Journal of Physical Chemistry C
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2023
·
IF 3.7
Yumiao Dong,Qinhui Xie,Shuo Wu,Junbo Li,Lei Sun,Wei Ji
p-Mercaptobenzoic acid (4-MBA) is a typical molecular probe for a surface-enhanced Raman scattering (SERS) study of the enhancement performance of semiconductor nanoparticles. Understanding the molecular adsorption mechanism of 4-MBA on a semiconductor surface is crucial to reveal the enhancement mechanism of semiconductor SERS. Herein, two types of submicrometer-sized TiO2 particles with amorphous (denoted as a-TiO2) and anatase structures (denoted as c-TiO2) were fabricated, and their potential as SERS-active substrates with high electric-field enhancement was explored based on the near-field scattering theory and finite-element method simulation. The electric field-enhanced semiconductor SERS provide a better vision for us to study the adsorption modes of molecules on the TiO2 surface. On this basis, adsorption behaviors of 4-MBA on a-TiO2 and c-TiO2 particles were systematically studied by the semiconductor SERS and density functional theory. The results demonstrated that the adsorption mechanism of 4-MBA with TiO2 surfaces is highly dependent on the exposure of acid sites of TiO2 surfaces. 4-MBA adsorbs preferentially on Brønsted acid sites of a-TiO2 through a carboxyl group, in contrast on Lewis acid sites of c-TiO2 through a sulfhydryl group. Furthermore, 4-MBA molecules may form multilayer adsorption on TiO2 surfaces through the hydrogen bond and/or π–π stacking interaction. Research results not only provide a new insight to re-evaluate the chemical enhancement mechanism for TiO2–4-MBA systems but also provide a theoretical guidance for the modification of TiO2 surface with organic molecules containing carboxyl and sulfhydryl groups.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Ya-Nan Zhao,Kai-Sheng Yao,Ao-Zhou Wang,Wei-Wei Lu
Developing a facile green strategy to one-step prepare anisotropic bimetallic nanomaterials with hierarchical structures is preferred choice but remains technically challenge. Here, a simple ionic liquid-directed route is developed for the fabrication of Pd 3 Cu 1 alloy nano-urchins (NUs) at room temperature in aqueous solution. To achieve the synthetic protocol, water-soluble Na 2 PdCl 4 and CuCl 2 are used as the initial raw materials, ascorbic acid as the reducing agent, and a common ionic liquid 1-butyl-3-methylimidazolium chloride ([C 4 mim]Cl) is applied to guide the growth and formation of Pd 3 Cu 1 NUs, vividly demonstrating the green and cost-saving features. The various factors affecting the shapes and sizes of products are researched. The results show that [C 4 mim]Cl is vital to the formation of thorny Pd 3 Cu 1 NUs. The Pd 3 Cu 1 NUs possess uniform morphology, lots of sharp thorns, high specific surface area and 3D freestanding structures, and exhibit outstanding catalytic activity, selectivity and durability for p -nitrobenzaldehyde hydrogenation having 100% conversion and 94.6% selectivity to p -aminobenzaldehyde. It is believed that the 3D Pd 3 Cu 1 NUs would also have hopeful prospects in electrocatalysis , sensor and beyond.
