MICROCHIMICA ACTA
·
2021
·Vol. 189
·期 1
·1-7
·
IF 5.833
Xia Chunqiu,Huang Wenying,Kang Xiutang,Chen Pingyun,You Longjie,Guo Liangqia
Mo 5 N 6 nanosheets were synthesized by a nickel-induced growth method and were found to possess peroxidase-like activity in acidic condition and catalase-like activity in weak basic condition. In acidic condition, Mo 5 N 6 nanosheets can catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by H 2 O 2 to form a blue color product (TMB OX ). At the co-existence of 4-aminophenol (4-AP), 4-AP can react with H 2 O 2 and TMB OX , resulting in the decrease of TMB OX and the fading of blue color. Therefore, a facile, sensitive colorimetric method for the quantitative detection of 4-AP was developed. The linear range for 4-AP was 1.0 to 80.0 μmol⋅L ‒1 ( R 2 = 0.999), and the detection limit was 0.56 μmol⋅L ‒1 based on 3 σ / k . Resorcinol, aniline, humic acid, and common ions and anions in surface water did not interfere the determination of 4-AP. This colorimetric method was applied to measure the 4-AP in real water sample from Wulong River in Fujian Province of China. The relative standard deviation for the determination of 4-AP was ranged from 0.03 to 1.88%, and the recoveries from spiked samples were ranged between 99.2 and 107.6%. The determination results were consistent with those obtained by HPLC. Graphical abstract
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高影响因子
Advanced Science
·
2021
·Vol. 9
·期 1
·2101527
·
IF 16.806
Min Qian,Ziqiang Cheng,Guanghong Luo,Massimiliano Galluzzi,Yuehong Shen,Zhibin Li,Hongyu Yang,Xue-Feng Yu
Chemodynamic therapy (CDT) is an emerging treatment that usually employs chemical agents to decompose hydrogen peroxide (H 2 O 2 ) into hydroxyl radical (•OH) via Fenton or Fenton-like reactions, inducing cell apoptosis or necrosis by damaging biomacromolecules such as, lipids, proteins, and DNA. Generally, CDT shows high tumor-specificity and minimal-invasiveness in patients, thus it has attracted extensive research interests. However, the catalytic reaction efficiency of CDT is largely limited by the relatively high pH at the tumor sites. Herein, a 808 nm laser-potentiated peroxidase catalytic/mild-photothermal therapy of molybdenum diphosphide nanorods (MoP 2 NRs) is developed to improve CDT performance, and simultaneously achieve effective tumor eradication and anti-infection. In this system, MoP 2 NRs exhibit a favorable cytocompatibility due to their inherent excellent elemental biocompatibility. Upon irradiation with an 808 nm laser, MoP 2 NRs act as photosensitizers to efficiently capture the photo-excited band electrons and valance band holes, exhibiting enhanced peroxidase-like catalytic activity to sustainedly decompose tumor endogenous H 2 O 2 to •OH, which subsequently destroy the cellular biomacromolecules both in tumor cells and bacteria. As demonstrated both in vitro and in vivo, this system exhibits a superior therapeutic efficiency with inappreciable toxicity. Hence, the work may provide a promising therapeutic technique for further clinical applications.
