MICROCHIMICA ACTA
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2022
·Vol. 189
·期 9
·1-10
·
IF 6.408
Zhou Xuemei,Qi Yuji,Tang Yulian,Gao Hui,Lv Li,Lei Xingyu,Hu Lei,Yan Zhengquan
To enhance the peroxidase-like performance and its application in detection of toxic o -aminophenol ( o -AP), a kind of bimetal Cu–Zn oxide-based mesoporous nanosphere (Cu 2/3 Zn 1/3 O PNPs) was constructed under microwave-radiation conditions. Its mesoporous microstructure and peroxidase-like catalytic activity were investigated in detail. The results showed that Cu 2/3 Zn 1/3 O PNPs possessed a high specific surface area of 34.89 m 2 g −1 and a well-distributed mesoporous size of approximate 6.07 nm, which endowed the superior peroxidase-like performance. The material catalyzes the oxidization of 3,3′,5,5′-tetramethylbenzidine (TMB) with K m / V max of 0.104 mM/3.79 × 10 −8 M·s −1 in the presence of H 2 O 2 . Especially o -AP could exclusively deteriorate the characteristic UV–Vis absorbance intensity at 653 nm ( A 653 ) of the Cu 2/3 Zn 1/3 O PNPs-TMB-H 2 O 2 system with obvious color change from blue to colorless. Under the optimal conditions, the effect of some interfering substances was low and the limit of detection (LOD) for o -AP was 1.65 × 10 −8 mol/L (S/N = 3). When applied to the colorimetric detection of o -AP in practice, the recovery was between 96.1 and 107.2% with R.S.D. less than 2.04%. The mechanism of synergic-enhancement peroxidase-mimic activity of Cu 2/3 Zn 1/3 O PNPs and its exclusive colorimetric response to o -AP were proposed as well. Graphical abstract
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Scientific Reports
·
2021
·Vol. 11
·期 1
·1-9
·
IF 4.38
Zhang Shujie,Zhang Yating,Fu Lisong,Jing Mengke
The application shell uses cellulose as a green and recyclable fiber material, which has great value in the field of water treatment environment. Varying factors, including pH value, dosage of CS, reaction time and original Cr(VI) ions and Cu(II) ions were studied to investigate the Cr(VI) and Cu(II) ions removal efficiency. The obtained shell trichlorocellulose has better permeability to copper ions, which is mainly due to the different oxide states of copper ions and chromium ions in a pH environment, which lead to different combinations. The price of shell cellulose neutralization is relatively low. Metal ions have better absorption properties. The kinetic and thermodynamic characteristics of the adsorption process of copper ions by chitosan yarns were discussed. The adsorption process of copper ions conformed to the quasi-second-order kinetic equation. It can be fitted by Langmuir isotherm. The adsorption of copper ions by the yarn is a spontaneous thermal reaction with both physical adsorption and chemical adsorption. Compared with chromium ions, chitosan fibers have better adsorption of copper ions, which is mainly because the amino groups in chitosan fibers can have good chelation with copper ions. SEM, FTIR, XRD were used to characterize the adsorption of copper ions by chitosan fibers, and the mechanism of the adsorption of metal ions by chitosan fibers was explored.
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Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Linhai Yang,Xuechang Ren,Yujie Zhang,Zuoyan Chen
This article is an in-depth study of the basis of Cu + -decorated triazine-based g-C 3 N 4 (Cu + /g-C 3 N 4 ) nanosheet-activated H 2 O 2 . In this study, peroxymonosulfate (PMS) was activated by Cu + /g-C 3 N 4 under sunlight and used to treat simulated wastewater RhB. The properties of g-C 3 N 4 and Cu + /g-C 3 N 4 were characterized by UV–Vis DRS and PL . The results indicated that the introduction of Cu + in g-C 3 N 4 can enhance the separation of photogenerated electron-hole pairs. The Cu + /g-C 3 N 4 (1:4) samples exhibited the best PMS activation performance under sunlight when 0.5 g/L catalyst dose and 0.5 mmol/L PMS concentration were used, and the removal rate of RhB reached 95.7% in 30 min. Moreover, better catalytic activity of the system can be achieved in the initial pH range of 2.0–10.0. The investigation results of the catalytic mechanisms showed that the prepared Cu + /g-C 3 N 4 catalyst constructs a dual reaction center of Cu + /Cu 2+ cycling and e CB − / h VB + transfer for efficient PMS activation. The degradation of pollutants benefits from the participation of a variety of free radicals, which are generated by sunlight-assisted heterogeneous activation of PMS. This study has resulted in substantial progress in activating multiple oxidants with a single heterogeneous catalyst and provides a feasible way to treat refractory wastewater using Cu + /g-C 3 N 4 with PMS under sunlight.
