Nanomaterials
·
2022
·Vol. 12
·期 12
·2026
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IF 5.719
Weizhuo Zhang,Xin Li,Chencheng Peng,Fei Yang,Linyuan Lian,Runda Guo,Jianbing Zhang,Lei Wang
Colloidal cesium lead halide (CsPbX3, X = Cl, Br, and I) perovskite nanocrystals (NCs) demonstrate supreme optical properties in the spectra region of infrared, red, and green. High-performance blue-emitting counterparts are still eagerly required for next-generation full-color displays. However, it is challenging to obtain efficient blue perovskite NCs, especially in a deep blue region with an emission wavelength of around 460 nm or shorter. Herein, calcium halide and ammonium ions are applied simultaneously to modify the CsPb(Br/Cl)3NCs in situ to reduce surface defects, finally remarkably enhancing the photoluminescence quantum yield (PLQY) from 13% to 93% with an emission peak at 455 nm and the Commission Internationale de l’Eclairage (CIE) coordinates at (0.147, 0.030), which is close to the requirement of the Rec.2020 standard and also meets the requirement of blue emission in DCI-P3. Bright white emission and a wide color gamut are also achieved by combining the commercial red-emitting and green-emitting phosphors. The combination of time-resolved PL spectra and femtosecond transient absorption results discloses the reason for PLQY improvement as suppressing the nonradiative recombination.Keywords:CsPb(Br/Cl)3nanocrystals;surface passivation;blue emission;ammonium ion;calcium
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INORGANIC CHEMISTRY
·
2022
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IF 5.436
Qiang Huang,Changqing Tian,Junan Lai,Fei Qi,Nan Zhang,Jiaxin Liu,Zhiyu Liang,Daofu Wu,Xiaosheng Tang
In response to calling for a sustainable and carbon-neutral economy, the conversion of CO2 to useful chemicals using the solar energy is a potential tactic to relieve the global energy dilemma and environmental issues, which has been a hot topic so far. Recently, the lead halide perovskites as novel photocatalysts have attracted researchers’ interests. However, they generally encounter poor stability and lead toxicity, restricting their large-scale practical applications. Here, the lead-free Cs2TeX6 (X = Cl, Cl0.5Br0.5, Br, Br0.5I0.5, and I) perovskite microcrystals with strong stability were prepared and used to realize the CO2 photocatalytic reduction efficiently. The prepared Cs2TeBr6 microcrystals delivered stronger photocatalytic ability than many previously reported photocatalysts, with the CO and CH4 yields of 308.63 and 60.42 μmolg–1, respectively, under 3 h of illumination. The presented strategy in our work provides new ideas of designing and preparing efficient and practical CO2 reduction photocatalysts based on nonleaded and high-stability halide perovskites.
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Molecular Catalysis
·
2021
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IF 5.062
Tao Yang,Wenzhi Li,Ajibola T. Ogunbiyi
This study was focused on investigating a novel catalytic system for the selective conversion of furfural to maleic acid (MA) in an aqueous system with hydrogen peroxide as an oxidant. A series of experiments that study the impacts of catalyst species, furfural concentration, catalyst dosage, reaction temperature, residue time, hydrogen peroxide concentration, excess water content, and solvent types on the oxidation of furfural to MA was carried out. The results showed that the co-existence of Br- and alkali sites might play a vital role in furfural oxidation, which could improve the MA yield remarkably. Under 90 °C for 3 h, 72.4 % MA yield was obtained with KOH and KBr as co-catalyst in an aqueous phase. Moreover, a possible reaction pathway of furfural oxidation was proposed on the basis of our reaction system.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Zhuyu Sun,Dan Geng,Chaojie Zhang,Jiabin Chen,Xuefei Zhou,Yalei Zhang,Qi Zhou,Michael R. Hoffmann
Due to the extremely high stability of perfluorooctane sulfonate (PFOS), effective defluorination is difficult. Previous studies indicated that PFOS can be decomposed under the catalysis of vitamin B12 (VB12) with strong artificial reductants such as Ti(III)-citrate and nZn 0 . In this study, we explored if naturally occurring reductant like sulfide (S 2− ) could initiate the reaction. In S 2− /VB12 system, branched PFOS (br-PFOS) can undergo effective decomposition and defluorination at the temperature of 70 °C and pH greater than 12. The degradation of br-PFOS fits pseudo-first-order kinetic with a rate constant of 0.0984 ± 0.0034 d -1 in the presence of 30 mM Na 2 S and 300 μM VB12, while linear PFOS (L-PFOS) remained stable during 30 d reaction process. UV–Vis spectral characterization indicates that S 2− reduces VB12(Co III ) to Co II , which is able to initiate the reductive defluorination. Based on the product analysis, HF/2F elimination followed by C–C scission is the dominant degradation pathway of br-PFOS instead of stepwise H/F exchange. The primary products include F − and polyfluorinated sulfonates and carboxylates. The degradation of br-PFOS is strongly dependent on temperature due to a relatively high apparent activation energy of 62.86 kJ/mol. Strong alkaline condition can greatly enhance the decomposition efficiency since S 2− is the primary reactive form. This study provides new insights into the VB12-catalyzed defluorination of PFOS and a feasible approach for future natural or engineered remediations of br-PFOS.
