Acting by producing reactive oxygen species (ROS) in situ, nanozymes are promising as antimicrobials. ROS’ intrinsic inability to distinguish bacteria from mammalian cells, however, deprives nanozymes of the selectivity necessary for an ideal antimicrobial. Here we report that nanozymes that generate surface-bound ROS selectively kill bacteria over mammalian cells. This result is robust across three distinct nanozymes that universally generate surface-bound ROS, with an oxidase-like silver-palladium bimetallic alloy nanocage, AgPd0.38, being the lead model. The selectivity is attributable to both the surface-bound nature of ROS these nanozymes generate and an unexpected antidote role of endocytosis. Though surface-bound, the ROS on AgPd0.38 efficiently eliminated antibiotic-resistant bacteria and effectively delayed the onset of bacterial resistance emergence. When used as coating additives, AgPd0.38 enabled an inert substrate to inhibit biofilm formation and suppress infection-related immune responses in mouse models. This work opens an avenue toward biocompatible nanozymes and may have implication in our fight against antimicrobial resistance.

are extremely reactive, metal centers are commonly stabilized on supports via coordination of nonmetal dopants. In this regard, excess dopants are employed to optimize the loading content of SACs on the carbon. Such an excess content of dopants can in turn lead to inevitable interference on the catalytic performance of SACs, [2] which may hamper the mechanism study on the catalytic reaction. Taking nitrogen (N, the most commonly explored dopant for preparation of carbonbased SACs) for instance, with various metallic loading of single-atom catalysts, [3] most of the N dopants do not take part in coordinating with SACs through formation of M-N x species (M, metallic atom and x , coordination number). The other N dopants remained in the form of pyrrole N, pyridine N, graphitic N, and N-O on the carbon-based SACs. During the catalytic reaction, these N species can possibly induce various unfavorable effects on the carbon-supported SACs. In many cases, enormous property differences have been observed on the SACs that were reported to have similar or even the same structure, concluding contradict relationship between coordination and selectivity. [4] For example, similar Ni-N x SACs showed different potential window of CO selectivity in electrocatalytic CO 2 reduction reaction (CO 2 RR). [1c,5] As a consequence, it remains a huge gap between the understanding on the correlation of the Carbon-supported single-atom catalysts (SACs) are extensively studied because of their outstanding activity and selectivity toward a wide range of catalytic reactions. Amidst its development, excess dopants (e.g., nitrogen) are always required to ensure the high loading content of SACs on the carbon support. However, the use of excess dopants is accompanied by formation of miscellaneous structures (particularly the uncoordinated N species) on catalysts, leading to adverse effects on their performance. Herein, the synthesis of carbon-supported Ni SACs with precisely controlled single-atom structure via joule heating strategy, showing the coordination of 80% of N dopants with metal elements, is reported. The preclusion of the unfavorable N species is confirmed to be the main reason for the superior performance of optimized Ni SACs in electrocatalytic carbon dioxide reduction reaction, which demonstrates unprecedented activity, selectivity, and stability under an exceptionally broad voltage range (>92% CO selectivity in the range of −0.7 to −1.9 V reversible hydrogen electrode). Such a synthetic strategy is further applicable for the design of SACs with various metals. This work demonstrates a facile method for preclusion of unfavorable dopants in the SACs and its importance in catalytic application.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.202104090.

Light utilization largely governs the performance of CO2 photoconversion, whereas most of the materials that are implemented in such an application are restricted in a narrow spectral absorption range. Plasmonic metamaterials with a designable regular pattern and facile tunability are excellent candidates for maximizing light absorption to generate substantial hot electrons and thermal energy. Herein, a concept of coupling a Au‐based stacked plasmonic metamaterial with single Cu atoms in alloy, as light absorber and catalytic sites, respectively, is reported for gas‐phase light‐driven catalytic CO2 hydrogenation. The metamaterial structure works in a broad spectral range (370–1040 nm) to generate high surface temperature for photothermal catalysis, and also induces strong localized electric field in favor of transfer of hot electrons and reduced energy barrier in CO2 hydrogenation. This work unravels the significant role of a strong localized electric field in photothermal catalysis and demonstrates a scalable fabrication approach to light‐driven catalysts based on plasmonic metamaterials.

The inability of commercial personal protective equipment (PPE) to inactivate microbes in the droplets/aerosols they intercept makes used PPE a potential source of cross-contamination. To make PPE spontaneously and continuously antimicrobial, we incorporate PPE with oxidase-like catalysts, which efficiently convert O2 into reactive oxygen species (ROS) without requiring any externally applied stimulus. Using a single-atom catalyst (SAC) nanoparticle containing atomically dispersed copper atoms as the reactive centers (Cu-SAC) and a silver–palladium bimetallic alloy nanoparticle (AgPd0.38) as models for oxidase-like catalysts, we show that the incorporation of oxidase-like catalysts enables PPE to inactivate bacteria in the droplets/aerosols they intercept without requiring any externally applied stimulus. Notably, this approach works both for PPE that are fibrous and woven such as a commercial KN95 facial respirator and for those made of solid plastics such as an apron. This work suggests a feasible and global approach for preventing PPE from spreading infectious diseases.