Advanced Science
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2023
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IF 15.1
Li Zhang,Qian Dong,Yumin Hao,Zihan Wang,Wenjuan Dong,Yang Liu,Yueping Dong,Hongpeng Wu,Shaomin Shuang,Chuan Dong,Zhuo Chen,Xiaojuan Gong
Single-atom nanozymes (SAzymes) with high catalytic activity exhibit the potential to disequilibrate the reactive oxygen metabolic balance in the tumor microenvironment (TME), which contains several endogenous reductive substances such as glutathione (GSH). Herein, a novel nano-assembly (CDs@Pt SAs/NCs@DOX) is first constructed using drug-primed platinum (Pt) single-atom or nanocluster nanozymes with a Pt loading of 34.8%, which exhibits prominent dual enzymatic activities to mimic peroxidase (POD) and glutathione oxidase (GSHOx). The unique GSHOx-like activity can efficiently scavenge GSH with a relatively low K m (1.04 m m ) and high V max (7.46 × 10 −6 m s −1 ), thus avoiding single oxygen ( 1 O 2 ) depletion. CDs@Pt SAs/NCs@DOX simultaneously demonstrates low-temperature photothermal therapy and TME- or laser-controlled disassembly and drug release, which can effectively regulate cellular redox homeostasis and achieve high tumor growth inhibition. These outcomes may provide promising strategies for the preparation of Pt SAzymes with multiple activities and variable-sized nano-assemblies, allowing for broader applications of SAzymes and nano-assemblies in the biomedical field.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
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IF 11.4
Yuyao Zhang,Wentao Yu,Jian Wang,Tingjie Zhan,Muhammad Aqeel Kamran,Kun Wang,Xiangyu Zhu,Chiheng Chu,Xiaoying Zhu,Baoliang Chen
Understanding the environmental transformation and fate of graphene oxide (GO) is critical to estimate its engineering applications and ecological risks. While there have been numerous investigations on the physicochemical stability of GO in prolonged air-exposed solution, the potential generation of reactive radicals and their impact on the structure of GO remain unexplored. In this study, using liquid-PeakForce-mode atomic force microscopy and quadrupole time-of-flight mass spectroscopy, we report that prolonged exposure of GO to the solution leads to the generation of nanopores in the 2D network and may even cause the disintegration of its bulk structure into fragment molecules. These fragments can assemble themselves into films with the same height as the GO at the interface. Further mediated electrochemical analysis supports that the electron-donating active components of GO facilitate the conversion of O2 to •O2– radicals on the GO surface, which are subsequently converted to H2O2, ultimately leading to the formation of •OH. We experimentally confirmed that attacks from •OH radicals can break down the C–C bond network of GO, resulting in the degradation of GO into small fragment molecules. Our findings suggest that GO can exhibit chemical instability when released into aqueous solutions for prolonged periods of time, undergoing transformation into fragment molecules through self-generated •OH radicals. This finding not only sheds light on the distinctive fate of GO-based nanomaterials but also offers a guideline for their engineering applications as advanced materials.
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Journal of Cleaner Production
·
2023
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IF 11.1
Jiajun Pan,Zhaopeng Xia,Haibao Zhang,Liwei Wu,Yang Lu,Yong Liu,Yujie Cao
Animal fibres are coloured using dyes to satisfy the individual needs; thus, dark animal fibres must be bleached. Compared with frequently used Fe 2+ -catalysed H 2 O 2 (Fe 2+ /H 2 O 2 ) bleaching, persulphate (PDS)/H 2 O 2 bleaching is advantageous owing to its high efficiency, low damage of fibre and environmental friendliness. Herein, different free radical species were precisely controlled by changing the pH of the PDS/H 2 O 2 solution and regulating the existence of NH 4 + . When NH 4 + was absent, sulphate radicals (·SO 4 − ) and hydroxyl radicals (·HO) could be produced at pH = 8–9 and superoxide anions (·O 2 − ) could be produced at pH = 10. In the presence of NH 