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Journal of Materials Chemistry C
·
2021
·Vol. 9
·期 15
·5182-5189
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IF 7.393
Liang Bao,Wenqiang Liu,Yonghua Chen,Yanbo Zhang,Yang Zhang
The local surface plasmon resonance effect induced by metal nanoparticles on perovskites provides a powerful approach to enhance the photoluminescence of such all-inorganic systems. Here, we show that the decoration of CsPb(Br/Cl)3 nanocrystals (NCs) with Au nanoparticles (NPs) leads to a significant enhancement of the blue emission centered at 465 nm, resulting in a photoluminescence quantum yield (PLQY) of up to 73%. Our simulations based on finite difference time domain (FDTD) analysis indicate that the distance between the Au NPs and CsPb(Br/Cl)3 NCs plays a crucial role in determining the local electric field intensity. Our data suggest that an excessive decoration of CsPb(Br/Cl)3 NCs with Au NPs can also reduce the PLQY, as a result of decreased coupling strength.
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BIOMEDICINE & PHARMACOTHERAPY
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2021
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IF 6.53
Yi-yu Liang,Kun-wei Li,Feng-jv Niu,Ying Li,Hao-cheng Wei,Yun-lei Dai,Yun-yu Wang,Chang-zheng Zhou,Xin-huan Wan
Objective To investigate the antiviral effect of Salvia plebeia R. Br. polysaccharides (SPP) against RSV and underlying mechanisms. Methods SPP was extracted via alcohol-precipitation method and extract was separated into various fractions using ultrafiltration method. The polysaccharide content was determined using UV-Vis. Antiviral effect of SPP and fractions was measured using MTT method and Reed-Muench method. Sixty Balb/c mice were randomly divided into 6 groups, and received either Ribavirin or SPP. Their body weight and food intake were recorded every day throughout the experiment period. The lung index inhibition ratio and pulmonary virus titer were determined followed by the histological analysis of lungs. Furthermore, time-of-addition and effective stage analysis were carried out to determine the mechanism of action. The TLR-3 and TLR-4 levels in the lungs were determined using qRT-PCR. The levels of IFN-γ, IL-2 and TNF-α in serum were determined using ELISA. Results The SPP content is 4.396%. SPP has shown a good anti-RSV effect both in vitro (TI = 123.041) and in vivo models. The antiviral activity of fractions with molecular weight ≥ 10,000 is found to possess more potent antiviral activity than other fractions. SPP inhibits the RSV proliferation and reduces the lung lesions induced by RSV. The mechanism of action involves the inhibition of TLR-3 and TLR-4 in lungs, up-regulation of IFN-γ and IL-2, and down-regulation of TNF-α in serum. It is also shown to improve the body’s immune function. Conclusion SPP has a potential to treat diseases caused by RSV.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Jiafu Li,Jiahui He,Md. Tareq Aziz,Xiaocui Song,Ying Zhang,Zhiguang Niu
As a well known endocrine-disrupting and model chemical, bisphenol A (BPA) may pose a serious threat to human health, since it and its disinfection by-products (DBPs) have been detected in drinking water , urine, human colostrum, adipose tissue , and placenta samples. Although chlorinated BPAs (Cl-BPAs) and iodinated BPAs (I-BPAs) have been well studied, brominated BPAs (Br-BPAs), and mixed halogenated DBPs like bromo-iodo-BPAs (Br-I-BPAs), and bromo-chloro-iodo-BPAs (Cl-Br-I-BPAs) are less well understood. Notably, the role of iodide (I - ) during chlorination is not well understood, since the studies of the I-DBPs mainly focus on their genotoxicity and cytotoxicity. To understand the formation mechanisms of halogenated bisphenol A (HBPs) during chlorination with bromide (Br - ) and/or I - , and the role of I - during chlorination, three set of reactions were performed in the laboratory (“BPA + chlorine + Br - ”, “BPA + chlorine + I - ” and “BPA + chlorine + Br - +I - ” assigned as group A, B and C respectively). Thirty HBPs were identified and 18 of them were never reported before. I - increases the transformation rate of BPA into HBPs as I-BPAs act as intermediate HBPs during chlorination that easily react with HClO/ClO - and HBrO/BrO - to form Cl-BPAs and Br-BPAs. HIO/IO - showed higher reactivity towards BPA and HBPs than that of HBrO/BrO - and HClO/ClO - . The recycling of I - was observed in the reactions of “BPA + chlorine + I - ” and “BPA + chlorine + Br - +I - ”, which may explain why I - can induce BPA to transform into HBPs and suggests that I - may act as a catalyst during the BPA chlorination reactions. The reaction pathways are proposed which present the reactions of BPA and HBPs with HClO/ClO - , HBrO/BrO - , and HIO/IO - , as well as the recycling of I - . This study describes the potential DBP formation and transformation mechanisms of BPA and its 16 alternatives, as well as the role of I - on the transformation of phenol compounds during chlorination.