CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Jiameng Wang,Hao Cheng,Weiyi Chen,Peide Han,Xiaohong Yao,Bin Tang,Wangping Duan,Pengcui Li,Xiaochun Wei,Paul K. Chu,Xiangyu Zhang
Antibacterial hydrogels with injectable and self-healing properties have attracted much attention in the field of wound dressings because they not only can prevent bacterial infections, but also meet the basic needs for wound healing. However, how to achieve high antibacterial efficacy and low drug resistance for hydrogels is still a challenge. Herein, an injectable, self-healing, near-infrared (NIR) photosensitive antibacterial hydrogel composed of CuS-grafted-curcumin ( [email protected] ) and carboxymethyl cellulose modified with aldehyde groups and hydroxypropyl trimethyl ammonium chloride chitosan is prepared for wound dressings. The p-n junction formed between curcumin and CuS promotes separation of electron-hole pairs, enhances the mobility of photogenerated charges, and destroys the conjugated structure of curcumin simultaneously consequently increasing the photocatalytic activity. [email protected] is immobilized and distributed uniformly in the hydrogel via the π-π conjugation ring. The hybrid hydrogel exhibits excellent antibacterial activity after irradiation with 808 NIR light for 10 min due to the enhanced photodynamic and photothermal antibacterial effects. In addition, the hybrid structure improves the biocompatibility of CuS and expedites infected-wound healing at a mild temperature of 45 ℃. This organic/inorganic hybrid is shown to be an excellent wound dressing for the treatment of bacterial-infected wounds.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2022
·Vol. 30
·期 5
·11959-11977
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IF 5.19
He Haonan,Zhao Junfeng
In this study, the degradation efficiency and reaction mechanisms of diclofenac (DCF), a nonsteroidal anti-inflammatory drug, by the combination of ferrate (Fe(VI) and peroxymonosulfate (PMS) (Fe(VI)/PMS) were systematically investigated. The higher degradation efficiency of DCF in Fe(VI)/PMS system can be obtained than that in alone persulfate (PS), Fe(VI), PMS, or the Fe(VI)/PS process at pH 6.0. DCF was efficiently removed in Fe(VI)/PMS process within a wide range of pH values from 4.0 to 8.0, with higher degradation efficiency in acidic conditions. The increasing reaction temperature (10 to 30 ℃), Fe(VI) dose (6.25 to 100 µM), or PMS concentration (50 to 1000 µM) significantly enhanced the DCF degradation. The existences of HCO 3 ¯, Cl¯, and humic acid (HA) obviously inhibited the DCF removal. Electron paramagnetic resonance (EPR), free radical quenching, and probing experiments confirmed the existence of sulfate radicals (SO 4 • ¯), hydroxyl radicals ( • OH), and Fe(V)/ Fe(IV), which are responsible for DCF degradation in Fe(VI)/PMS system. The variations of TOC removal ratio reveal that the adsorption of organics with ferric particles, formed in the reduction of Fe(VI), also were functioned in the removal process. Sixteen DCF transformation byproducts were identified by UPLC-QTOF/MS, and the toxicity variation was evaluated. Consequently, eight reaction pathways for DCF degradation were proposed. This study provides theoretical basis for the utilization of Fe(VI)/PMS process. Graphical abstract
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Wanfeng Wu,Yanan Qin,Yan Fang,Yukun Zhang,Shuxuan Shao,Fanxing Meng,Minwei Zhang
Currently, graphene quantum dots (GQDs) are widely used as antibacterial agents, and their effects are dependent on the reactive oxygen species (ROS) generated by photodynamic and peroxidase activities. Nevertheless, the supply of substrates or light greatly limits GQDs application. Besides, due to compensatory mechanisms in bacteria, comprehensive analysis of the molecular mechanism underlying the effects of GQDs based on cellular-level experiments is insufficient. Therefore, N-GQDs with inherent excellent, broad-spectrum antibacterial efficacy under acidic conditions were successfully synthesized. Then, via multi-omics analyses, the antibacterial mechanisms of the N-GQDs were found to not only involve generation ROS but also be associated with changes in osmotic pressure , interference with nucleic acid synthesis and inhibition of energy metabolism. More surprisingly, the N-GQDs could destroy intracellular acid-base homeostasis , causing bacterial cell death. In conclusion, this study provides important insights into the antibacterial mechanism of GQDs, offering a basis for the engineering design of antibacterial nanomaterials .
