Catalysis Science & Technology
·
2021
·Vol. 11
·期 22
·7467-7474
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IF 6.119
Yangfan Ming,Gang Li
When Cu–TEPA (Cu2+ coordinated with tetraethylenepentamine) is used as a template in the one-pot synthesis of Cu–SSZ-13, Cu2+ will be reduced to Cu0, resulting in a too high Cu content in the product. Herein, by adding iron complexes to the precursor, the reduction of Cu2+ could be inhibited and FeCu–SSZ-13 samples with rational Cu and Fe contents were prepared by a simple one-pot strategy. Although these samples show high activity in the NH3-SCR at low temperature, their high temperature performance is poor due to the lack of strong NH3 adsorption sites such as Brønsted acid sites. Meanwhile, different iron complexes were used as iron sources to synthesize FeCu–SSZ-13, and among them the sample with sodium nitroprusside shows the highest activity. Due to the large ionic radius of K+, it is easily retained which blocks the pores, so the performance of the samples synthesized with a K-type iron source is poorer than that of their Na-type counterparts. Moreover, the activity of the catalyst synthesized with an Fe3+ source is higher than that synthesized with an Fe2+ source because the valence state of Fe sources has a great influence on the Fe chemical state in the catalysts.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 40
·19032-19042
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IF 3.591
Chengmin Hou,Hanxiao Ma,Congjun Cao,Xiaojian Ding,Jingting Duan
The composite particles (St/Fe3O4) of starch and Fe3O4 were prepared by a co-precipitation method. Then AA and HEMA were grafted and cross-linked on St/Fe3O4 by a one-step method to obtain St/Fe3O4-g-p(AA-r-HEMA). The effects of the adsorbent dosage, pH value, initial Cu(II) concentration, time and temperature on adsorption were studied. Experiments showed that St/Fe3O4-g-p(AA-r-HEMA) showed a good adsorption performance for Cu(II), with a unit adsorption capacity of 75.5 mg g−1 and a maximum removal rate of 95.0%. The adsorption process followed the Langmuir model and the pseudo-second-order kinetic model, was dominated by chemical adsorption, and belonged to single-layer adsorption. Renewable performance studies showed that after 8 adsorption cycles, 91.2% of the first adsorption effect was still retained.
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JOURNAL OF ELECTRONIC MATERIALS
·
2021
·Vol. 50
·期 6
·3222-3227
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IF 1.938
Han Wensong,Guo Qin,Su Tianhui
Cu@HBP-SH@Ag particles have been prepared by a facile synthesis strategy. Initially, thiol-terminated hyperbranched polymer (HBP-SH) was synthesized by stepwise polymerization. Subsequently, Cu particles covered with HBP-SH were prepared by reduction technology using HBP-SH as dispersant and template. Finally, Cu@HBP-SH@Ag particles were obtained by reduction reaction. Fourier-transform infrared (FT-IR) and ultraviolet–visible (UV–Vis) spectroscopy confirmed presence of HBP-SH on the surface of the Cu particles. The crystal structure was examined by x-ray diffraction (XRD) analysis. Scanning electron microscopy (SEM) and energy-dispersive spectrometry (EDS) analysis confirmed formation of Cu@HBP-SH@Ag particles. Thermogravimetric analysis (TGA) showed that the Cu@HBP-SH@Ag particles had better antioxidation properties than the Cu particles.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 13
·8372-8377
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IF 12.732
Songliang Liu,You Xu,Shiqian Jiao,Wenjing Tian,Tongqing Zhou,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Current methods for industrial-scale ammonia synthesis rely excessively on fossil fuels, causing severe CO2 emissions. The electrochemical nitrogen reduction reaction (NRR) is a sustainable and environmentally friendly technology for ammonia synthesis under environmental conditions. Herein, we demonstrate the rational construction of Au3Cu@Cu nanocages with unique porous core–shell heterostructured walls by a facile two-step synthetic strategy. Due to the hollow cavities, porous core–shell heterostructured walls, and Au3Cu@Cu two-component composition, the as-constructed Au3Cu@Cu nanocages exhibit excellent NRR performance in 0.1 M Na2SO4 saturated with N2, achieving a high ammonia yield up to 33.97 μg h−1 mgcat.−1 and a faradaic efficiency of 21.41% at −0.2 V (vs. the reversible hydrogen electrode). This study will provide insight into the reasonable design and construction of hollow nanostructures with porous heterostructured walls for electrocatalytic applications.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2021