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xueqing Jin,Penglei Xu,Feiyang Zhang,Qi Shen,Chunyan Sun
The activation of carbon-halogen bonds is of great significance to realize the breakdown of halogenated contaminants. Herein, a series of iodine vacancies enriched BiOI 1-x photocatalysts prepared by simple temperature regulation were successfully applied in photocatalytic debromination of decabromodiphenyl ether (BDE209) under irradiation (λ > 360 nm). The obtained BiOI-450℃ composed of Bi 7 O 9 I 3 /Bi 5 O 7 I homojunction with iodine vacancies exhibited the best photocatalytic capacity to debromine BDE209. The removal of the first bromine atom from BDE209 on BiOI-450℃ displayed strong position selectivity that meta-debromination is superior to para -debromination, with essentially no ortho -debromination products formed. The selectivity of meta -debromination on iodine vacancies is as high as 72 %, which is higher than the selectivity on oxygen vacancies and sulfur vacancies. The larger space of iodine vacancy is more conducive to accommodating the bromine atom, therefore stabilizing the meta- bromine atomic adsorption configuration of BDE209 and promoting the C-Br bond activation by O…Br halogen bond with the support of surrounding oxygen atoms. This work will provide a feasible strategy for efficient dehalogenation of halogenated persistent organic pollutants based on halogenated bond activation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Xiaoxiao Wang,Awei Guo,Yunlong Wang,Zhipeng Chen,Yuxuan Guo,Haijiao Xie,Weilong Shan,Junjie Zhang
Electrochemical conversion of CO 2 into chemical feedstock , such as an energy-dense liquid product (formate), is desirable to address the excessive emission of greenhouse gases and store energy. Cu-based catalysts exhibit great advantages in electrochemical CO 2 reduction reaction (eCO 2 RR) due to their low cost and high abundance, but suffer from low selectivity of formate. In this work, a facile one-pot approach is developed to synthesize CuBr nanoparticle (CuBr NP) that can conduct in situ dynamic restructuring during eCO 2 RR to generate Br-doped Cu NP. The in situ-formed Br-doped Cu NP can afford up to 91.6% Faradaic efficiency (FE) for formate production with a partial current density of 15.1 mA·cm −2 at −0.94 V vs. reversible hydrogen electrode (RHE) in an H-type cell. Moreover, Br-doped Cu NP can deliver excellent long-term stability for up to 25 h. The first-principles density functional theory (DFT) calculations show that the doped Br can regulate the electronic structure of Cu active sites to optimize the adsorption of the HCOO* intermediate, greatly hindering the formation of CO and H 2 . This work provides a strategy for electronic modulation of metal active site and suggests new opportunities in high selectivity for electrocatalytic reduction of CO 2 to formate over Cu-based catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xiaomeng Yang,Zhen Zhang,Puhua Shao,Armin Rezayan,Dan Wu,Chunbao Charles Xu,Jianshe Wang,Yongsheng Zhang
Selective hydrogenolysis of 4-O-5 bond in lignin under relatively mild conditions is an important strategy for the production of valuable aromatic products, e.g. phenols, from renewable carbon resources. However, the easy saturation of benzene rings under reductive conditions over metal catalyst reduces the selectivity to aromatics. In this work, we investigated the effect of bromination of supported Ni nanoparticles on the phenol selectivity during the hydrogenolysis of diphenyl ether (DPE), a commonly used lignin model compound. Compared with the unmodified catalysts, Br-Ni/Al 2 O 3 catalyst derived from Ni-Al layered double oxides exhibits enhanced phenol selectivity (37% vs. 15%) under similar DPE conversions (60%). Various characterizations