ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2022
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IF 7.129
Chao Zhao,Hu Zhang,Jingjing Zhou,Qiwei Liu,Qiang Lu,Ying Zhang,Xiaojin Yu,Shizhi Wang,Ran Liu,Yuepu Pu,Lihong Yin
Esophageal squamous cell carcinoma (ESCC) is an environment-relevant malignancy with a high mortality. Nitrosamines, a class of nitrogen-containing environmental carcinogens, are widely suggested as a risk factor for ESCC. However, how nitrosamines affect metabolic regulation to promote ESCC tumorigenesis is largely unknown. In this study, the transition trajectory of serum metabolism in the course of ESCC induced by N-nitrosomethylbenzylamine (NMBA) in rats was depicted by an untargeted metabolomic analysis, and the potential molecular mechanisms were revealed. The results showed that the metabolic alteration in rats was slight at the basal cell hyperplasia (BCH) stage, while it became apparent when the esophageal lesion developed into dysplasia (DYS) or more serious conditions. Moreover, serum metabolism of severe dysplasia (S-DYS) showed more similar characteristics to that of carcinoma in situ (CIS) and invasive cancer (IC). Aberrant nicotinate (NA) and nicotinamide (NAM) metabolism, tryptophan (TRP) metabolism, and sphingolipid metabolism could be the key players favoring the malignant transformation of esophageal epithelium induced by NMBA. More particularly, NA and NAM metabolism in the precancerous stages and TRP metabolism in the cancerous stages were demonstrated to replenish NAD + in different patterns. Furthermore, both the IDO1-KYN-AHR axis mediated by TRP metabolism and the SPHK1-S1P-S1PR1 axis by sphingolipid metabolism provided an impetus to create the pro-inflammatory yet immune-suppressive microenvironment to facilitate the esophageal tumorigenesis and progression. Together, these suggested that NMBA exerted its carcinogenicity via more than one pathway, which may act together to produce combination effects. Targeting these pathways may open up the possibility to attenuate NMBA-induced esophageal carcinogenesis. However, the interconnection between different metabolic pathways needs to be specified further. And the integrative and multi-level systematic research will be conducive to fully understanding the mechanisms of NMBA-induced ESCC.
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Journal of Environmental Sciences
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2022
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IF 6.796
Yong Wang,Cheng Liu,Haoyun Hu,Qiujun Lu,Haiyan Wang,Chenxi Zhao,Fuyou Du,Ningli Tang
The construction and application of novel highly efficient photocatalysts have been the focus in the field of environmental pollutant removal . In this work, a novel CuFe 2 O 4 /Bi 12 O 17 Cl 2 photocatalysts were synthesized by simple hydrothermal and chemical precipitation method. The fabricated CuFe 2 O 4 /Bi 12 O 17 Cl 2 composite exhibited much higher photocatalytic activity than pristine CuFe 2 O 4 and Bi 12 O 17 Cl 2 in the removal of bisphenol A (BPA) under visible-light illumination, which ascribed to the intrinsic p-n junction of CuFe 2 O 4 and Bi 12 O 17 Cl 2 . The photocatalytic degradation rate of BPA on CuFe 2 O 4 /Bi 12 O 17 Cl 2 with an optimized CuFe 2 O 4 content (1.0 wt.%) reached 93.0% within 30 min. The capture experiments of active species confirmed that the hydroxyl radicals (•OH) and superoxide radicals (•O 2 − ) played crucial roles in photocatalytic BPA degradation process. Furthermore, the possible degradation mechanism and pathways of BPA was proposed according to the detected intermediates in photocatalytic reaction process.