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Small
·
2022
·Vol. 18
·期 45
·2203619
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IF 15.153
Bin Li,Rui Shu,Wenyu Dai,Fan Yang,Hui Xu,Xiuyuan Shi,Yunfei Li,Ding Bai,Weizhong Yang,Yi Deng
Diabetic infectious micromilieu (DIM) leads to a critical failure rate of osseointegration by virtue of two main peculiarities: high levels of topical glucose and inevitable infection. To tackle the daunting issue, a bioheterojunction-engineered orthopedic polyetheretherketone (PEEK) implant consisting of copper sulfide/graphene oxide (CuS/GO) bioheterojunctions (bioHJs) and glucose oxidase (GO x ) is conceived and developed for DIM enhanced disinfection and boosted osseointegration. Under hyperglycemic micromilieu, GO x can convert surrounding glucose into hydrogen peroxide (H 2 O 2 ). Then, upon infectious micromilieu, the bioHJs enable the catalyzation of H 2 O 2 to highly germicidal hydroxyl radical (·OH). As a result, the engineered implants massacre pathogenic bacteria through DIM twin-engine powered photo-chemodynamic therapy in vitro and in vivo. In addition, the engineered implants considerably facilitate cell viability and osteogenic activity of osteoblasts under a hyperglycemic microenvironment via synergistic induction of copper ions (Cu 2+ ) and GO. In vivo studies using bone defect models of diabetic rats at 4 and 8 weeks further authenticate that bioHJ-engineering PEEK implants substantially elevate their osseointegration through biofilm elimination and vascularization, as well as macrophage reprogramming. Altogether, the present study puts forward a tactic that arms orthopedic implants with DIM twin-engine powered antibacterial and formidable osteogenic capacities for diabetic stalled osseointegration.
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Water
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2022
·Vol. 14
·期 18
·2811
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IF 3.53
Zhixiong Liu,Wenlei Qin,Lei Sun,Huiyu Dong,Xiangjuan Yuan,Fei Pan,Dongsheng Xia
The degradation of acyclovir (ACY) and atenolol (ATL) in the UV/peroxydisulfate (UV/PDS) process has been systematically considered, focusing on the degradation kinetics, theoretical models, and reaction pathways via applying a microfluidic UV reaction system. The removal efficiencies of ACY and ATL were >94.8%, and the apparent degradation rate constants (kobs) were 0.0931 and 0.1938 min−1at pH 6.0 in the UV/PDS system. The sulfate radical (SO4•−) and hydroxyl radical (•OH) were identified as the major reactive radicals. The pH-dependent reaction rate constants of ACY and ATL with•OH and SO4•−were measured via the competing kinetics. Meanwhile, the contributions of•OH and SO4•−for ACY and ATL degradation were calculated by the radical steady-state hypothesis, and the results revealed that SO4•−occupied a decisive position (>84.5%) for the elimination of ACY and ATL. The contribution of•OH became more significant with the increasing pH, while SO4•−was still dominant. Moreover, ACY and ATL degradation performance were systematically evaluated via the experiments and Kintecus model under different operational parameters (Cl−, Br−, HCO3−, NOM, etc.) in the UV/PDS process. Furthermore, the plausible reaction pathways of ACY and ATL were elucidated based on the Fukui function theory and ultra-performance liquid chromatography-tandem quadrupole time-of-flight mass spectrometry (UPLC-QTOF-MS) analysis. The UV/PDS process has been demonstrated to be an efficient and potential application for micropollutants mitigation.Keywords:UV/PDS;micropollutants;radical contribution rates;kinetic models;degradation pathways
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Cheng Yu,Xiaoxi Zhu,Abdelkader Mohamed,Ke Dai,Peng Cai,Shilin Liu,Qiaoyun Huang,Baoshan Xing