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Polymers
·
2022
·Vol. 14
·期 24
·5419
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IF 4.967
Puyu Jin,Aimin Pang,Rongjie Yang,Xiaoyan Guo,Jiyu He,Jinxian Zhai
To improve the mechanical properties of polyurethane cross-linked poly (ethylene oxide-co-tetrahydrofuran) (P(E-co-T)) elastomers at room temperature, using poly (ethylene oxide-co-tetrahydrofuran) and high-molecular-weight polyethylene glycol (PEG) as raw materials and polyisocyanate N100 as curing agent, a series of polyurethane cross-linked blended polyether elastomers were prepared by changing the elastomer-curing parameter R value (n(-NCO)/n(-OH)) and P(E-co-T)/PEG ratio. Equilibrium swelling measurements showed that the chemical cross-linkage of the elastomers tended to decrease with the decreasing R value, the average molecular weight (Mc) of the network chain increased, and the density of the network chain (N0) decreased. Wide-angle X-ray diffraction (WAXD) and differential scanning calorimetry (DSC) tests showed that PEG chain segments within the elastomers crystallized at room temperature, while the crystallinity increased with decreasing R value and increasing PEG content. The mechanical property tests showed that the elongation at break tended to decrease with increasing R value; the tensile strength first increased and then decreased. At R value 0.9, the elastomer presented good comprehensive mechanical properties. In addition, the mechanical properties of polyurethane cross-linked P(E-co-T)/PEG blended polyether elastomer showed an increasing trend with the increase in PEG content when the curing parameter of 0.9 remained unchanged.Keywords:polyurethane cross-linked elastomer;polyether blend;crystallinity;mechanical properties
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NEUROCHEMICAL RESEARCH
·
2022
·Vol. 48
·期 5
·1424-1437
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IF 4.414
Zhao Yanling,Yan Han,Liang Xue,Zhang Zhenyu,Wang Xuan,Shi Nianwei,Bian Weihong,Di Qing,Huang He
Astrocyte activation is key in neurodegenerative diseases. Hydrogen sulfide (H 2 S) exhibits neuroprotective effects on astrocytes, although the underlying molecular mechanism remains unclear. Here, we explored the effects of H 2 S on lipopolysaccharide (LPS)-induced astrocyte activation and astrocyte-mediated neuroinflammation. After inducing primary astrocytes via LPS exposure, H 2 S levels were altered. The generation and secretion of inflammatory mediators by astrocytes and their interrelation with P-glycoprotein (P-gp), an important transporter belonging to the ABC transporter family, were assessed. Activated astrocytes showed upregulated glial fibrillary acidic protein ( GFAP ) mRNA expression, and significantly increased proinflammatory factor mRNA/protein expression and release. The secretory capacity of astrocytes was reduced, with significantly decreased proinflammatory factor levels in culture supernatant after P-gp inhibitor verapamil pretreatment. The increase in the intracellular H 2 S level inhibited LPS-induced GFAP expression and P65 nuclear entry in astrocytes. mRNA expression and release of proinflammatory factors were reduced significantly, with no significant changes in cytoplasmic protein expression. S-sulfhydration levels increased significantly with the increased concentration of sodium hydrosulfide or S-adenosyl- l -methionine addition, with only moderate changes in astrocyte P-gp expression. H 2 S regulates NF-κB activation, leads to S-sulfhydration of P-gp, and inhibits the biosynthesis and secretion of proinflammatory factors by astrocytes. The regulatory effects of H 2 S on astrocytes may have clinical value for exploring new therapeutic strategies against neurodegenerative diseases.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Yanyan Chen,Manlin Zhang,Tiantian Chen,Ganbing Zhang,Hui Xu,Hongwei Sun,Lizhi Zhang
The application of powdered nanoscale zero-valent iron (nZVI) in conventional reactors for water treatment is limited by insufficient mass-transfer and difficult post-separation of catalysts. Herein, a novel microreactor was constructed by anchoring nZVI on the reduced graphene oxide/polypyrrole nanocomposite (rGO/PPy) substrate within the microchannel of a stainless-steel tube through two-step electrodeposition , which catalyzed the Fenton-like reaction to remove > 99% p-nitrophenol (PNP) within 50 s, outperforming traditional batch reactors. The rGO/PPy composite substrate consolidated the adhesion on steel surface, stabilized the nZVI by forming electron-transfer complex, facilitated the decomposition of H 2 O 2 to free •OH, and promoted the redox cycle of Fe(III)/Fe(II) via the electron donating capacity of rGO/PPy. Besides, the significant convection and highly-effective mass transfer within the microreactor also contributed to the ultrafast PNP removal. With acceptable durability, easy re-generation, and scalability, the rGO/PPy/nZVI microreactor is promising for the ultrafast removal of pollutants from water.