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Yao Li,Le Xin Song,Wei Ping Wang,Yue Teng,Juan Xia,Nan Ning Liu
In this work, we prepared a series of Fe-MOF polyhedra [metal organic framework (MOF)-1 ∼ −13] by introducing β-cyclodextrin (CD) as a morphology modifier using an interaction between ferric chloride and terephthalic acid in dimethylformamide. A novel structural evolution from a hexagonal bipyramid to a bipyramidal hexagonal prism was clearly observed. This evolution was gradual and could be well reflected by the height ratio of the prism and pyramid in these polyhedral structures. It is the relative concentration of β-CD that drives this structural evolution. Although the reaction temperature and time can also affect the height ratio to some extent, their influence can only be realized in the presence of β-CD. In the absence of β-CD, only hexagonal bipyramid structures were obtained. It is worth noting that Fe-MOF-1 with a bipyramidal hexagonal prism structure (prism height, ∼130 nm) showed typical paramagnetic characteristics, and its saturation magnetization was determined to be 23.1 emu·g–1. Furthermore, we found that Fe-MOF-1 exhibited good photocatalytic performance for different types of dyes (crystal violet with positives and methyl orange with negative charges). At the same time, a possible photocatalytic mechanism was proposed to explain the difference of degradation efficiency between the two dyes. Also, we use the combination of specific surface area and zeta potential to explain the differences in the catalytic properties of a series of Fe-MOF materials. In addition, MOF-1 shows the same electrocatalytic oxygen evolution reaction performance as some bimetallic MOFs such as Fe-Co-MOF. For example, the overpotential of MOF-1 is 398 mV at 10 mA·cm–2 current density, while that of Fe-Co-MOF is 410 mV. We believe that the current work can contribute to the adjustment, modification, and application of MOF nanostructures.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Zhihui Li,Aiping Wu,Ying Xie,Ying Gu,Haijing Yan,Dongxu Wang,Siyu Wang,Chengxu Jin,Lei Wang,Chungui Tian
The design of the electrocatalysts with the plentiful heterojuctional interface and large-accessible surface is desired to boost the HER performance, but it remains a challenge. Herein, we showed the design of 2D Ni/Ni 0.2 Mo 0.8 N porous heterojunction nanobelts as effective catalyst for the HER. The intimate combination of Ni and Ni 0.2 Mo 0.8 N can make the formation of the heterojuctional interface with plentiful active sites. The 2D porous structure can provide large accessible surface with less resistance for the transmission of the electrolytes, thus promoting the mass/charge transfer. The ratio of Ni and Ni 0.2 Mo 0.8 N can be easily tuned by regulating the precursor composition, which is important to give catalysts with optimized interface and suitable pores. Density functional theory calculations reveal that the interaction between Ni and Ni 0.2 Mo 0.8 N at the heterointerface can largely improve the intermediate H* adsorption kinetics (ΔG H* = -0.07 eV). Due to the above advantages, the optimized catalysts exhibited excellent HER activity with a low overpotential of 48 mV in 1 M KOH at 10 mA cm −2 (without iR correction), which is superior to the most reported non-noble metal-based catalysts, and the long-term durability with no obvious degradation after continual operation of 48 h Notably, an electrolyzer assembled by the optimized Ni/Ni 0.2 Mo 0.8 N cathode with NiFe-LDH anode only requires a low operating voltage of 1.47 V to deliver 10 mA cm −2 in 1 M KOH, surpassing the corresponding Pt/NF||RuO 2 /NF electrolyzer (1.61 V) and most of reported electrolyzers.
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CLAY MINERALS
·
2021
·Vol. 56
·期 3
·169-177
·
IF 1.478
Xuefen Zhang,Mingxue Xiang,Zhongbang Zhu,Youqin Zou,Ping Zhang
Hierarchical layered double hydroxide (HLDH) was synthesized by using sodium dodecyl sulfate (SDS) as a soft-template agent for the removal of two charged organic dyes (i.e. methylene blue (MB; cationic dye) and methyl orange (MO; anionic dye)). The experimental results based on response surface methodology (RSM) demonstrated distinct removal behaviours of HLDH towards these two dyes: (1) the maximum capacity was 416.7 mg g–1 for MO and 58.7 mg g–1 for MB at 25°C; (2) the increase in temperature could enhance MO removal significantly, whereas it had a negligible effect on the MB treatment process; and (3) rapid removal of MB (5 min) compared to MO (480 min) was observed. In addition, the removal process for both dyes was pH-independent. Multiple characterization techniques further revealed the removal mechanisms, demonstrating that SDS played a significant role in the removal of both dyes; that is, MO replaced SDS to be intercalated into the HLDH interlayer via anion exchange. MB could influence the –SO3 group of SDS, resulting in it modifying the electrodensity of SDS. It could then be further combined with an SDS anion (DS–) via hydrophobic and electrostatic interactions to form DS-MB monolayers. This work not only provides an efficient capture agent for charged dyes, but also offers a deep insight into the underlying removal mechanism.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Xuesong Zhao,Yingying You,Yiyang Ma,Chenchen Meng,Zhenghua Zhang