Biochar can act as a shuttle to accelerate the extracellular electron transfer (EET) by exoelectrogens. However, it is poorly understood how the persistent free radicals (PFRs) in biochar affected EET and the redox reaction. Herein, the effects of the biochar and chitosan modified biochar (CBC) on the Cr(VI) bioreduction by Shewanella oneidensis MR-1 (MR-1) was investigated. Kinetic study indicated that the Cr(VI) bioreduction rate constant by MR-1 was increased by 1.8–33.7 folds in the presence of biochar, and by 2.7–60.2 folds in the presence of CBC, respectively. Moreover, Cr(VI) bioreduction rates increased with the decreasing pH. Results suggested that the electrostatic attraction between Cr(VI) and redox-active particles could accelerate the EET by c -cytochrome due to the promotion of the Cr(VI) migration from aqueous phase to biochar or CBC. Electron paramagnetic resonance analysis suggested that the PFRs affected the electron transfer from the ·O 2 - generated by MR-1 to Cr(VI) and accelerate the Cr(VI) bioreduction. Remarkably, in the presence of PFRs, this electron shuttling process was dependent on the non-metal-reducing respiratory pathway. Our results offer new insights that free radicals may be widely involved in the EET and strongly impact on the redox reaction in the environment.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2022
·
IF 11.357
Xiao-Chi Feng,Zi-Jie Xiao,Hong-Tao Shi,Bai-Qin Zhou,Yong-Mei Wang,Hui-Zhong Chi,Xiao-Hang Kou,Nan-Qi Ren
Current research has widely applied heteroatom doping for the promotion of catalyst activity in peroxymonosulfate (PMS) systems; however, the relationship between heteroatom doping and stimulated activation mechanism transformation is not fully understood. Herein, we introduce nitrogen and sulfur doping into a Co@rGO material for PMS activation to degrade tetracycline (TC) and systematically investigate how heteroatom doping transformed the activation mechanism of the original Co@rGO/PMS system. N was homogeneously inserted into the reduced graphene oxide (rGO) matrix of Co@rGO, inducing a significant increase in the degradation efficiency without affecting the activation mechanism transformation. Additionally, S doping converted Co3O4 to Co4S3 in Co@rGO and transformed the cooperative oxidation pathway into a single non-radical pathway with stronger intensity, which led to a higher stability against environmental interferences. Notably, based on density functional theory (DFT) calculations, we demonstrated that Co4S3 had a higher energy barrier for PMS adsorption and cleavage than Co3O4, and therefore, the radical pathway was not easily stimulated by Co4S3. Overall, this study not only illustrated the improvement due to the heteroatom doping of Co@rGO for TC degradation in a PMS system but also bridged the knowledge gap between the catalyst structure and degradation performance through activation mechanism transformation drawn from theoretical and experimental analyses.
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Journal of Environmental Chemical Engineering
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2022
·
IF 7.968
Qinghui Yu,Guotao Liu,Jinhang Shi,Ting wen,Lei Li
It is generally challenging to design efficient, low-cost, and environmentally friendly persulfate catalytic materials for wastewater purification. We report a simple strategy to synthesize a steel converter slag-sludge carbon catalyst with steel converter slag as a template, suspended sludge as a precursor, and one-step pyrolysis . A persulfate activator was used to remove phenol and organic matter from actual wastewater leachate. The catalyst had a shell structure, a large surface area, abundant adsorption groups, and polymetallic catalytic capacity. The catalytic capacity depended on zero-valent iron (Fe 0 ), which effectively leached active Fe 2+ composite to produce hydroxyl and persulfate radicals by activating persulfate. The maximum phenol degradation was 94.5% in 55 min with 2 mM persulfate, 100 mg/L catalyst, and 20 mg/L phenol, which was 6 and 44 times greater than that of pure sludge carbon and steel converter slag, respectively. For actual wastewater leachate, the maximum removal rate of total organic carbon was 77.75% with 0.15 M persulfate, 50 g/L catalyst, and 1125 mg/L total organic carbon; all the fluorescent substances were removed. This work provides a new approach for designing persulfate catalysts derived from green resources. Further, our approach is practical for the treatment of wastewater that has high concentrations of organic material.