·Vol. 96
·期 8
·2382-2389
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IF 3.174
Jianxin Tang,Jianmin Huang,Thein Tun,Sihua Liu,Jue Hu,Guiyin Zhou
BACKGROUND At present, various kinds of hydrogel adsorbents are applied to the treatment of heavy metal ions in wastewater. In this work, we focused on the adsorption of cadmium [Cd(II)] and copper [Cu(II)] onto microspheres of a novel thermosensitive hydrogel (NH 2 -SA/PNIPA, aminated sodium alginate/poly- N -isopropyl acrylamide), studied the effect of temperature on the phase transition of the hydrogel in detail, and discussed the influence on the adsorption behavior of metal ions in the hydrogel. RESULTS The NH 2 -SA/PNIPA exhibited a higher adsorption efficiency under the conditions of interfering monovalent cationic and neutral pH. The adsorption capacities based on the Langmuir model were 57.2 mg g –1 for Cu(II) and 100.5 mg g –1 for Cd(II) at 20 °C, respectively. Higher temperature facilitated the adsorption process and also led to the volume shrinkage and hydrophobicity of NH 2 -SA/PNIPA. The metal ions had different hydration and hence different adsorption capacities, of 56.7 mg g –1 for Cu(II) and 88.6 mg g –1 for Cd(II) at 40 °C. The results of diffusion behavior analysis showed that the diffusion coefficients were ≈1 × 10 −11 m 2 s –1 . The adsorption performance of NH 2 -SA/PNIPA hardly decreased even after five cycles. In addition, the adsorption process was controlled mainly by the complexation reaction. CONCLUSION The novel hydrogel microspheres overcame the deficiency of conventional adsorbents and possessed high diffusibility. This work provides a theoretical basis and empirical evidence for enhancement of adsorbents for removing heavy metals in wastewater. © 2021 Society of Chemical Industry (SCI).
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Wenxin Liu,Zhaofan Tao,Duo Wang,Qianqian Liu,Yinan Zhang,Yanling Zhang,Alideertu Dong
The past several decades have witnessed tremendous research to discover ways for controlling heavy metal pollution, but most of the strategies do not involve reuse of the captured heavy metals. Herein, we propose a graphene oxide -based strategy for the effective removal of Cu 2+ ions from water, coupled with their reuse as an antibacterial agent. Using GO nanosheets as an adsorbent and nanosupport, the Cu 2+ ions were effectively extracted from water (>99.9%) and reduced in situ to copper nanoparticles (Cu NPs) containing both crystalline Cu and Cu 2 O. The as-captured Cu NPs showed efficient in vitro antibacterial ability against Escherichia coli , reducing the bacteria from 10 9 to 10 1 CFU mL –1 by using 1 mg mL –1 Cu NPs/GO NSs for 1 h. The minimum inhibitory concentration determined to be only 16 μg mL –1 . For practical applications, Cu recovered from wastewater could reduce bacteria by 8 log CFU in 1 h. The recovered Cu was still able to reduce the bacteria by 7 log CFU after 2 months of storage in an argon atmosphere. This strategy of extracting heavy metals and subsequently reutilizing to kill bacteria will be of great significance for environmental remediation and public healthcare.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yanqiao Xu,Ting Chen,Zhixiang Xie,Weihui Jiang,Lianjun Wang,Wan Jiang,Xiaojun Zhang
Understanding the surface characteristic-optical property relationship of Cu-In-Zn-S (CIZS) quantum dots (QDs) is necessary for tuning the optoelectronic performances, and the photoluminescence quantum yields (PLQYs) of CIZS QDs prepared in aqueous solution are still relative low compared with that of obtained in organic phase, which seriously restricts their applications. Herein, an efficient method was proposed to prepare CIZS/ZnS/PVP composites and their application in white light-emitting diodes (WLEDs) was investigated. CIZS QDs were synthesized through hydrothermal process with the assistance of ionic liquid (IL), which could enhance the PL performance and reduce the reaction time simultaneously. The effects of hydrothermal temperature