Journal of Materials Chemistry A
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2024
·Vol. 12
·期 48
·33917-33925
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IF 10.7
Yi Ma,Luming Li,Jialing Tang,Zongkun Hu,Yong Zhang,Huan Ge,Ning Jian,Jun Zhao,Andreu Cabot,Junshan Li
Plastics have become an integral part of modern society due to their excellent mechanical properties, light weight, chemical stability and low cost. However, their continuous production and use worldwide have resulted in a major environmental problem. In this context, the green degradation and upcycling of waste plastics using electrochemical oxidation present a promising solution. To make this solution practical, the development of cost-effective catalysts optimized for this reaction is essential. In this study, we propose a new catalyst for the electrocatalytic reforming of ethylene glycol (EG) derived from polyethylene terephthalate (PET) to formic acid. The catalyst comprises layered Ni–Co9S8 nanosheet arrays (NSAs) grown on nickel foam (NF) via the hydrothermal method. Under EG oxidation reaction (EGOR) conditions, the Ni–Co9S8 NSAs/NF catalyst achieves Faraday efficiencies (FEs) of up to 92%. Additionally, the direct use of commercial PET plastic powder hydrolysate still enables formate FEs to exceed 90%. These outstanding results are rationalized using density functional theory (DFT) calculations providing insights into the role of the different elements in the EGOR. Overall, this study demonstrates both a synthetic strategy for transition metal sulfides and an efficient and sustainable strategy for the upgraded recycling of PET plastics.
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PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
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2024
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IF 4.2
Hong Sun,Xinyu Li,Xinyue Yuan,Zhen Tian,Yifan Li,Yalin Zhang,Jiyuan Liu
As an important class of detoxifying enzymes , glutathione S-transferases (GSTs) are pivotal in decreasing insecticide toxicity to insects. Periplaneta americana GSTd1 (PaGSTd1) has been verified as a key enzyme in detoxifying pyrethroid insecticides, but its detoxification capability against a broader spectrum of insecticides has never been investigated. It is revealed that PaGSTd1 expression showed a rapid and significant increase upon exposure to various insecticides (organophosphates, neonicotinoids , and fipronil). Subsequent in vitro metabolic assays indicated that organophosphates , particularly chlorpyrifos-methyl, can be effectively metabolized by PaGSTd1. Further knockdown of PaGSTd1 via RNA interference significantly heightened the susceptibility of P. americana to chlorpyrifos-methyl, underscoring the enzyme's key role in detoxifying chlorpyrifos-methyl. Additionally, this study confirmed that PaGSTd1 cannot mitigate insecticide toxicity through countering oxidative stress . Collectively, these findings elucidate the involvement of PaGSTd1 in the detoxification processes for organophosphates, offering a comprehensive insight into the metabolic mechanisms mediated by GSTs in P. americana . This research provides a foundational understanding for managing GSTs-mediated metabolic resistance in this species, which is crucial for effective pest control strategies.