4 + , ·SO 4 − and ·HO could be produced at pH = 8, and ·O 2 − was dominant in the solution when pH = 9–10. Black yak wool was used as the research object to demonstrate that the bleaching ability of the generated ·O 2 − was stronger than those of the generated ·SO 4 − and ·HO. Compared with that of the commercial product (prepared using Fe 2+ /H 2 O 2 bleaching), the bleaching time of the decolourised yak wool was reduced by 83.33% (from 24 to 4 h) without the catalysis by heavy metal ions . Meanwhile, the whiteness of the decolourised yak wool (72.31%) was close to that of the commercial product (78.79%). Furthermore, the damage to the cuticle layer and cortex of yak wool was low after bleaching. The breaking strength of the decolourised yak wool was 1.79 cN·dtex −1 , which only decreased by 17.13% compared with that of raw yak wool. These results hold great potential in developing environmental-friendly bleaching methods for dark animal fibres with high efficiency and low damage.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2023
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IF 6
Yuan-song Zhang,Xuechao Xu,Juanli Yang,Mengyuan Tan,Wenyuan Zhou,Lu Gao,Zhen-quan Yang
Cronobacter sakazakii in powdered infant formula (PIF) can cause infections in newborns that are life-threatening. Establishing a High-performance evaluation method for C. sakazakii in the PIF is urgently needed. In this study, a chromogenic system based on phage-directed immobilized nanozyme for colorimetric measurement of C. sakazakii in PIF was constructed . Initially, our acquired phage EspYZU15 was electrostatically immobilized on the surface of a palladium-based nanozyme to produce EspYZU15 directionally immobilized Pd (EspYZU15@Pd). EspYZU15@Pd possesses outstanding peroxidase-like properties, catalyzing the chromogenic reaction of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H 2 O 2 . The ability of EspYZU15@Pd to recognize and trap host bacteria allows C. sakazakii to specifically inhibit the TMB chromogenic process catalyzed by EspYZU15@Pd. Based on this detection strategy, a visual quantification method for C. sakazakii ranging from 3.2 × 10 2 to 3.2 × 10 7 CFU mL −1 was developed, yielding a low limit of detection (LOD) of 3.6 × 10 1 CFU mL −1 . This method was able to successfully detect C. sakazakii in PIF, with outstanding recoveries ranging from 95.8% to 104.9%. These characteristics indicate that the EspYZU15@Pd-based chromogenic system has considerable promise for the colorimetric determination of C. sakazakii in PIF.
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ACS Nano
·
2023
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IF 17.1
Wenzhe Xu,Yang Chen,Ruixu Yang,Yiying Fu,Wanxin Zhuang,Yonggang Wang,Yi Liu,Hao Zhang
Nanoprecipitation, which is achieved through the diffusion and precipitation of drug molecules in blended solvent and antisolvent phases, is a classic route for constructing nanodrugs (NDs) and previously directed by diffusion-controlled theory. However, the diffusion-controlled mechanism is out of date in the recent preparation of self-delivery supramolecular NDs (SDSNDs), characterized by the construction of drug nanoparticles through supramolecular interactions in the absence of carriers and surfactants. Herein, a “reaction”-like complement, contributed from supramolecular interactions, is proposed for the preparation of naphthoquinone SDSNDs. Different from the diffusion-controlled process, the formation rate of SDSNDs via the “reaction”-like process is almost constant and highly dependent on the supramolecular interaction-determined Gibbs free energy of molecular binding. Thus, the formation rate and drug availability of SDSNDs are greatly improved by engineering the supramolecular interactions, which facilitates the preparation of SDSNDs with expected sizes, components, and therapeutic functions. As a deep understanding of supramolecular-interaction-involved nanoprecipitation, the current “reaction”-like protocol not only provides a theoretical supplement for classic nanoprecipitation but also highlights the potential of nanoprecipitation in shaping self-assembled, coassembled, and metal-ion-associated SDSNDs.