including transmission electron microscopy (TEM), in-situ X-ray photoelectron spectroscopy (XPS), extended X-ray absorption fine structure (EXAFS), and CO-Fourier transform infrared spectroscopy (FTIR) indicate that Br preferentially located at the terrace site of Ni nanoparticles, deactivating the continuous Ni sites for benzene ring hydrogenation. In addition, the electron-withdrawing effect of Br creates positively charged Ni sites at the corners, facilitating the hydrogenolysis of C–O aryl ether bonds. During the hydrogenation of real lignin, the selective poisoning and electronic effects introduced by Br synergistically increased the yield of phenols from 12.20% on the initial Ni/Al 2 O 3 to 30.47% over the Br-Ni/Al 2 O 3 catalyst. This work provides an advanced strategy for the catalytic valorization of lignin by halogen modified metal-based catalysts.
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Journal of Herbal Medicine
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2023
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IF 2.3
Ying Liu,Xia Zhang,Huaiyu Cheng,Yifang Li,Guangxiong Zhou
ABSTRACT Introduction It has a long history to employ Macleaya cordata (Willd.) R. Br. (Papaveraceae) for the treatment of a variety of diseases in China. Chelerythrine, one of the major of M. cordata with detoxifying and anti-inflammatory effect, is reported to combat bacteria and fungus. This work aims to explore the effect of chelerythrine against fluconazole-resistant C. albicans and also illustrate its potential mechanism. Methods The microdilution method, following CLSI-M27-A3 was used to evaluate the effect of chelerythrine against fluconazole-resistant C. albicans. Meanwhile, biofilm viability was assessed by XTT assay and cell morphology was observed by inverted microscope. RT-qPCR and confocal laser scanning microscope were employed to detect the mRNA expression and DCFH-DA staining, respectively. Fluorescence intensity was quantified by flow cytometry. Results The total alkaloids extract of M. cordata significantly inhibited the viability of C. albicans, concentration of which in 64 μg/mL presented to 40% inhibitory effect . In addition, the MIC 80 for chelerythrine was 8 μM, whereas chelerythrine in 4 μM inhibited biofilm formation by 47.7%. Further studies revealed that chelerythrine reduced the hydrophobicity of cellular surface, inhibited hyphal growth, downregulated the expression of genes related to cAMP pathway, increased cellular permeability and promoted the production of reactive oxygen species (ROS). Conclusion Chelerythrine inhibited biofilm formation by decreasing CSH and inhibiting the cAMP pathway. Chelerythrine increased cellular permeability and promoted the production of reactive oxygen species, which leads to the cell death of fluconazole-resistant C. albicans .
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Molecular Catalysis
·
2023
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IF 4.6
Lianyang Zhang,Yue Meng,Bo Xie,Zheming Ni,Shengjie Xia
The activity of single-crystal catalysts with different crystal faces varies greatly, and the construction of catalysts with highly exposed active facets is essential for the improvement of photocatalytic performance. In this paper, Cu 2 O (100) crystal facets were transformed into high degrade-active Cu 2 O (111) crystal facets by doping with halogen atoms Br for the photocatalytic degradation of tetracycline. The effect of the optimal Br/Cu 2 O ratio on the degradation activity was investigated by adjusting the amount of Br. Meanwhile, based on photocatalytic degradation performance tests, photoelectric performance characterization and theoretical calculations, it was found that the doped Br-Cu 2 O introduced impurity energy levels, reduced the band gap, broadened the absorption range of the photocatalyst under visible light, and enhanced the oxidation capacity and the rate of photogenerated electron leap. In addition, the highly active Cu 2 O (111) crystal surface facilitates the adsorption of oxygen to generate superoxide radicals and promote the photocatalytic reaction. The synergistic effect of these two aspects promotes the efficient degradation of tetracycline by Br-Cu 2 O. This work provides a promising idea for the design and construction of highly efficient active surface highly exposed photocatalysts.
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