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ACS Applied Polymer Materials
·
2024
·
IF 4.4
Benteng Liu,Qiao Li,Zhaopeng Hu,Hongda Meng,Xin Jiang,Min Zuo,Miao Du,Yihu Song,Qiang Zheng
N-Cyclohexyl-2-benzothiazolesulfenamide (CZ) is commonly used in the rubber industry as a vulcanization accelerator, while the mechanism for promoting vulcanization is not clear. Herein, CZ was mixed with sulfur (S) at high temperatures to study the structure of mixtures and their effects on the vulcanization and rheological responses of isoprene rubber (IR). It is shown that polysulfides and residual S existed in the pretreated CZ/S mixtures, and the mixtures could adjust the crosslinking density (vc) of vulcanizates by the modulation of mixing temperature and time. Furthermore, pretreated CZ/S affects the nonlinear rheological and thermo-oxidative aging behaviors of IR vulcanizates. The pretreated CZ/S mixed for 10 min can improve the vc and mechanical properties, weaken the Payne effect and the Mullins effect, and delay the thermo-oxidative aging of IR vulcanizates in comparison with the CZ/S mixture without being pretreated. This work provides a way to modulate the cross-linking network to prepare rubber products with high strengths and low hysteresis energies at lower vulcanization temperatures and ZnO amounts.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Jie Cui,Ruotong Zhu,Meiqi Ding,Guoli Chen,Shuhua Liang,Shaodong Sun
Construction of S-scheme heterojunction with 2D/2D structure can accelerate the carrier separation and migration owing to the induced built-in electric field, short carrier migration distance and large contact area. Herein, we develop a simple one-step solvent thermal method for the synthesis of novel Bi 2 O 3 -BiOI 2D/2D S-scheme heterojunction with intimate interfacial contact. As expected, the as-prepared Bi 2 O 3 -BiOI heterojunction presents higher visible-light driven photodegradation of tetracycline (TC), as well as rhodamine B (RhB), methyl orange (MO), and tetracycline hydrochloride (TC-HCl), than the counterparts. Besides, the potential degradation pathways of TC are elucidated and the toxicities of intermediates are assessed in detail. Significantly, the mechanism insight into S-scheme charge transfer mechanism in Bi 2 O 3 -BiOI 2D/2D heterojunction is uncovered in depth by density functional theory calculations and a series of experimental evidences. This work affords a useful inspiration on constructing high-performance BiOI-based photocatalysts via engineering of heterojunction and morphology for organic hazards removal.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Quanqi Zhang,Zhonghua Jiang,Yimin Zhang,Xinyu Xu,Ye Yang,Yucai Qin,Lijuan Song,Yi Mei,Yun Zu
Carbon deposition, an inevitable product operated at high temperatures, is a headache-inducing obstacle to enhance catalyst stability for methane dry reforming (MDR). Herein, we have ingeniously designed sintering-resistant Ni@S-1 nanosheet zeolites to purposefully induce common linear and non-linear deactivation of catalysts during MDR reaction for deciphering carbon footprint. Multiple evidences unveiled that "transient carbon", composed of multi-phenyl-rings via rapidly rearrangement of CH x * fragments, was a crucial vane for catalyst deactivation. Accordingly, we proposed a dynamic equilibrium theory for the generation and elimination of "transient carbon". Achieving this balance was dependent of the matching degree between Ni 0 nanoparticles and NiO x (OH) y , which both separately originated from the evolutions of 1:1 and 2:1 Ni phyllosilicates controlled by nanosheet thickness. Delightfully, synthetic Ni@S-1–60nm catalyst with an optimal ratio of Ni 0 /NiO x (OH) y contributed higher MDR activity and durability. These findings derived a new MDR reaction pathway and afforded value-filled information for developing high carbon-resistant MDR catalysts.
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RARE METALS
·
2024
·
IF 9.6
Wan Si-Jie,Hou Yan-Ting,Wang Wang,Luo Guo-Qiang,Wang Chuan-Bin,Tu Rong,Cao Shao-Wen
Photocatalytic reduction of CO 2 has attracted considerable interest owing to its potential to resolve the energy and environmental problems. Nevertheless, the lack of proficient photocatalysts has restricted the application of solar-driven photocatalytic CO 2 reduction. Herein, we reported an S-scheme heterojunction by combining g-C 3 N 4 with La 3+ and Rh 3+ co-doped SrTiO 3 through the electrostatic self-assembly method for the efficient photocatalytic CO 2 reduction. In comparison with g-C 3 N 4 , the as-prepared CN/LRSTO-30 wt% S-scheme heterojunction not only possesses a broadened visible-light response due to the defect states in La, Rh co-doped SrTiO 3 induced by co-doped La 3+ and Rh 3+ but also has more adsorption sites for the capture