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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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Nature Communications
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2022
·Vol. 13
·期 1
·1-9
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IF 17.694
Zhang Xiaoran,Zhu Xiaorong,Bo Shuowen,Chen Chen,Qiu Mengyi,Wei Xiaoxiao,He Nihan,Xie Chao,Chen Wei,Zheng Jianyun,Chen Pinsong,Jiang San Ping,Li Yafei,Liu Qinghua,Wang Shuangyin
Electrocatalytic urea synthesis emerged as the promising alternative of Haber–Bosch process and industrial urea synthetic protocol. Here, we report that a diatomic catalyst with bonded Fe–Ni pairs can significantly improve the efficiency of electrochemical urea synthesis. Compared with isolated diatomic and single-atom catalysts, the bonded Fe–Ni pairs act as the efficient sites for coordinated adsorption and activation of multiple reactants, enhancing the crucial C–N coupling thermodynamically and kinetically. The performance for urea synthesis up to an order of magnitude higher than those of single-atom and isolated diatomic electrocatalysts, a high urea yield rate of 20.2 mmol h −1 g −1 with corresponding Faradaic efficiency of 17.8% has been successfully achieved. A total Faradaic efficiency of about 100% for the formation of value-added urea, CO, and NH 3 was realized. This work presents an insight into synergistic catalysis towards sustainable urea synthesis via identifying and tailoring the atomic site configurations.
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PROGRESS IN ORGANIC COATINGS
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2022
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IF 6.206
Jiayao Zhang,Minzhe Peng,Zhiyong Li,Yajiang Huang,Guangxian Li
Non‑silicone release agents with good temperature resistance and low release force are highly desired in the electronics industry to meet quality and safety regulations. In this study, a series of poly(vinyl n-octadecyl carbamate) (PVODC) containing different amounts of long alkyl side chains were synthesized based on poly(vinyl alcohol) (PVA) and octadecyl isocyanate (ODI). The effects of alkyl side chains on the chemical structure , crystallization, chain stacking, and thermal stability of PVODCs were explored by spectroscopy, scattering/diffraction, and thermal analysis techniques. The results showed that the alkyl side chains of PVODCs formed hexagonally stacked lamellar structures at room temperature. Introducing more side chains gradually destroyed the regularity of PVODC chains, leading to lower melt viscosity, melting points, and thermal stability. The surface energy and peel strength of PVODC-coated release films decreased and then leveled off as more side chains were introduced. The optimal degree of graft substitution was determined to be 45 %, at which the PVODC achieved a good balance of release performance, melting point, and cost as a non‑silicone release agent.
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Frontiers in Chemistry
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2022
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IF 5.545
Yan Long,Wang Xianjie,Wang Yufei,Li Jian,Liu Qianqian,Zhong Xiang,Chang Yuan,Li Qingchao,Verma Santosh Kumar
Contamination of phenolic compounds has devastating effects on the environment. Therefore, its harmless treatment and recycling have received extensive attention. Herein, a novel method for preparing N-S doped phenolic resin (NSPR) from phenols, N and S groups in semi-coking wastewater, and formaldehyde are developed. The KOH is consequently incorporated into the NSPR through simultaneous carbonization and activation in a single step to produce porous carbon material (NSPC). The as-obtained NSPC exhibits a high specific capacitance of 182 F g−1 at 0.5 A g−1, a high energy density of 9.1 Wh kg−1 at a power density of 0.15 kW kg−1, and remarkable cycling stability in aqueous KOH electrolyte. This outstanding electrochemical performance is attributed to its ultrahigh specific surface area (SSA, 2,523 m2 g−1), enormous total pore volume (Vt, 1.30 cm3 g−1), rational pore structure, and N-S heteroatom self-doping (0.76 at% N and 0.914 at% S), which ensures adequate charge storage, rapid electrolyte ion diffusion, and contributed pseudo-capacitance. This work not only provides a facile method for transforming phenolic wastewater into high-value products but also offers a cost-effective and high-performance porous carbon material for supercapacitors.