Toxic organic dyes are a serious threat to the global environment, and membranes with catalytic properties show great promise as a green water treatment method for removing these pollutants. Herein, Ti 3 C 2 /W 18 O 49 photocatalytic membranes were constructed by vacuum filtrating Ti 3 C 2 and W 18 O 49 to form a hybrid layer on a mixed cellulose ester (MCE) support. The efficient separation of dyes was attributed to the negative charge and abundant –OH groups of Ti 3 C 2 /W 18 O 49 , which can capture cationic dyes by electrostatic adsorption and form hydrogen bonds with the amino groups of dye molecules. Moreover, the Ti 3 C 2 /W 18 O 49 membrane exhibited excellent photocatalytic performance and a dye-contaminated membrane was regenerated under visible light in 120 min. The two component materials complement each other, with the W 18 O 49 providing adsorption sites and photocatalytic ability and the Ti 3 C 2 serving as an electron trap and improving charge separation. Photoinduced electrons in the conduction band of W 18 O 49 are transferred to Ti 3 C 2 to form O 2 – , while holes remain in the valence band of W 18 O 49 to generate OH, and h + . O 2 – and OH are mainly responsible for the degradation of dyes. Therefore, this efficient and easily prepared membrane shows practical potential as a next-generation method for dye removal from water.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Shuangjie Sun,Yameng Wang,Binbin Sun,Feifei Zhang,Qing Xu,Hao-Yang Mi,Heng Li,Xiaoming Tao,Zhanhu Guo,Chuntai Liu,Changyu Shen
Solar steam generation is an efficient way of harvesting solar energy for water purification. Developing a versatile solar absorber with salt resistance and the capability to purify an oil-in-water emulsion is a grand challenge. Herein, a polypropylene (PP) nonwoven fabric-based photothermal absorber is fabricated by the combination of carbon nanotubes (CNTs), polypyrrole (PPy), and a fluorinated hydrophobic coating in a layer-by-layer approach. The specially designed architecture displays a hierarchical microstructure and Janus wetting properties, facilitating solar absorption and heat generation on the evaporation surface, and can effectively prevent salt crystallization. The water layer formed on the superhydrophilic/underwater superoleophobic bottom surface could repel oil droplets and form a channel to advect concentrated salt back into bulk water, which enabled high purity separation of an oil-in-water emulsion and continuous desalinization of seawater without the reduction of the evaporation rate. As a result, the solar absorber can achieve a remarkable evaporation rate of 1.61 kg m–2 h–1 and an energy efficiency of 91.2% under 1 sun irradiation and shows extraordinary performance in the purification of contaminated wastewater (over 99.8% purity). The strategy proposed provides a pathway for developing versatile high-performance solar absorbers for the sustainable treatment of saline water, wastewater, and oil-containing water.
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CHEMOSPHERE
·
2021
·
IF 7.086
Yu Li,Yong Feng,Bin Yang,Zequn Yang,Kaimin Shih
The activation of persulfate by ferrous iron (Fe(II)) is of great interest to the environmental remediation community, but the reduction of ferric iron (Fe(III)) to Fe(II) is slow and the accumulation of iron sludge resulted from the precipitation of Fe(III) is a great concern. Here, molybdenum disulfide (MoS 2 ) was studied as a co-catalyst to improve the activation of peroxymonosulfate (PMS) by Fe(III) for sulfadiazine (SDZ) degradation and different characterization technologies were used to reveal the reactive species. The results showed that a strong synergy existed between MoS 2 and Fe(III); approximately 94.3% of the SDZ was removed by MoS 2 -Fe(III)-PMS after reaction for 30 min, while only 8.5% and 56.4% of the SDZ was removed by Fe(III)-PMS and MoS 2 -PMS, respectively. Both hydroxyl radicals and sulfate radicals were generated and the latter was the primary species. In addition to the radicals, singlet oxygen was found to be generated and contributed to the degradation of SDZ. The chemical probe reaction with methyl phenyl sulfoxide showed that the generation of high-valent iron-oxo species was not obvious by MoS 2 -Fe(III)-PMS under both acidic and neutral conditions. MoS 2 had good stability. No noticeable deactivation was observed during the 1st to 5th run and no obvious oxidation of surface Mo(IV) occurred. Based on the characterization of catalyst and oxidizing species, a mechanism for the activation of PMS by MoS 2 -Fe(III) was proposed. The results from this study are expected to clarify the reactive species and deepen the understanding of MoS 2 -promoted persulfate activation by Fe(II)/Fe(III).
