance between paired atoms. As a demonstration, the pairing Pt ₁ -Au ₁ DACs exhibited almost three times catalytic activity for nitrate reduction to ammonia compared to their unpaired counterparts. Furthermore, shorter distanced Pt ₁ -Au ₁ DAC reveals four times activity in photothermal catalyzed hydrogenation reactions than longer ones. This work not only introduces a novel design strategy for the atomic-scale fabrication of complex catalysts but also provides valuable insights into nanoscale reaction mechanisms in heterogeneous catalysis.