and activation of CO 2 molecules. Additionally, separation and transfer efficiency of the photoinduced charge carriers is much enhanced in the CN/LRSTO-30 wt% S-scheme heterojunction via its robust internal electric field, which is firmly demonstrated by in situ irradiation X-ray photoelectron spectroscopy technology. Consequently, the prepared S-scheme heterojunction achieves impressive photocatalytic CO 2 reduction performance with an average CO and CH 4 evolution rate of 4.1–1.8 μmol·g −1 ·h −1 , respectively, which are ~ 1.9 and ~ 22.5-fold higher than those of pure g-C 3 N 4 . This study provides innovative perspectives on the design of creative S-scheme heterojunctions for applications in photocatalytic CO 2 reduction. Graphical abstract
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npj Clean Water
·
2024
·Vol. 7
·期 1
·1-14
·
IF 10.4
Chen Weizi,Xing Zipeng,Zhang Na,Cheng Tao,Ren Bo,Liu Xinyue,Wang Zibin,Li Zhenzi,Zhou Wei
Hierarchical Bi 2 Fe 4 O 9 /BiOI S-scheme nanoflower heterostructures are prepared by hydrothermal method, which exhibit exceptional photo-piezoelectric catalytic performance. The tight binding between the sheets ensures the efficient electron transport, and provides a large interface area and adequate reaction sites for photo-piezoelectric catalytic reactions. At the same time, because the water flow in the water body produces hydraulic shear force on the material, the material produces piezoelectric effect. Bi 2 Fe 4 O 9 /BiOI exhibit a remarkable degradation efficiency of 99.4% for tetracycline and a hydrogen production rate of 4089.36 µmol h −1 g −1 . The observed behavior can be explained by the combined influence of the formation of S-scheme structure and the process of photo-piezoelectric catalysis, confirmed by in-situ XPS, transient/steady-state fluorescence and piezoelectric response force test. The excellent stability of the material suggests its possible use in the sectors of energy and environment. This work introduces novel concepts for the future advancement of photo-piezoelectric synergistic catalysis.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Xueqing You,Qing Ju,Yichang Ma,Guiqin Yi,Zhangtang Jiang,Nanwen Li,Qiugen Zhang
Phosphoric acid (PA)-doped membranes are regarded as a promising candidate for high temperature proton exchange membranes (HT-PEMs), but the trade-off between mechanical property and conductivity is a major problem limiting their application. Here, two poly( meta -terphenyl alkylene)s ( m -TPNs), namely m -TPN-MeIm and m -TPN-TMA, are synthesized by 1-methylimidazole (MeIm) and trimethylamine (TMA) reacting with precursor polymer, respectively. The influence of different cationic groups on the properties of m -TPNs HT-PEMs is investigated in detail. m -TPNs diminish plastication of PA molecules on the mechanical property by separating the adsorption sites for PA molecules from the polymer backbone through long alkyl side chains. As a result, both m -TPN-MeIm and m -TPN-TMA membranes exhibit good mechanical property. Besides, m -TPN-TMA/PA surpasses m -TPN-MeIm/PA in most of aspects owing to the higher ion exchange capacity (IEC) and more distinct microphase separation structure. Noticeably, the proton conductivity of m -TPN-TMA/PA is as high as 0.191 S cm −1 and exhibits excellent stability over a testing time of 100 h at 160 °C thanks to the remarkable acid uptake and microphase separation structure. The m -TPN-TMA/PA-based single cell produces an impressive peak power density of 552 mW cm −2 at 200 °C. Therefore, this work offers a viable alternative for structure design to mitigate the trade-off effect of PA-doped HT-PEMs.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Mei Cai,Chao He,Hulei Yu,Anze Shui
The construction of heterojunction for photocatalysis has garnered much research interest. Herein, we report the successful fabrication of a ternary dual S-scheme ZnO/ZnS/In 2 S 3 heterojunction with a higher photocatalytic capacity via a hydrothermal method . Specifically, the optimized ternary heterojunction ZSI0.35 sample achieves the 100 % photodegradation efficiency of RhB (10 mg/L, 50 mL) within 10 min, approximately 17 and 8 times higher than pure ZnO and ZnO/ZnS binary heterojunction, respectively. Further characterization results confirm the dual S-scheme heterojunction structure in the fabricated ZnO/ZnS/In 2 S 3 ternary heterojunction, and the improvement of photocatalytic properties can be attributed to the enhanced Brunauer Emmett-Teller (BET) surface area, the improved redox capacity of the photocatalyst, and the quick charge transfer. Additionally, the possible photocatalytic mechanism is discussed according to the measurements. This work provides an efficient strategy of promising heterojunction photocatalysts for photocatalytic environmental remediation.