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Materials Horizons
·
2023
·Vol. 10
·期 10
·4303-4316
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IF 13.3
Xingqi Luo,Zhaoyang Yuan,Xiangyan Xie,Yuanjie Xie,Hongyi Lv,Jin Zhao,Hao Wang,Yuanji Gao,Lijuan Zhao,Yi Wang,Jinrong Wu
Hydrogels with rapid gelation ability and robust mechanical properties are highly desirable for nascent applications in biomedical, wearable electronic, industrial and agricultural fields. However, current rapid-gelation hydrogels are compromised by poor mechanical properties, complex design of precursor molecular structures and limited precursor species. Herein, we propose a facile and universal strategy to achieve rapid gelation, strengthening and toughening of free-radical polymerized hydrogels by introducing cheap and accessible amino acids. Amino acids not only activate persulfate to quickly produce free radicals and thus induce fast free radical polymerization, but also can form strong hydrogen bonds with the network chains to strengthen and toughen the hydrogels. For example, with the presence of L-serine, the acrylamide (AM) monomer shows rapid gelation within tens of seconds, and moreover the resulting hydrogel reaches a tensile strength of 0.45 MPa and a breaking strain of 2060%. More importantly, owing to the extremely dynamic feature of the hydrogen bonds between L-serine molecules and network chains, the hydrogel possesses the advantages of low hysteresis, rapid self-recovery capability and outstanding fatigue resistance. Furthermore, this strategy is general to a wide range of amino acids and monomers. We also demonstrate that this rapid, controllable and universal strategy for the fabrication of mechanically robust hydrogels holds tremendous potential for diverse practical applications, such as flexible electronic sensors and ultraviolet (UV)-blocking artificial skins.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2023
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IF 6.8
Qingyun He,Wuduo Zhao,Peiru Luo,Lingyun Wang,Qiannan Sun,Wenfen Zhang,Dan Yin,Yanhao Zhang,Zongwei Cai
As one of the most important transportation hubs and industrial bases in China, Zhengzhou has suffered from serious PM 2.5 pollution for a long time. However, the investigation of contamination status and possible exposure risks of environmentally persistent free radicals (EPFRs) in PM 2.5 from Zhengzhou is rare. In this work, a comprehensive study of pollution levels, seasonal variations, sources, and potential health risks of PM 2.5 -bound EPFRs in Zhengzhou was conducted for the first time. The atmospheric concentrations of EPFRs in PM 2.5 from Zhengzhou ranged from 1.732 × 10 12 spin m −3 to 7.182 × 10 14 spin m −3 between 2019 and 2020. Relatively serious contamination was noticed in winter and spring. Primary fossil fuel combustion and Fe-mediated secondary formation were apportioned as possible sources of PM 2.5 -bound EPFRs in Zhengzhou. Moreover, to avert the bias of the toxicity assessment induced by utilization of incompletely extracted EPFRs from sample filter, simulatively generated EPFRs were applied to toxicological evaluations (cell viability and reactive oxygen species assays). Corresponding experimental dosages were based on the estimated adults’ annual exposure amounts of EPFRs in real PM 2.5 samples. The results elucidated that EPFRs might cause growth inhibition and oxidative stress of human lung cells, suggesting the possible exposure-induced health concerns for local people in Zhengzhou. This study provides practical information of real contamination status of PM 2.5 -bound EPFRs in Zhengzhou, which is favorable to local air pollution control and reduction of exposure risks on public health in central China.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lin Chen,Xia Jiang,Shenggui Ma,Wenhua Chen,Bo Xu,Zhongde Dai,Wenju Jiang,Yue Peng,Junhua Li
In this study, Edge-N-rich carbon nanosheet @ porous biochar (NCN@PB) was synthesized successfully from waste biomass self-assembly in a simple and green approach. The accessible and efficient utilization of edge-N enriched on the surface, together with the hybrid structure of NCN@PB improved the H 2 S oxidation capacity up to 390.1 mg/g at room temperature, reflecting an 8-fold enhancement compared with the blank biochar. The Density functional theory calculation, in-situ DRIFTS, and the characterization results further uncovered the desulfurization mechanism of active sites. Edge-N species decreased the barriers in critical steps governing H 2 S catalytic oxidation, i.e., H 2 S dissociation and O 2 activation, especially the pyrrolic N. This strategy is beneficial for the development of surface engineering on metal-free catalysts and provides a new idea for improving the catalytic combustion activity of N-doped biochar.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Yue Wang,Lele Qiao,Xueyi Zhang,Zhenglong Liu,Tielong Li,Haitao Wang
Biochar-based nanocomposites are recognized as promising catalysts for peroxymonosulfate (PMS) activation due to their cost-effectiveness, large surface area, and desirable activity. However, their conventional preparation involves laborious and energy-consuming high-temperature pyrolysis. In this study, we introduce an efficient approach to synthesize FeCu@BC nanocomposites using iron and copper chlorides with green tea via a mechanochemical method. Characterization results show that copper incorporation enhances the defect degree of biochar, increasing oxygen vacancies in FeCu@BC. Remarkably, FeCu@BC exhibits an outstanding efficiency of 92.24% in degrading TC, achieving more than 85% TC removal even under challenging conditions with varying pH levels and competing ions, making it a promising catalyst for practical applications. Through detailed investigations, we identify O 2 − and 1 O 2 as the primary active species responsible for TC degradation, supported by quenching and EPR tests. Furthermore, copper doping significantly improves electron transfer between FeCu@BC and PMS, promoting PMS activation during degradation. XPS analysis provides insights into the transformation of doped copper species, acting as potential active sites that facilitate PMS decomposition to generate O 2 − and 1 O 2 . With significant advantages in cost-effectiveness and avoidance of energy-intensive pyrolysis, the mechanochemically synthesized FeCu@BC nanocomposites hold great promise for wide application in efficient wastewater treatment and environmental remediation.
