Steering N/S coordination number to accelerate catecholase-like catalysis over low-coordinated Cu site.

Modulation of coordination configuration is crucial for boosting the biomimetic catalytic activity of nanozymes, but remains challenging. Here, we found that the non-first-shell amino group in the ligand was capable of steering the N/S coordination number through remote induction to enable the formation of a low-coordinated CuNS configuration. This endowed the resulting nanozyme (ATT-Cu) with an upshifted d-band center compared with a control nanozyme (TT-Cu) with CuNS configuration, enhancing the adsorption capabilities of ATT-Cu for O and HO intermediates as well as its affinity for catechol.