The attachment and subsequent colonization of bacteria on the surfaces of synthetic materials and devices lead to serious problems in both human healthcare and industrial applications. Therefore, antibacterial surfaces that can prevent bacterial attachment and biofilm formation have been a long-standing focus of considerable interest and research efforts. Recently, a promising "kill-release" strategy has been proposed and applied to construct so-called smart antibacterial surfaces, which can kill bacteria attached to their surface and then undergo on-demand release of the dead bacteria and other debris to reveal a clean surface under an appropriate stimulus, thereby maintaining effective long-term antibacterial activity. This Review focuses on the recent progress (particularly over the past 5 years) on such smart antibacterial surfaces. According to the different design strategies, these surfaces can be divided into three categories: (i) "K + R"-type surfaces, which have both a killing unit and a releasing unit; (ii) "K → R"-type surfaces, which have a surface-immobilized killing unit that can be switched to perform a releasing function; and (iii) "K + (R)"-type surfaces, which have only a killing unit but can release dead bacteria upon the addition of a release solution. In the end, a brief perspective on future research directions and the major challenges in this promising field is also presented.

Smart Antibacterial Surfaces with Switchable Bacteria-Killing and Bacteria-Releasing Capabilities

Due to the emerging bacterial resistance and the protection of tenacious biofilms, it is hard for the single antibacterial modality to achieve satisfactory therapeutic effects nowadays. In recent years, photothermal therapy (PTT)-derived multimodal synergistic treatments have received wide attention and exhibited cooperatively enhanced bactericidal activity. PTT features spatiotemporally controllable generation of hyperthermia that could eradicate bacteria without inducing resistance. The synergy of it with other treatments, such as chemotherapy, photo-dynamic/catalytic therapy (PDT/PCT), immunotherapy, and sonodynamic therapy (SDT), could lower the introduced laser density in PTT and avoid undesired overheating injury of normal tissues. Simultaneously, by heat-induced improvement of the bacterial membrane permeability, PTT is conducive for accelerated intracellular permeation of chemotherapeutic drugs as well as reactive oxygen species (ROS) generated by photosensitizers/sonosensitizers, and could promote infiltration of immune cells. Thereby, it could solve the currently existing sterilization deficiencies of other combined therapeutic modes, for example, bacterial resistance for chemotherapy, low drug permeability for PDT/PCT/SDT, adverse immunoreactions for immunotherapy, etc. Admittedly, PTT-derived synergistic treatments are becoming essential in fighting bacterial infection, especially those caused by antibiotic-resistant strains. This review firstly presents the classical and newly reported photothermal agents (PTAs) in brief. Profoundly, through the introduction of delicately designed nanocomposite platforms, we systematically discuss the versatile photothermal-derived multimodal synergistic therapy with the purpose of sterilization application. At the end, challenges to PTT-derived combinational therapy are presented and promising synergistic bactericidal prospects are anticipated.

Emerging photothermal-derived multimodal synergistic therapy in combating bacterial infections.

Synthesis, Self-Assembly, and Biomedical Applications of Antimicrobial Peptide–Polymer Conjugates

Polypeptides have attracted considerable attention in recent decades due to their inherent biodegradability and tunable cytocompatibility. Macromolecular design in conjunction with rational monomer composition can direct architecture, self-assembly and chemical behavior, ultimately guiding the choice of appropriate application within the biomedical field. This review focuses on the applications of polypeptides alongside the synthetic advances in the ring opening polymerization of α-amino acid N-carboxyanhydrides achieved in the past five years. Key architectures obtained through NCA ROP or in combination with other polymerization methods are reviewed, as these play an important role in the wide range of applications towards which polypeptides have been applied.

Ring opening polymerization of α-amino acids: advances in synthesis, architecture and applications of polypeptides and their hybrids.

The human society is faced with daunting threats from bacterial infections. Over decades, a variety of antibacterial polymeric nanosystems have exhibited great promise for the eradication of multidrug-resistant bacteria and persistent biofilms by enhancing bacterial recognition and binding capabilities. In this Review, the "state-of-the-art" biodegradable antibacterial polymeric nanosystems, which could respond to bacteria environments (e.g., acidity or bacterial enzymes) for controlled antibiotic release or multimodal antibacterial treatment, are summarized. The current antibacterial polymeric nanosystems can be categorized into antibiotic-containing and intrinsic antibacterial nanosystems. The antibiotic-containing polymeric nanosystems include antibiotic-encapsulated nanocarriers (e.g., polymeric micelles, vesicles, nanogels) and antibiotic-conjugated polymer nanosystems for the delivery of antibiotic drugs. On the other hand, the intrinsic antibacterial polymer nanosystems containing bactericidal moieties such as quaternary ammonium groups, phosphonium groups, polycations, antimicrobial peptides (AMPs), and their synthetic mimics, are also described. The biodegradability of the nanosystems can be rendered by the incorporation of labile chemical linkages, such as carbonate, ester, amide, and phosphoester bonds. The design and synthesis of the degradable polymeric building blocks and their fabrications into nanosystems are also explicated, together with their plausible action mechanisms and potential biomedical applications. The perspectives of the current research in this field are also described.

Yashao Chen

Papers

Methacrylate-ended polypeptides and polypeptoids for antimicrobial and antifouling coatings