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ATMOSPHERIC ENVIRONMENT
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2022
·
IF 5.755
Jinwen Li,Qingcai Chen,Dongjie Guan
Atmospheric aerosols contain organic compounds that can form triplet organics ( 3 C*) excited by sunlight, which plays a significant role in the aging process of aerosols. The formation characteristics of 3 C* of aerosol components with different polarities were investigated, including highly polar water-soluble matter (HP-WSM), humic-like substances (HULIS), and methanol-soluble matter (MSM). Carbon analysis, probe method and electron paramagnetic resonance were used to investigate the photochemical properties of ambient samples. The coupling effect of generation of 3 C* and reactive oxygen species (ROS) between different aerosol components was also examined. The results showed that the 3 C* generation characteristics are strongly dependent on the polarity of these components. HULIS has the strongest generation ability of 3 C*, and the MSM contributes the most to the total generation of 3 C*. It was found that the high-energy triplet states ( E T ≥ 250 kJ mol −1 ) of HULIS and HP-WSM components account for up to 80% of the water soluble components. These 3 C* have an important contribution to the photochemically generation of ROS, and the generated ROS of different components are also different, which is determined by the chromophore composition of complex organic compounds. A tyrosine-like chromophore is the main substance leading to the formation of water-soluble 3 C*, while the highly oxidized HULIS chromophore plays a leading role in the water-insoluble component. This study also found that there is a coupling effect between HP-WSM and HULIS on 3 C* and ROS generation. The generation rate of 3 C* increases by about 40% after mixing, but the generation of 1 O 2 is severely reduced. In general, this study provided deep insights into the generation characteristics and aging impact of the triplet state on atmospheric aerosols.
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Nanoscale
·
2022
·Vol. 14
·期 39
·14471-14481
·
IF 8.307
Danyang Li,Enna Ha,Jingge Zhang,Luyang Wang,Junqing Hu
Near-infrared light-induced catalysts are considered to be potential nanoagents for tumor therapy. Cerium (Ce) is a non-biotoxic lanthanide element and exhibits variable valence states for catalytic reactions. In this work, we report a one-step hydrothermal synthesis for Ce-doped MoOx (CMO) nanomaterials. The obtained CMO nanomaterials show high absorption in the NIR II regime and a high photothermal conversion efficiency of 67.7% (1064 nm). Moreover, due to the doping of Ce element, the consumption of hydrogen peroxide (H2O2) and glutathione (GSH) is boosted which enhances the chemodynamic and photodynamic therapy simultaneously. Under NIR II laser irradiation, the designed CMO nanocatalysts induce metabolism disruption and mitochondrial damage in the tumor cells. As-prepared CMO nanomaterials also show good biocompatibility and pH-responsive degradation behavior, which can be degraded rapidly under alkaline conditions (pH = 7.4) and remain stable in acidic solution (pH = 5.6). These properties make CMO nanomaterials ideal biodegradable nanotheranostic agents for synergistic chemodynamic–photodynamic–photothermal antitumor therapy.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2022
·
IF 5.876
Yi Chen,Shuai Dong,Shiyue Wei,Shiruo Zhang,Jiaxin Zhang,Jinchuan Gu
Mesoporous sodalite (SOD) zeolite was fabricated from industrial waste lithium silica fume (LSF) through the reactive oxygen species (ROS) method under ultraviolet (UV) irradiation without the template. Persulfate (PS) and peroxymonosulfate (PMS) under UV irradiation would further induce ROS generation and result in faster crystallization to obtain highly crystalline and abundant mesopores (mesopore volume, Vmes＞0.34 cm³/g) SOD within 2 h. The ROS produced in the synthesis system were detected by electron spin resonance (EPR), and the results revealed that ·OH, O 2 · − , 1 O 2, and SO 4 · − may be related to the accelerating process. Zeolite produced superior adsorptive capacity (112.4 mg/g) and reusability in copper ion (Cu(II)) adsorptive experiments. The abundance of mesoporous in zeolite facilitates the removal of Cu(II) by ion exchange and hydroxyl complexation. This work opens up a new route for green and fast synthesis of zeolite and highly efficient Cu(II) removal adsorbent.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Kexuan Gao,Li-an Hou,Xiaoqiang An,Doudou Huang,Yu Yang
The rapid recombination rate of photogenerated charges make the rational design of high-performance stable photocatalysts challenging. Herein, the features of heterojunctions, oxygen vacancies (OVs), and MXene quantum dots (MQDs) were simultaneously collected in CBM (gC 3 N 4 /BiOBr/MXene) using a simple solvothermal method for the first time. OVs promoted the chemisorption of O 2 , MQDs not only accelerated electron transport but also promoted a photogenerated charge to selectively generate singlet oxygen, 99% of the tetracycline hydrochloride (TC-HCl) was degraded by CBM within 30 min under visible light irradiation. Thirteen intermediates and possible photocatalytic degradation pathways were proposed. It was discovered that CBM is nontoxic to the environment but can swiftly produce an excellent antibacterial effect when exposed to visible light irradiation. This research provides fresh insights into the effective removal of organic pollutants from water by combining cutting-edge defect engineering and quantum dot doping technology in photocatalytic heterojunctions.
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