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Membranes
·
2022
·Vol. 13
·期 1
·14
·
IF 4.562
Jingjun Peng,Bhaskar Jyoti Deka,Shaodi Wu,Zhongyuan Luo,Jehad A. Kharraz,Wei Jia
Water pollution caused by oil spills or sewage discharges has become a serious ecological environmental issue. Despite the membrane separation technique having a promising application in wastewater purification, the membrane fabrication method and separation robustness have remained unsatisfactory until now. Herein, we developed a novel strategy, spacer-assisted sequential phase conversion, to create a patterned polyvinylidene fluoride@polypropylene (P-PVDF@PP) substrate membrane with a multiscale roughened surface. Based on that surface structure, the underwater oil resistance behavior of the P-PVDF@PP membrane was improved. Moreover, owing to the abundant active sites on the P-PVDF@PP surface, the polydopamine/P-PVDF@PP (PDA/P-PVDF@PP) Janus membrane could be readily fabricated via wet chemical modification, which exhibited excellent switchable oil–water separation performance. Regarding surfactant-stabilized oil-water emulsion, the as-prepared PDA/P-PVDF@PP Janus membrane also had robust separation efficiency (as high as 99% in the n-hexane/water, chloroform/water, and toluene/water emulsion separation cases) and desirable reusability. Finally, the underlying mechanism of emulsion separation in the PDA/P-PVDF@PP Janus membrane was specified. The as-designed PDA/P-PVDF@PP Janus membrane with high-efficiency oil–water separation shows potential application in oily wastewater treatment, and the developed fabrication method has implications for the fabrication of advanced separation membranes.Keywords:emulsion separation;Janus membrane;patterned interface;switchable wettability
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Jiajie Xing,Qian Peng,Wanling Zhong,Yingjie Zhang,Xin Wang,Kun Liu
A novel CuO-Chrysotile thin membrane catalyst was prepared by simple impregnation-calcination route, which provided new insights of catalytic membranes by natural mineral fiber for the degradation of organic contaminants in wastewater treatment . Through intermittent and continuous catalytic degradation experiments, peroxymonosulfate (PMS) was efficiently activated by the membrane to degrade p-nitrophenol (PNP), and the effects of experimental parameters (including initial solution pH value, PMS dosage, catalyst dosage, reaction temperature, membrane mass and flow rate) on PNP degradation were systematically studied. The results showed that the catalytic membrane had great catalytic performance and long-term stability, it could completely degrade 10 mg/L of PNP within 60 min and its degradation ratio could remain above 90 % after 5 cycles. Meanwhile, it was worth noting that 0.15 g of CuO-Chrysotile catalytic membrane used as fixed bed could continuously degrade 12.5 L of PNP solution with gratifying performance, which proved that the catalytic membrane had convenient use method and great application effect. The mechanism study found that 1 O 2 produced in this process played a key role in the degradation of PNP. From the aspects of manufacturing cost, catalytic performance and service life, the novel CuO-Chrysotile catalytic membrane has excellent industrial application potential.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Huayi Cai,Jingjing Wang,Zhao Du,Zhiyuan Zhao,Yaxin Gu,Zhonglu Guo,Yang Huang,Chengchun Tang,Guifeng Chen,Yi Fang
Photocatalysis has attracted much attention in the field of environmental remediation. However, the photocatalytic performance largely depends on efficient charge migration and solar light utilization. Herein, the ternary MoSe 2 /ZnO/p-BN (MZB) photocatalyst was successfully designed and synthesized. The degradation rate of the optimal sample 30 wt% MZB for ofloxacin (OFL) under visible light irradiation can reach 99.2%, and the photocatalytic reaction rate is 5.33 times and 2.10 times higher than that of pure ZnO and ZnO/p-BN. In the MoSe 2 /ZnO/p-BN system, p-BN can achieve the enrichment of pollutant to accelerate the catalytic rate, while the hybridization of MoSe 2 expands the spectral response of the catalysts. In addition, the formation of stepped electron transport routes reduces the electron-hole pair recombination rate. The active species quenching experiments reveal that e - , •O 2 − , h + and •OH play a major role in the removal of antibiotic contaminants. The analysis of OFL degradation intermediates reveals the possible degradation pathways and proposes a reasonable photocatalyst mechanism. Therefore, this work provides new ideas for designing high-performance visible light responsive photocatalysts for pollution treatment.