and time on the phase composition, morphology, and optical properties of CIZS QDs were systematically investigated. The results showed that the BF 4 − anion played a crucial role in boosting the emission property of CIZS QDs owing to the effective reduction of dangling bonds on the surface of QDs, which induced by the corrosion of F − deriving from the decomposition of BF 4 − . The surface modulation led to the improvement of PLQY from 6.2% to 8.4%. In addition, the PLQY of QDs was further improved to 31.2% by coating with ZnS shell around CIZS cores. Furthermore, highly luminescent CIZS/ZnS/PVP composites were prepared to eliminate the aggregation-induced fluorescence quenching effect, which was beneficial to the application in WLEDs. Consequently, a WLED achieved the color rending index (CRI) of 87.2, correlated color temperature (CCT) of 4977 K, and luminous efficacy (LE) of 90.11 lm/W by using the orange-yellow CIZS/ZnS/PVP composites and green Lu 3 Al 5 O 12 :Ce 3+ phosphors as the color conversion layer, suggesting the potential for solid state lighting application.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Kun Wu,Meng Wang,Angzhen Li,Zixuan Zhao,Ting Liu,Xiaodan Hao,Shengjiong Yang,Pengkang Jin
Mn-oxide-containing adsorbents have shown outstanding performances for the removal of As(III) through an “oxidation-adsorption” process. In this study, a new adsorbent of Fe-Mn-Cu ternary oxide (FMCTO) was fabricated to improve the redox reaction rate and to enhance the recovery of oxidative ability. FMCTO exhibited a stronger ability for As(III) removal than most of other adsorbents, because it has better oxidative capability for As(III) oxidation. The state of dynamic equilibrium for As(III) removal by FMCTO could be basically achieved within 3 h, and the As removal efficiency reached 98.9% at time = 24 h. The Langmuir As adsorption capacity of FMCTO was determined to be 204.8 mg/g. The As(III) removal efficiency of FMCTO was further boosted by 7% through oxygen gas aeration and decreased by 19% with nitrogen gas in the ambient during the first 3 h, indicating the positive effect of oxygen on As(III) oxidation. EPR and UV spectra methods were used to confirm the generation of superoxide radical (O 2 − ) and the enhanced production of Mn(III) soluble species on FMCTO surfaces, thus achieving a better As(III) oxidation performance. The XPS analysis results showed that the electron transfer from Cu(I) to Mn(IV) could improve the stability of Mn(III) within FMCTO. Meanwhile, Mn(II) ions could be oxidized to Mn(III) by O 2 − . Hence, the formation of a redox cycle between Mn(II) and Mn(III) along with the production of O 2 − plays a vital role in the upgraded As(III) removal mechanisms. This study provides new insights into the promotion of the capability of Mn-containing adsorbents for achieving the improved removal of As from As(III)-contaminated water.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2020
·
IF 3.232
Lan-Fang Pang,Hao Wu,Meng-Xia Wei,Xiao-Feng Guo,Hong Wang
The spores of Bacillus anthracis are highly deadly to human beings and animals, and are concurrently potential biological warfare agents. Hence, the rapid and sensitive monitoring Bacillus anthracis biomarker, dipicolinic acid (DPA), is very desirable. Herein, orange/green dual-emissive carbon dots (OG-CDs) were synthesized via the hydrothermal approach. The OG-CDs not only emitted dual fluorescence at 527 and 590 nm under the single 503 nm excitation, but also exhibited excellent water solubility, good photostability and great salt tolerance. The fluorescence of the OG-CDs at 527 nm can be completely quenched when chelated with Cu(II). However, because of the stronger chelation between DPA and Cu(II), the fluorescence restored rapidly on subsequent addition of DPA. As such, the CD-Cu(II) system can be used for determination of DPA based on the fluorescence “off-on” response. Under optimum conditions, the detection limit for DPA was 56 nM, with a linear range of 0.5–12.5 μM. The established CD-Cu(II) based spectrofluorometric method has been applied to the analysis of DPA in real water samples with recoveries of 93.6%–104.3%. More remarkably, the CD-Cu(II) probe also has been successfully applied for the imaging of DPA in Escherichia coli with excellent bio-compatibility.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Lele Cui,Zhiwen Li,Qingqing Li,Meifei Chen,Wenheng Jing,Xuehong Gu