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FUEL
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2022
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IF 8.035
Yang Liu,Xiaobei Cheng,Yuchen Ya,Bowen Wang,Pu Zhang,Kai Zhang,Yishu Xu
PODE 3 , with the molecular formula of CH 3 O(CH 2 O) 3 CH 3 , is considered a highly competitive alternative fuel due to the absence of C C bond and its high oxygen content, and have been shown to significantly reduce soot emission when applied as a diesel fuel additive. However, the effect of PODE 3 addition on the oxidation reactivity of soot generated in the flame remains unclear which is of great importance for the optimal design of the post-treatment devices during its application. In this work, the impact of PODE 3 (0 %, 10 %, and 20 % by volumetric fraction) addition on the oxidation reactivity of soot at different maturity and oxidation degrees in n -heptane/toluene co-flow diffusion flames was specially investigated combining information on thermogravimetric analysis, high-resolution transmission electron microscope, and Raman spectroscopy. Results showed that PODE 3 substitution significantly shrank soot generation region, and increased the flame temperatures before height above burner (HAB) < 45 mm. The addition of PODE 3 improved the soot oxidation reactivity, which had a strong ability to hinder the growth of the microcrystalline carbon layers and resulted in a high content of amorphous carbon in soot particles. Specifically, it had more significant impacts on the soot in the oxidation stage than the surface growth stage. These can be explained that with PODE 3 addition, on the one hand, the “reliable carbon atom” for soot formation is significantly reduced and the amount of oxidizing species is increased, resulting in a smaller particle size and a higher content of disordered and amorphous carbon in soot particles. On the other hand, the flame temperatures increased where HAB < 45 mm, which would promote the soot formation reactions. The combined effects of these factors make PODE 3 have more significant inhibitory impacts in reactivity of soot sampled at oxidation stage than that at surface growth stage. Therefore, the impact of PODE 3 addition on soot nanostructures and oxidation reactivity is not only reflected in its chemical effect but also in temperature effect.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 30
·期 8
·20790-20803
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IF 5.19
Huang Hua,Tao Xin,Niu Zhirui,Shan Baoqin,Liu Yu,Ren Jingyu
To improve the photocatalytic performance of Mn 0.6 Zn 0.4 Fe 2 O 4 (MZFO) and ZnIn 2 S 4 (ZIS) for organic pollutants, the p-n MZFO@ZIS heterojunctions with different weight percentage (10 ~ 40%) of MZFO are constructed from spent batteries and added indium ion via a green bioleaching and hydrothermal method. Structural, optical, and photocatalytic properties for the heterojunctions are investigated systematically by XRD, FT-IR, SEM–EDX, TEM, BET, VB-XPS, UV–vis DRS, PL, etc. The results confirm that p–n junction significantly improves the visible light adsorption and the separation efficiency of photogenerated carriers. Specifically, MZFO-25%@ZIS shows the highest photodegradation performance toward Congo red (CR), and its reactive kinetic constant is about 9.6, 7.8, and 7.0 times higher than that of P25 TiO 2 , MZFO, and ZIS, respectively, and MZFO-25%@ZIS still possesses a high reusability and simple magnetic separation after 5 cycles of reuse. The radical trapping experiments and electronic paramagnetic resonance (EPR) tests show that · O 2 − , · OH, and h + are the most important active substance for degrading CR. The pathways for the CR degradation are further proposed based on the intermediate analysis. DFT + U calculations confirm that the high charge density of Zn–O, Fe–O, and Zn–S bonds in the MZFO and ZIS molecules provides the electrons for the sufficient production of free radicals. This work also provides a novel high value-added strategy for the green utilization of spent batteries.
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APPLIED CATALYSIS A-GENERAL
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2022
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IF 5.723
Chencheng Dong,Yan Bao,Mingyang Xing,Masakazu Anpo,Jinlong Zhang