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Nano Research
·
2020
·Vol. 14
·期 3
·646-653
·
IF 8.183
Jiao Handong,Jiao Shuqiang,Song Wei-Li,Xiao Xiang,She Dongmei,Li Na,Chen Haosen,Tu Jiguo,Wang Mingyong,Fang Daining
Rechargeable Al-ion batteries (AIBs) are considered as one of the most fascinating energy storage systems due to abundant Al resource and low cost. However, the cycling stability is subjected to critical problems for using Al foil as negative electrode, including Al dendrites, corrosion and pulverization. For addressing these problems, here a lightweight self-supporting N-doped carbon rod array (NCRA) is demonstrated for a long-life negative electrode in AIBs. Experimental analysis and first-principle calculations reveal the storage mechanism involving the induced deposition of N-containing function groups to Al as well as the ideal skeleton of the NCRA matrix for Al plating/stripping, which is favorable for regulating Al nucleation and suppressing dendrites growth. Compared with the Al foil, the NCRA exhibits lower areal mass density (∼ 72% of Al foil), smaller thickness (40% of Al foil), but much longer cycle life (> 4 times of Al foil). Benefiting from the remarkable stability of the array structure, symmetric cells show excellent cycling stability with small voltage hysteresis (∼ 80 mV) and meanwhile there are no corrosion and pulverization problems even after cycled for 120 hours. Besides, full cells also manifest long lifespan (1,500 cycles) and increased Coulombic efficiency (100±1%).
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BIOMACROMOLECULES
·
2021
·
IF 6.988
Shuai Zhu,Ruizhong Xue,Zikun Yu,Xu Zhang,Shifang Luan,Haoyu Tang
Poly(l-cysteine)s with methylthio pendants (PMTLCs) were synthesized by ring-opening polymerization of a new l-cysteine-based N-carboxyanhydride. The thioether bonds of PMTLC can be readily oxidized by H2O2 yielding water-soluble PMTLCOX. The methylthio groups can undergo an alkylation reaction using methyl iodide and a subsequent ion-exchange reaction yielding sulfonium-based polypeptides (PPLC-DMS-X, where X = I, BF4). PPLC-DMS-X showed upper critical solution temperature-type thermo- and oxidation-responsive properties in aqueous solutions. Both PMTLC and PPLC-DMS-X showed oxidation-induced β-sheet to α-helix transitions. The absorbance of PPLC-DMS-I and methyl orange aqueous solution displayed a significant linear correlation with temperature, which makes the sulfonium-based polypeptides good candidates in the field of temperature sensors.
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Journal of the Taiwan Institute of Chemical Engineers
·
2021
·
IF 5.876
Junli Zheng,Linlin Du,Peng Gao,Kaiwei Chen,LiLi Ma,Yuanli Liu,Shaohong You
The excessive discharge of dye wastewater is a great threat to human health and environment with the development of industry. And it is of great significance to use biomass materials to remove dyes from wastewater with the low cost, renewability and environmental friendliness. In this study, the amine-modified passion fruit peel (ACPFP) was prepared by amination reaction, which exhibited highly efficient removal for anionic dyes (methyl orange (MO) and amaranth (ART)). The adsorption capacities of ACPFP for MO and ART were 1530.81 and 970.87 mg⋅g −1 , respectively. And the adsorption conditions (pH, ionic strength, temperature, initial dye concentration, and contact time) and mechanism (kinetic and isotherm models) were investigated. The results revealed that 99% of MO and ART was removed in the best adsorption conditions: pH=5, an adsorbent dose of 1 g⋅L −1 , 600 mg⋅L −1 of MO and ART initial concentration. The adsorption process correlated well with the pseudo-second-order kinetic model and the Langmuir isotherm. And ACPFP had good adsorption selectivity, stability and recyclability for anionic dyes. In conclusion, ACPFP has broad application prospects in actual water treatment.
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JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Shuangshuang Lin,Haiming Hua,Jiyang Li,Peng Zhang,Jinbao Zhao
We have found that the formation of passivation film plays a major role in the negative shift of the decomposition voltage in the hydrogen-generating process. Both the hydrolysis of weak acid ions and the decarboxylation reaction of carboxylate can make the LiCO 2 CH 3 produce a passivation film to inhibit the water decomposition to a certain extent. As for the LiCO 2 CF 3 without hydrolysis of weak acid ion, it can be highly possible to facilitate the introduction of CO 2 via its carboxylate specific decarboxylation reaction, and further produce lithium carbonate passivation film as well. However, the water decomposition voltage in the oxygen-producing process is more dependent on the properties of lithium salt anions. Those with strong electron-absorbing groups such as the trifluoromethyl are more likely to effectively endue the aqueous electrolyte with a high oxidative decomposition potential . Moreover, the concentration of LiCO 2 CF 3 aqueous electrolyte can reach up to 28 mol kg −1 , and hence the electrochemical stability window of this water-base electrolyte can be expanded to about 3.0 V. This work provides a new idea for the selection of high concentration lithium salt.
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