The development of transition metal oxide-based integrated carbonaceous materials for use as bifunctional electrodes of high stability and activity in the heterogeneous electro-Fenton (EF) process is supposed to have great potential in environmental governance. Herein, Cu/CuFe 2 O 4 (CCFO) with different Cu 0 ratios were synthesized by a facile one-step solvothermal approach. These materials were subsequently used to fabricate modified graphite felt through the polytetrafluoroethylene (PTFE)-bonding technique. Importantly, with its hydrophobicity PTFE effectively inhibited metal leaching from the thus obtained cathodes and improved the oxygen utilization rate. Cathode performance in EF-based tetracycline (TC) degradation was found to increase with Cu 0 ratio. The observed increase in activity was attributed to Cu 0 enhancing the 2-electron oxygen reduction reaction selectivity (i.e., H 2 O 2 production) and endowing the cathode with abundant electron-rich centers that accelerated active Fe(II) regeneration, causing rapid conversion of H 2 O 2 to hydroxyl radical ( OH). The possible TC mineralization pathway was inferred by liquid chromatography–mass spectrometry (LC–MS) analysis, and a catalytic mechanism of the heterogeneous EF process was proposed. The most effective cathode fabricated displayed high stability even at pH 3 (0.84 ± 0.11 mg/L Fe and 1.35 ± 0.17 mg/L Cu leaching) and exhibited nearly 80% TC removal efficiency after five oxidation cycles, demonstrating its potential use in heterogeneous EF technology for efficient and durable wastewater treatment.
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JOURNAL OF HAZARDOUS MATERIALS
·
2020
·
IF 9.038
Xinpeng Liu,Baohua Wang,Xiaoli Lv,Qingmei Meng,Menghong Li
The H 2 S removal performances of four deep eutectic solvent (DES) based nanofluid (NF) systems were measured using dynamic absorption experiment. The Cu containing NF system is found to be an excellent absorbent for H 2 S removal with a significantly enhanced desulfurization performance compared with DES original solution. Besides, the NF systems have relatively high regeneration performance. The NF systems and Cu nanoparticles before and after absorption as well as after regeneration were characterized by Fourier transform infrared (FT-IR) spectra, scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), transmission electron microscope (TEM) and energy dispersive spectrum (EDS). It is found that the ethanolamine , choline cation and sulfur were accumulated on the surface of Cu nanoparticles after absorption, and the bulk elements on the surface were identified as Cu and S after regeneration. The S −2 was existed in the form of Cu 2 S, and some sulfur was oxidized to zero-valent sulfur after regeneration.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Xin Zhou,Haopeng Luo,Bo Sheng,Xingyu Chen,Yihao Wang,Quanyuan Chen,Juan Zhou
The limited production of Cu + in the Cu 2+ /PMS processes constrained its large-scan application for the elimination of organic pollutants . In this study, molybdenum powder (Mo) was applied as the co-catalyst to improve the degradation of 2,4-dichlorophenol (2,4-DCP) in Cu 2+ /PMS system at pH 5.6. By the assistance of Mo, Cu 2+ was rapidly reduced to Cu + which exhibited super activity for the peroxymonosulfate (PMS) activation. Compared with Cu 2+ /PMS processes, the PMS decomposition rate and 2,4-DCP degradation efficiency respectively increased by 62.1% and 83.6% in the Mo co-catalytic Cu 2+ /PMS system after reaction for 20 min. The degradation of 2,4-DCP was completed via both the free radical and non-radical pathways and the free radicals rather than Cu 3+ contributed most to the reaction. In contrast to fresh Mo, the ratio of Mo 4+ increased and Mo 6+ decreased in the used Mo powder, due to the oxidation of Mo 0 by Cu 2+ and/or ∙OH and the reduction of Mo 6+ by O 2 ∙ − . Additionally, the coexistence of Cl - and humic acid with low concentrations showed little effects on the Mo/Cu 2+ /PMS system while HCO 3 − presented an obvious depression for 2,4-DCP degradation. During five cycling runs, all the degradation rates were higher than 92.8%, indicating the good stability of Mo/Cu 2+ /PMS system.
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