Advanced oxidation processes (AOPs) are reckoned effective for removing persistent and recalcitrant pollutants by reactive oxygen species (ROSs), including hydroxyl radicals (•OH), sulfate radicals (SO 4 • - ), and superoxide radicals (•O 2 - ), as well as singlet oxygen ( 1 O 2 ). In this work, the Mo 2 C quantum dots enriched N-doped graphitic carbon layers (Mo 2 C QDs/NGCLs) were constructed via a facile two-step methodology. Interestingly, the Mo 2 C QDs/NGCLs acted as a highly efficient cocatalyst and/or catalyst simultaneously in AOPs, in particular visible-light-driven (VLD) Fenton and VLD PMS activation. In the hydroxyl radical-based AOPs (•OH-AOPs), it exhibited a remarkable removal efficiency for a range of aromatic organic pollutants , including rhodamine B (RhB) (99.9 %), phenol (90 %), benzophenone-3 (BZP) (83 %), methyl orange (MO) (58 %), methyl blue (MB) (89 %), ibuprofen (IBU) (100 %), and carbamazepine (CBZ) (50 %). Sulfate radicals-based AOPs (SR-AOPs) effectively degrade RhB (72 %), MO (83 %), IBU (70 %), and BZP (100 %). Thus, the present findings confirmed the potential of transition metal carbides for AOP applications and established a solid theoretical and technical basis for further research.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Baowei Cao,Dachuan He,Fei Rao,Qadeer Ul Hassan,Xiaolong Cai,Lingna Liu,Fan Xue,Gangqiang Zhu
BiOI-loaded flower-like CeO 2 (BiOI/CeO 2 ) p-n heterojunction was synthesized via a simple two-step chemical route. The phase structure and chemical states of the heterojunction were analyzed by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS), respectively. The transmission electron microscopic (TEM) and the scanning electron microscope (SEM) reveal the close contact between BiOI and CeO 2 . The formation of the p-n heterojunction is verified by the Mott-Schottky curves. The p-type BiOI with a narrow band-gap when loaded on CeO 2 can not only improve the separation of photogenerated electron-hole pairs but also facilitate the absorption of visible light. The photo-oxidative removal efficiency of 9%BiOI/CeO 2 among other heterojunctions for NO reaches 45.49% and remains highly stable with an efficiency of 40.40% after the five cycles. Trapping experiments and ESR measurements were conducted to explore the contribution of charge carriers and the reactive oxygen species during the photocatalytic NO removal. This work highlights that constructing such p-n heterojunction by loading BiOI on CeO 2 microstructures can significantly enhance photocatalytic NO removal.
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ACS Applied Materials & Interfaces
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2022
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IF 10.383
Xiaona Yang,Kun Zhang
Three-dimensional thermoelectric (TE) textiles (TETs) fabricated with TE filaments (TEFs) possess merits over other types such as thickness–direction thermal energy harvesting and excellent conformability with dynamic body curves, revealing the prospect of generating electricity for on-body application. Nonetheless, there is still a lack of a costless but scalable method to automatically and seamlessly produce in-series interconnected p–n segmented TEFs with high TE properties via conventional fiber spinning processes. Here, we developed an alternate wet-spinning strategy to continuously manufacture single-walled carbon nanotube-based p–n segmented TEFs at large scale. The TEF with high electrical conductivity (400–800 S cm–1) displays a low contact resistivity of 189.8 μΩ cm2 between the segments and interelectrode, showing 2 orders of magnitude smaller than that reported in the literature. More importantly, the power factors of p-type and n-type segments are 26.25 and 17.14 μW m–1 K–2, respectively, which are 3 and 4 orders of magnitude higher than those of advanced studies. We finally embroidered it into spacer fabric to fabricate a wearable TET, demonstrating an output power density of 501 nW m–2 at ΔT = 27.7 K. The methodology can inspire the development of fiber-based electronics such as wearable TEs and diodes and so forth.
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TALANTA
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2022
·
IF 6.556
Jingjing Shu,Wenli Xiong,Ran Zhang,Shanyun Ma,Kaiqiang Zhou,Xuwei Wang,Fen Yan,Da Huang,Jianhua Li,Yuanzi Wu,Jian'an He
In view of the biological significance and micro-heterogeneity of protein glycosylation for human health, specific enrichment of N -glycosylated proteins/peptides from complex biological samples is a prerequisite for the discovery of disease biomarkers and clinical diagnosis. In this work, we propose a “grafting-from” N-glycoprotein enriching method based on the in-situ growth of thermoresponsive polymer brushes from the N -glycosylated site of proteins. The initiator was first attached to the pre-oxidized glycan moieties by hydrazide chemistry , from which the thermoresponsive polymers can be grown to form giant protein-polymer conjugates (PPC). The thermosensitive PPC can be precipitated and separated by raising the temperature to above its lower critical solubility temperature (LCST). Mass spectrometry verified 210 N -glycopeptides corresponding to 136 N-glycoproteins in the rabbit serum. These results demonstrate the capability of the tandem thermoprecipitation strategy to enrich and separate N-glycoprotein/glycopeptide. Due to its simplicity and efficiency specifically, this method holds the potential for identifying biomarkers from biological samples in N -glycoproteome analysis.
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