Single copper sites dispersed on metal-organic frameworks boost the degradation of nerve agent simulants

The detoxification of nerve agents, a class of extremely toxic chemical warfare agents, is urgently needed because they have remained a threat to humanity. To date, zirconium-based metal-organic frameworks (Zr-MOFs) are the most popular catalysts in this realm. However, it is still essential to develop new and efficient catalysts based on Zr-MOFs to achieve more rapid hydrolysis. Herein, we report that the single-atom catalyst (SAC) with Cu single atoms on a UiO-66-NH2 support (Cu@UiO-66-NH2) could significantly boost the degradation of the nerve agent simulant. Compared with the pristine UiO-66-NH2, this SAC exhibited remarkable catalytic activity with a half-life for hydrolysis of ∼2 min and better reusability in cyclic experiments. Both experimental and theoretical studies suggest that the atomically dispersed Cu species anchored to the amino groups rather than to the Zr6 node of UiO-66-NH2 acted as the catalytic active sites, leading to favorable binding geometries with the substrate and the product. A catalytic mechanism on the SAC different from that generally considered on the pristine Zr-MOFs was thus presented to elucidate the enhanced catalytic efficiency.