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CHEMOSPHERE
·
2021
·
IF 7.086
Fuyou Du,Zhan Lai,Huiyang Tang,Haiyan Wang,Chenxi Zhao
In this work, a novel BiOCl/Cu-doped Bi 2 S 3 photocatalyst was designed to efficiently remove ciprofloxacin (CIP) with high photocatalytical activity and good stability over a wide pH range. Compared with Cu-doped Bi 2 S 3 , Bi 2 S 3 , BiOCl, BiOCl/Bi 2 S 3 , and Cu-doped BiOCl, the photocatalytical degradation rate of CIP (97.1% at 20 mg/L) over BiOCl/Cu-doped Bi 2 S 3 was enhanced by about 84.77, 44.23, 2.95, 2.27, and 1.96 times within 20 min, respectively. Notably, the BiOCl/Cu-doped Bi 2 S 3 photocatalyst also displayed high photocatalytical performance in the degradation of other antibiotics including norfloxacin, ofloxacin, and tetracycline (40 mL, 20 mg/L; 88.3%, 100%, and 95.2% of degradation rate within 30 min, respectively) under visible light irradiation. Radical trapping experiments and electron spin resonance technique indicated that superoxide radicals (•O 2 − ) and photogenerated holes (h + ) played crucial roles in the photocatalytic degradation of CIP. Finally, the possible CIP degradation pathways was proposed by detecting the CIP intermediates in photocatalytical reaction process.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
·
IF 9.028
Shuhui Sun,Chao Shan,Zhichao Yang,Shu Wang,Bingcai Pan
Phosphonate is an important category of highly soluble organophosphorus in contaminated waters, and its oxidative transformation into phosphate is usually a prerequisite step to achieve the in-depth removal of the total phosphorus. Currently, selective oxidation of phosphonate into phosphate is urgently desired as conventional advanced oxidation processes suffer from severe matrix interferences. Herein, we employed 1-hydroxyethylidene-1,1-diphosphonic acid (HEDP) as a model phosphonate and demonstrated its efficient and selective oxidation by the Cu(II)/H2O2 process at alkaline pH. In the presence of trace Cu(II) (0.020 mM), 90.8% of HEDP (0.10 mM) was converted to phosphate by H2O2 in 30 min at pH 9.5, whereas negligible conversion was observed by UV/H2O2 or a Fenton reaction (pH = 3.0). The oxidation of HEDP by Cu(II)/H2O2 was insignificantly affected by natural organic matters (10.0 mg TOC/L) and various anions including chloride, sulfate, and nitrate (10.0 mM). The complexation of Cu(II) with HEDP coupling Cu(III) produced in situ enabled an intramolecular electron transfer process, which features high selective oxidation. Selective degradation of HEDP was further validated by adding stoichiometric H2O2 into an industrial effluent, where the existing Cu(II) could serve as the catalyst. This study also provides a successful case to trigger selective oxidation of trace pollutants of concern upon synergizing with the nature of the contaminated water.
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Journal of the Taiwan Institute of Chemical Engineers
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2021
·
IF 5.876
Yang Bai,Gongzhe Nie,Yi He,Chao Li,Xianbo Wang,Liqun Ye
Background The Fenton-like reaction is a highly potential advanced oxidation process. The photo-Fenton-like reaction formed by the combination of photocatalytic advanced oxidation process, which combines their advantages, breaks the original Fenton-like reaction rate bottleneck. Methods In this study, an ultra-thin MOF (Cu-TCPP(BA)-MOF) with porphyrin as the ligand and copper as the metal node was synthesized via a simple one-pot method for the first time. Significant Findings It activates Peroxymonosulfate (PMS) under visible light to degrade 10 mg/L Rhodamine B which can be completely degraded within 40 min. The pseudo-first-order rate constant of RhB is 0.9011 min −1 , being 5 folds larger than this for CuO as catalysts. ESR analysis shows that Cu-TCPP(BA)-MOF/PMS/vis system produces a large amount of non-radical 1 O 2 . Also under visible light, with E. coli concentration of 10 7 cfu/mL, it can be completely inactivated within 50 min. Dilution spreading plate method and Fluorescence spectroscopy confirmed the complete death of bacteria. In terms of mechanism, the ultra-thin MOF provides a large number of Cu 2+ active sites. Under visible light, the cycle between Cu 2+ and Cu + is accelerated and the pathways that produce reactive oxygen species (ROS) is changed, thereby improving the performance of contaminant treatment and sterilization.