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MOLECULES
·
2023
·Vol. 28
·期 3
·1122
·
IF 4.6
Juan He,Xiaomin Xu,Hainan Sun,Tengfei Miao,Meisheng Li,Shouyong Zhou,Wei Zhou
The harmful effects on the human body from p-phenylenediamine (PPD) in hair dyes can cause allergies and even cancer. Therefore, it is particularly important to accurately control and detect the content of PPD in our daily products and environment. Here, a small amount of non-metallic elemental P doped in perovskite oxide of SrCoO3−δ(SC) forms a good catalytic material, SrCo0.95P0.05O3−δ(SCP), for PPD detection. The improved performance compared with that of the parent SC can be attributed to three contributing factors, including a larger amount of highly oxidative oxygen species O22−/O−, better electrical conductivity, and more active sites on the P5+-oxygen bonds of SCP. Moreover, the lattice oxygen mechanism (LOM) with highly active species of lattice O vacancies and adsorbed –OO for electrocatalytic oxidation of PPD by the SCP/GCE (glass carbon electrode) sensor is proposed in our work. More importantly, the SCP/GCE sensor exhibits good stability, a low limit of detection, and high reliability (error < 5.78%) towards PPD determination in real samples of hair dyes, suggesting the substantial research potential for practical applications.Keywords:lattice oxygen;phosphorus-doped SrCo0.95P0.05O3−δ;p-phenylenediamine (PPD);electrochemical sensors;hair dyes
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INTERNATIONAL JOURNAL OF ENVIRONMENTAL ANALYTICAL CHEMISTRY
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2023
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IF 2.6
Lu-Qing Xie,Guo-Ling Zhao,Xin-Yu Jiang,Jin-Gang Yu
Novel rape seedling peel-derived biochars (BCs) prepared by vacuum pyrolysis were used as cost-saving and sustainable biosorbents for wastewater remediation. The adsorption properties of BCs for p-nitrophenol (PNP) were investigated. The results showed that BC400 prepared at 400°C possessed the highest adsorption capacity of 55.78 mg g−1 towards PNP. Scanning electron microscopy, Energy dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, Zeta potential analysis and Brunauer-Emmett-Teller specific surface area analyses were performed to characterise the physicochemical properties of BC samples. The microporous structure and abundant surface heteroatomic functional groups of BC400 were confirmed. The effects of adsorption conditions (contact time, temperature, initial PNP solution pH, initial PNP concentration) on the adsorption of PNP by BC400 were investigated. Adsorption behaviour was more consistent with the linear Freundlich model and linear pseudo-second-order kinetic model. Thermodynamic study showed that the adsorption of PNP on BC400 was a spontaneous endothermic process, and the disorder degree increased after adsorption. In addition, the adsorption capacities of BC400 for different phenols including hydroquinone, 3-nitrophenol, 1-naphthol (AN) and tert-butyl hydroquinone were compared, and the mechanism was also proposed. BC400 with aromatic and heteroatom-containing functional groups could interact effectively with PNP through various intermolecular interactions including π-π stacking, hydrogen bonding and electrostatic attraction. Reusability assessment indicated BC400 remained high removal rate even after 10 consecutive adsorption-desorption cycles.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Hui Liu,Hongyan Li,Bin Lu,Songnan Li,Jingxiang Zhao,Qinghai Cai
A composite catalyst was prepared by impregnation of ZSM-5 in mixture solution of Co(NO 3 ) 2 , ZrOCl 2 and phosphotungstic acid (PW) and characterized by XRD , FT-IR, UV–vis, XPS , SEM and TEM techniques to confirm its structure and composition . The pre-prepared composite is composed of Co 2 (PO 4 )Cl, ZrO 2 , P 2 O 5 and WO 3 crystalline nanoparticles uniformly dispersed on ZSM-5 zeolite . The prepared composite demonstrates effective catalytic function for solvent-free oxidation of toluene into benzaldehyde with H 2 O 2 oxidant, achieving 16.6% conversion and 90% selectivity . The effect of various components composed of the catalyst and reaction conditions on the catalytic function were explored. Moreover, the recovery and reusability of the catalyst were estimated, presenting good reusability.
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GREEN CHEMISTRY
·
2023
·Vol. 26
·期 2
·968-978
·
IF 9.8
Xinwei Wen,Yue Zhao,Puyang Fan,Jiajie Wu,Kai Xiong,Chang Liu,Qing Qu,Lei Li
The production of ammonia under ambient conditions has been a long-standing challenge for the chemical industry. The electroreduction of nitrate presents a promising solution for nitrate wastewater treatment and decentralized ammonia production. However, traditional Ag-based catalysts suffer from nitrate-to-nitrite conversion, leading to toxicity concerns and hampering ammonia preparation. In this study, we synthesized an innovative Ag–Cu–P catalyst that effectively tunes the d-band centre and electronic structure. The catalyst exhibited a remarkable NH4+ yield rate of 566.30 μmol cm−2 h−1 at −0.3 V (vs. RHE), reducing nitrite content to below the drinking water standard. Characterization results revealed a distinctive fern leaf-like morphology, providing an expanded active surface area. The challenge of facile nitrate conversion to nitrite on Ag-based catalysts has been addressed through the implementation of electronic structure modulation in this work. Theoretical calculations confirmed the substantial reduction in the energy barrier by modulating the d-band centre and electronic structure, facilitating the conversion of nitrite to ammonia. The regulation and analysis of d-band centres yielded valuable insights for catalyst material design. Meanwhile, direct evidence for potential intermediates has also been presented through in situ spectroscopy. These findings hold significant potential for practical applications, such as enhanced wastewater treatment and decentralized ammonia production, and provide support in the pressing need for sustainable ammonia synthesis under ambient conditions.
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