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CHEMOSPHERE
·
2023
·
IF 8.8
Huiqi Zheng,Xiaorong Meng,Jiao Wu,Danghao Liu,Shanshan Huo
Heavy metal pollution can significantly harm water systems and human health. Combining photoelectrocatalytic (PEC) and nanofiltration (NF) membrane separation technologies can effectively remove heavy metal ions from wastewater. In this study, a water bath method was used to form SrF 2 /Ti 3 C 2 T x (ST) nanoparticles on the surface of polyvinylidene fluoride (PVDF) membranes and an additional polyamide (PA) functional layer was formed at the interface by crosslinking. ST@PA composite NF membranes (STPP) with good photocatalytic performance were obtained. The separation and catalytic properties of the STPP membranes were controlled by the ST content, which modifies the surface structure and properties of the membranes. The membrane with optimal ST crosslinking exhibited a water contact angle of 50.8°, pure water flux of 24.6 L·m −2 ·h −1 ·bar −1 , and rejection rates of Mn 2+ , Ni 2+ , Cu 2+ , and Zn 2+ of 98.8%, 95.3%, 95.7%, and 97.3%, respectively, under PEC-assisted separation with visible light illumination from a Xe lamp (300 W) and an applied voltage (2 V). The STPP membranes showed improved rejection rates of heavy metal ions under PEC-assisted operation. The mechanism for the improved membrane performance under PEC conditions was preliminarily clarified considering the relationship between the photocatalytic and filtration properties of STPP membranes along with the influence of light irradiation and an external voltage on the heavy metal ions. The generation of electrons, holes, superoxide radicals, and hydroxyl radicals during membrane operation enhances the rejection rates of heavy metal ions. Based on these results, STPP membranes are considered a promising technology for industrial applications in heavy metal removal.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Liangliang Wang,Chenhang Zhang,Tongzhou Xu,Lirong Lv,Zhongguo Zhang,Can He
A wet scrubbing – catalytic ozonation (WCO) process with activated carbon (AC) loaded MnOx (MnOx/AC) as the catalyst was developed, based on volatile organic compounds (VOCs) can be efficiently removed. The mineralization efficiency, degradation pathway and mechanism, and effects of the process operating parameters were investigated in detail using toluene as the target pollutant. The results show that the average removal efficiency of toluene reached 71.82 % within 90 min under optimal conditions (C Toluene = 100 mg/m 3 ; C O3 = 1 mg/L; catalyst loading = 5 g/L; pH = 7; gas flow = 500 mL/min), which outperformed that of the gaseous system. Quenching experiments and electron spin resonance spectroscopy indicate that OH and O 2 − are the two main reactive oxygen species (ROSs) in the system, which facilitate the opening of the benzene ring and significantly reduce by-products. The intermediates of toluene degradation were identified by proton-transfer reaction time-of-flight mass spectroscopy (PTR-TOF-MS). The results indicate that most of the intermediates generated in the system are captured in water rather than being emitted into the atmosphere. In the pilot-scale experiments, the WCO process exhibited a stable VOC removal efficiency (≥61.05 %) for 10 d in the treatment of actual low-concentration VOCs. Therefore, in this study, an effective process for the removal of low-concentration VOCs is proposed, which can be used for multiple VOC treatments.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yilin Wu,Xinlan Zhu,Dongyang Miao,Jun Song,Shaohai Fu,Jichao Zhang
Oily wastewater, resulting from oil recovery, petrochemical industries, or accidents, poses a significant threat to the aquatic environment. Membrane separation technology can offer unprecedented opportunities for highly efficient water remediation but at the cost of poor permeability and serious oil fouling. Here, we report a faveolate nanofibrous membrane through the steric growth of bismuth oxybromide-bismuth oxyiodide nanoflakes on the TiO 2 /polypyrrole nanofibers. The spatially faveolate cells create highly covered confined spaces that efficiently capture and coalesce nanosized oil droplets, thus achieving substantial selectivity for micron porous membranes. The faveolate membranes are capable of efficiently separating various oil-in-water emulsions, particularly nanoscale surfactant-stabilized emulsions with a high permeation flux of 6075 L m -2 h −1 and a good separation efficiency of 99.95 %. Moreover, the membranes with multi-heterostructure act as efficient photocatalysts, giving rise to visible light-induced sufficient fouling-tolerant property with nearly zero irreversible oil fouling. This study could provide a novel strategy for developing a new generation of membranes with high performance and long service lifetime for oily sewage remediation.
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危险品化学品经营许可证（带存储）