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MICROCHEMICAL JOURNAL
·
2024
·
IF 4.9
Yansheng Liu,Haonan Hu,Xiaobo Jia,Jin Zhou,Hongli Li,Xiaohong Wang,Shaohui Zhang,Haixin Chang,Fuchong Li,Guofu Wang
This study reported a sandwich SERS structure in detecting SARS-CoV-2 spike protein (SARS-CoV-2 S protein) with high performance. The periodic Ag nanoarrays (AgNAs) functionalized with angiotensin-converting enzyme 2 (ACE2) were utilized as the bottom structure to specifically bound to the SARS-CoV-2 S protein. A complex of SARS-CoV-2 S protein antibody and 4-mercaptobenzoic acid (4-Mba) modified Au nanoparticles (AuNPs@4-Mba@Antibody) were used as nanotags and top SERS enhancing structures. By utilized the “hot spots” in parallel and perpendicular directions, the SERS signals of the 4-Mba as reporters were largely enhanced. By modulated the diameters and the heights of the AgNAs, the SERS performance of the sandwich structures was optimized by using R6G as a stand analyst with limits of detection (LOD) of 1 × 10 −9 M. By applied the optimized sandwich structures in detecting SARS-CoV-2 S protein in phosphate buffered saline (PBS) and pharyngeal swabs solution (PSS), the proposed sandwich structure illustrates a high performance, and the LODs were 0.1 fg mL −1 and 1 fg mL −1 , respectively. This study presented an efficient way to construct a sandwich SERS structure in directly detecting SARS-CoV-2 S protein and this method illustrates a good potential in viral detection.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Wei Zhang,Guokang Han,Chunyu Du
The bimetallic center catalyst (DMC) injects new vitality into the accelerated oxygen reduction reaction (ORR) due to its unique structure. The regulation of the coordination environment composition and spatial structure of metal active centers also provides opportunities for optimizing the performance. Herein, we have successfully constructed stereoisomeric Fe2CN-bridge-S (abbreviated as Fe2CN-b-S) catalysts based on the biomimetic Fe–S cluster structure of ferredoxin. Adjacent Fe dual atoms skillfully weaken the O–O bond, crafting a peroxide bridge-like adsorption configuration. The incorporation of S atoms meticulously constructs the stereo configuration of active Fe sites, thereby inducing greater structural deformation tension and a downward shift in the Fe d-band center. These factors collectively facilitate the release of the OH* intermediate. Meanwhile, the reasonable spatial configuration of S can promote the optimal rigid structure of Fe diatomic active centers, improving the stability of the ORR reaction process. Thus, the Fe2CN-b-S catalyst, which has a half-wave potential of 0.865 V, demonstrates superior ORR activity in comparison to Fe2CN. This study offers a perspective on the joint regulation of elemental composition and geometric arrangement for enhanced catalytic activity in oxygen reduction.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Xiaoyu Lou,Duanlian Tang,Xuanjie Chen,Lanbin Mo,Yong Li,Changshen Ye,Jie Chen,Ting Qiu
The heavy-metal contamination of aquatic environments presents imminent threat. Herein, we report a class of dual-heteroatomic conjugated microporous poly(aniline)s showing high-affinity separation performance toward heavy metals. The prepared keto-CMPA shows monolayer adsorption capacity for Hg (II) as high as 980 mg g −1 according to the Langmuir model, and ultra-rapid kinetic with h reaching 30.41 mg g −1 that could be described by the pseudo-second-order model. It maintains excellent stability across six reuses under harsh conditions, and furthermore demonstrates ultradeep separation efficiency that could adsorb almost all of heavy metals to ppb level with low usage. For further industrialization, a competent adsorption device was developed to remove heavy metals down to 1 ppb with a remarkable breakthrough over 20,000 BV. Characterizations and DFT calculation showed that the triangular synergistic region formed by the N-O-sites in the singular CMPA structure provided a feasible binding energy to enable the above impressive performance.
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