Photothermal
treatment (PTT) involving a combination of therapeutic
modalities recently emerged as an efficient alternative for combating
biofilm. However, PTT-related local high temperature may destroy the
surrounding healthy tissues. Herein, we present an all-in-one phototherapeutic
nanoplatform consisting of l-arginine (l-Arg), indocyanine
green (ICG), and mesoporous polydopamine (MPDA), namely, AI-MPDA,
to eliminate the already-formed biofilm. The fabrication process included
surface modification of MPDA with l-Arg and further adsorption
of ICG via π–π stacking. Under
near-infrared (NIR) exposure, AI-MPDA not only generated heat but
also produced reactive oxygen species, causing a cascade catalysis
of l-Arg to release nitric oxide (NO). Under NIR irradiation,
biofilm elimination was attributed to the NO-enhanced photodynamic
therapy and low-temperature PTT (≤45 °C). Notably, the
NIR-triggered all-in-one strategy resulted in severe destruction of
bacterial membranes. The phototherapeutic AI-MPDA also displayed good
cytocompatibility. NIR-irradiated AI-MPDA nanoparticles not only prevented
bacterial colonization but also realized a rapid recovery of infected
wounds. More importantly, the all-in-one phototherapeutic platform
displayed effective biofilm elimination with an efficiency of around
100% in a abscess formation model. Overall, this low-temperature phototherapeutic
platform provides a reliable tool for combating already-formed biofilms
in clinical applications.
Flexible zinc–air batteries (ZAB) are a promising battery candidate for emerging flexible electronic devices, but the catalysis‐based working principle and unique semi‐opened structure pose a severe challenge to their overall performance at cold temperature. Herein, we report the first flexible rechargeable ZAB with excellent low‐temperature adaptability, based on the innovation of an efficient electrocatalyst to offset the electrochemical performance shrinkage caused by decreased temperature and a highly conductive hydrogel with a polarized terminal group to render the anti‐freezing property. The fabricated ZABs show excellent electrochemical performances that outperform those of many aqueous ZABs at room temperature. They also deliver a high capacity of 691 mAh g−1 and an energy density of 798 Wh kg−1 at −20 °C (92.7 % and 87.2 % retention of the room temperature counterparts, respectively), together with excellent flexibility and reverting capability.
Metal–nitrogen–carbon
(M–N–C) single-atom
catalysts (SACs) show high catalytic activity for many important chemical
reactions. However, an understanding of their intrinsic catalytic
activity remains ambiguous because of the lack of well-defined atomic
structure control in current M–N–C SACs. Here, we use
covalent organic framework SACs with an identical metal coordination
environment as model catalysts to elucidate the intrinsic catalytic
activity of various metal centers in M–N–C SACs. A pH-universal
activity trend is discovered among six 3d transition metals for hydrogen
peroxide (H2O2) synthesis, with Co having the
highest catalytic activity. Using density functional calculations
to access a total of 18 metal species, we demonstrate that the difference
in the binding energy of O2* and HOOH* intermediates (E
O2*
– E
HOOH*) on single metal centers is a reliable thermodynamic
descriptor to predict the catalytic activity of the metal centers.
The predicted high activity of Ir centers from the descriptor is further
validated experimentally. This work suggests a class of structurally
defined model catalysts and clear mechanistic principles for metal
centers of M–N–C SACs in H2O2 synthesis,
which may be further extendable to other reactions.
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