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史林启课题组 | ACTA BIOMATERIALIA

发布人:    发布时间:2024/06/28   浏览次数:

Cetyltrimethylammonium-chloride assisted in situ metabolic incorporation of nano-sized ROS-generating cascade-reaction containers in Gram-positive and Gram-negative peptidoglycan layers for the control of bacterially-induced sepsis


By

Yang, G (Yang, Guang) [1] , [2] , [3] ; Wang, DY (Wang, Da -Yuan) [1] , [2] , [3] ; Song, JW (Song, Jianwen) [1] ; Ren, YJ (Ren, Yijin) [4] , [5] ; An, YL (An, Yingli) [1] ; Busscher, HJ (Busscher, Henk J.) [2] , [3] ; van der Mei, HC (van der Mei, Henny C.) [3] ; Shi, LQ (Shi, Linqi) [1]
(provided by Clarivate)

Source

ACTA BIOMATERIALIA

Volume

181

Page

347-361

DOI

10.1016/j.actbio.2024.04.045

Published

JUN 2024

Indexed

2024-06-22

Document Type

Article

Abstract

Cascade -reaction containers generating reactive oxygen species (ROS) as an alternative for antibioticbased strategies for bacterial infection control, require endogenous oxygen -sources and ROS-generation close to or preferably inside target bacteria. Here, this is achieved by cetyltrimethylammonium-chloride (CTAC) assisted in situ metabolic labeling and incorporation of mesoporous SiO 2 -nanoparticles, dualloaded with glucose-oxidase and Fe 3 O 4 -nanoparticles as cascade -reaction containers, inside bacterial cell walls. First, azide-functionalized d-alanine (D -Ala -N 3 ) was inserted in cell wall peptidoglycan layers of growing Gram-positive pathogens. In Gram -negatives, this could only be achieved after outer lipidmembrane permeabilization, using a low concentration of CTAC. Low concentrations of CTAC had no adverse effect on in vitro blood clotting or hemolysis nor on the health of mice when blood -injected. Next, dibenzocyclooctyne-polyethylene-glycol modified, SiO 2 -nanoparticles were in situ click -reacted with dAla -N 3 in bacterial cell wall peptidoglycan layers. Herewith, a two-step cascade -reaction is facilitated inside bacteria, in which glucose-oxidase generates H 2 O 2 at endogenously -available glucose concentrations, while subsequently Fe 3 O 4 -nanoparticles catalyze generation of center dot OH from the H 2 O 2 generated. Generation of center dot OH inside bacterial cell walls by dual -loaded mesoporous SiO 2 -nanoparticles yielded more effective in vitro killing of both planktonic Gram-positive and Gram-negative bacteria suspended in 10 % plasma than SiO 2 -nanoparticles solely loaded with glucose-oxidase. Gram-positive or Gram-negative bacterially induced sepsis in mice could be effectively treated by in situ pre-treatment with tail -vein injected CTAC and d -Ala -N 3 , followed by injection of dual -loaded cascade -reaction containers without using antibiotics. This makes in situ metabolic incorporation of cascade -reaction containers as described attractive for further investigation with respect to the control of other types of infections comprising planktonic bacteria. Statement of Significance In situ metabolic -incorporation of cascade -reaction -containers loaded with glucose-oxidase and Fe 3 O 4 nanoparticles into bacterial cell -wall peptidoglycan is described, yielding ROS-generation from endogenous glucose, non-antibiotically killing bacteria before ROS inactivates. Hitherto, only Gram -positives could be metabolically -labeled, because Gram -negatives possess two lipid -membranes. The outer membrane impedes direct access to the peptidoglycan. This problem was solved by outer -membrane permeabilization using a quaternary -ammonium compound. Several studies on metabolic -labeling perform crucial labeling steps during bacterial -culturing that in real -life should be part of a treatment. In situ metabolic -incorporation as described, can be applied in well -plates during in vitro experiments or in the body as during in vivo animal experiments. Surprisingly, metabolic -incorporation proceeded unhampered in blood and a murine, bacterially -induced sepsis could be well treated.