Endogenous glucose-driven cascade reaction of nano-drug delivery for boosting multidrug-resistant bacteria-infected diabetic wound healing.

Multidrug-resistant (MDR) bacteria-infected wound healing remains greatly challenging, especially in diabetic patients. Herein, a novel nano-drug delivery based on endogenous glucose-driven cascade reaction is proposed for boosting MDR bacteria-infected diabetic wound healing with high efficacy by improving wound microenvironment and enhancing photodynamic antibacterial activity. The composite nanoagent is first self-assembled by integrating berberine (BBR) and epigallocatechin gallate (EGCG) from natural plant extracts, named as BENPs, which is successively coated with manganese dioxide nanoshells (MnO2 NSs) and glucose oxidase (GOX) to form the final BEMGNPs. The cascade reaction is triggered by glucose at the wound site of diabetes which is specifically catalyzed by GOX in the BEMGNPs to produce gluconic acid and hydrogen peroxide (H2O2). That is subsequently to decompose MnO2 NSs in the BEMGNPs to generate oxygen (O2). The BEMGNPs as photosensitizers effectively produce reactive oxygen species (ROS) to enhance the eradication of bacteria with the assistance of O2. Under the synergistic function of the cascaded reaction, the BEMGNPs present excellent antibacterial efficacy even for MDR bacteria. The in vivo experiments explicitly validate that the constructed nano-drug delivery can augment the MDR bacteria-infected diabetic wound healing with excellent biosafety. The as-proposed strategy provides an instructive way to combat ever-threatening MDR bacteria, which particularly is beneficial for diabetic patients.

Enhanced degradation of microplastics during sludge composting via microbially-driven Fenton reaction.

It has been increasingly documented that the hydroxyl radical (•OH) can promote the transformation of organic contaminants such as microplastics (MPs) in various environments. However, few studies have sought to identify an ideal strategy for accelerating in situ MPs degradation through boosting the process of •OH production in practical applications. In this work, iron-mineral-supplemented thermophilic composting (imTC) is proposed and demonstrated for enhancing in situ degradation of sludge-based MPs through strengthening •OH generation. The results show that the reduction efficiency of sludge-based MPs abundance was about 35.93% in imTC after treatment for 36 days, which was 38.99% higher than that of ordinary thermophilic composting (oTC). Further investigation on polyethylene-microplastics (PE-MPs) suggested that higher abundance of •OH (the maximum value was 408.1 µmol·kg-1) could be detected on the MPs isolated from imTC through microbially-mediated redox transformation of iron oxides, as compared to oTC. Analyses of the physicochemical properties of the composted PE-MPs indicated that increased •OH generation could largely accelerate the oxidative degradation of MPs. This work, for the first time, proposes a feasible strategy to enhance the reduction efficiency of MPs abundance during composting through the regulation of •OH production.

Reactive oxygen species accelerate humification process during iron mineral-amended sludge composting.

The production of hydroxyl radicals (OH) has been documented during composting. However, the effect of OH on composting efficiency remains unclear. Here, iron mineral supplemented thermophilic composting (imTC) is proposed and demonstrated for enhancing OH production and accelerating the maturation of composting. The results indicated that the maximum OH production of imTC was 1922.74 µmol·kg-1, which increased by 1.39 times than that of ordinary thermophilic composting (oTC). Importantly, the increase of OH could greatly enhance organic matter degradation and humic substances formation during imTC, resulting in shorting the maturity time by 25 %. Enrichment of laccase-producing bacteria resulted in higher laccase activity (31.85 U·g-1) in imTC compared with oTC (23.82 U·g-1), which may have contributed to the higher level of humification in imTC treatment. This work, for the first time, proposes a feasible strategy for improving composting efficiency through the regulation of OH production during aerobic composting.

Degradation of microplastics by hydroxyl radicals generated during microbially driven humus redox transformation.

The production of ·OH during transformation of redox active substances has been increasingly documented, and it causes the ageing or degradation of microplastics (MPs) in natural systems. However, the contribution of the humus redox cycle to ·OH generation and MPs transformation has previously been overlooked, even though it is ubiquitous in alternating anoxic-oxic environments. In this work, the integrated pathways of ·OH generation during the redox transformation of humic acids (HAs) and the contribution of this ·OH to the transformation of MPs were investigated for the first time. It was found that ·OH could be produced continuously during successive cycles of redox transformation of HAs mediated by Bacillus thermotolerans SgZ-8 through exogeneous HAs dependent and independent pathways. O2·- and H2O2 were identified as the key intermediate species, which were produced by both microbial aerobic respiration and HA oxidation. The ·OH generated by HA redox cycles could lead to a weight loss of PS-MPs of 18.1% through oxidative degradation during a period of 8 weeks of anoxic-oxic incubation. The EDC of HAs is closely related to ·OH production, which could have a large influence on the effectiveness of oxidative degradation of PS-MPs during various HAs redox cycles in temporarily anoxic environmental systems. These findings provide new insights into ·OH formation and MPs transformation through microbially driven humus redox cycles in alternating anoxic-oxic environments.

Extensive production and evolution of free radicals during composting.

The production of free radicals has been widely documented in natural systems, where they play an important role in most organic matter and contaminants transformation. Here, the production and evolution of free radicals were systematically investigated during composting. Results indicated that multiple reactive oxygen species and environmentally persistent free radicals (G-factor 2.003-2.004) were generated with dynamic changes during composting. The ·OH yield fluctuated significantly with a maximum content of 365.7-1,262.3 µmol/kg at the thermophilic phase of composting, which was closely correlated with the changes of Fe (II) (Pearson's r = 0.928-0.932) and the electron-donating capacity of humus (Pearson's r = 0.958-0.896) during composting. Further investigation suggested that microorganisms driven iron/humus redox conversion could contribute to the production and dynamic changes of free radical during composting. These findings highlight the abiotic processes involving free radicals, and provide a new perspective for humification and contaminants removal during composting.

Free radicals accelerate in situ ageing of microplastics during sludge composting.

Composting is the last "barrier" for microplastics (MPs) in the entry of organic solid wastes into the environment. The transformation of MPs is thought to be mainly driven by microorganisms during composting, whereas the contribution of abiotic processes that involve free radicals is often overlooked. Herein, we provide initial evidence for the generation of free radicals during sludge composting, including environmental persistent free radicals and reactive oxygen species, which accelerate the oxidative degradation of MPs. The ·OH yield of composting fluctuated greatly from 23.03 to 277.18 µmol/kg during composting, which was closely related to the dynamic changes in Fe(II) (R2 = 0.926). Analyses of the composted MPs physicochemical properties indicated that MPs were aged gradually with molecular weights decrease from 18% to 27% and carbonyl index value increase from 0.23 to 0.52. Further investigation suggested that the microbially-mediated redox transformation of iron oxides could occur on the MPs surface accompanied by the production of abundant free radicals, thereby leading to the damage of MPs during composting. These results reveal the critical role of free radicals in MPs ageing under oxic/anoxic alternation conditions of composting and provide new insights into the bio-chemical mechanism of contaminant removal or transformation during sludge composting.