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MATERIALS RESEARCH BULLETIN
·
2021
·
IF 4.641
Chuanfu Song,Kunyuan Chen,Xin Jin,Xinyu Zhao,Guangrong Liu,Feifei He,Qiang Huang
The biochar-supported Cu 2 O/Cu composite (Cu 2 O/Cu/BC) was fabricated by direct pyrolysis of hemp hurds pretreated with KOH and CuCl 2 , in which the synchronous carbonization-activation-functionalization was achieved to produce copper-modified biochars. Cu 2 O/Cu/BCs were characterized by XRD , Raman, XPS , SEM and N 2 adsorption-desorption techniques. The adsorption methyl orange by Cu 2 O/Cu/BCs showed that the incorporation of Cu 2 O/Cu has improved the adsorption capacity. The adsorption obeyed the pseudo-second-order kinetic model and Langmuir isotherm. The maximum adsorption capacity reached 379.4 mg∙g -1 at 303.5 K. Furthermore, assisted with the photoactivity of Cu 2 O/Cu heterojunction the saturated adsorbent can be regenerated under simulated sunlight, and the re-adsorption capacity was still as high as 77.1% of the fresh adsorbent after six cycles. The regeneration efficiency was much better than traditional thermal regeneration and solvent treatment. This work should allow to provide a convenient preparation of functionalized biochars and to develop solar-driven, self-regenerative sorbents for water decontamination with high efficiency.
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RSC Advances
·
2021
·Vol. 12
·期 1
·602-610
·
IF 3.361
Yingxin Liu,Kai Liu,Meihua Zhang,Kaiyue Zhang,Jiao Ma,Shuwen Xiao,Zuojun Wei,Shuguang Deng
Highly active and thermally stable Cu–Re bimetallic catalysts supported on TiO2 with 2.0 wt% loading of Cu were prepared via an incipient wetness impregnation method and were applied for liquid phase selective hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) in H2. The effect of the molar ratios of Cu : Re on the physico-chemical properties and the catalytic performance of the Cu–Re/TiO2 catalysts was investigated. Moreover, the influence of various reaction parameters on the hydrogenation of LA to GVL was studied. The results showed that the Cu–Re/TiO2 catalyst with a 1 : 1 molar ratio of Cu to Re (Cu–Re(1 : 1)/TiO2) exhibited the highest performance for the reaction. Complete conversion of LA with a 100% yield of GVL was achieved in 1,4-dioxane solvent under the reaction conditions of 180 °C, 4.0 MPa H2 for 4 h, and the catalyst could be reused at least 6 times with only a slight loss of activity. Combined with the characterization results, the high performance of the catalyst was mainly attributed to the well-dispersed Cu–Re nanoparticles with a very fine average size (ca. 0.69 nm) and the co-presence of Cu–Re bimetal and ReOx on the catalyst surface.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yu Chen,Senqing Fan,Boya Qiu,Jiaojiao Chen,Zenghui Mai,Yilin Wang,Ke Bai,Zeyi Xiao
A bimetallic catalytic membrane microreactor (CMMR) with bimetallic nanoparticles in membrane pores has been fabricated via flowing synthesis. The bimetallic nanoparticle is successfully immobilized in membrane pores along its thickness direction. Enhanced synergistic catalysis can be expected in this CMMR. As a concept-of-proof, Cu–Ag core–shell nanoparticles have been fabricated and immobilized in membrane pores for p-nitrophenol (p-NP) hydrogenation. Transmission electron microscopy (TEM) for the characterization of the bimetallic core–shell nanostructure and X-ray photoelectron spectroscopy (XPS) for the characterization of the electron transfer behavior between Cu–Ag bimetal have been performed. The Ag shell on the core of Cu can improve the utilization of Ag atoms, and electron transfer between bimetallic components can promote the formation of high electron density active sites as well as active hydrogen with strong reducing properties on the Ag surface. The dispersed membrane pore can prevent nanoparticle aggregation, and the contact between the reaction fluid and catalyst is enhanced. The enhanced mass transfer can be achieved by the plug-flow mode during the process of hydrogenation catalysis. The p-NP conversion rate being over 95% can be obtained under the condition of a membrane flux of 1.59 mL·cm–2·min–1. This Cu–Ag/PES CMMR has good stability and has a potential application in industry.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Xinyue He,Tao Zhang,Qing Xue,Yalan Zhou,Hailong Wang,Nanthi S. Bolan,Rongfeng Jiang,Daniel C.W. Tsang
Heavy metals removal from aqueous phase by adsorption technique has recently attracted a considerable interest. Although various adsorbing materials have been developed, introducing more functional groups is considered as the most efficient way to promote the adsorption capacity of the selected adsorbent. However, this approach is usually limited in costly modification precursor and unguaranteed loading efficacy. In this study, waste corn straw was converted to adsorbent precursor by hydrothermal carbonization . The obtained hydrochar (HC) was chemically activated before being modified by polyethyleneimine (PEI). Multiple analysis methods including Scanning Electron Microscopy, Fourier Transform Infrared analysis, and X-ray Photoelectron Spectroscopy analysis verified the alkali activated hydrochar (alkali-HC) was more efficacy to enhance PEI grafting than acid activation . Based on this, the modified HC materials obtained a better adsorption performance. The sorption process of Cu(II) and Zn(II) on the acid-PEI-HC, alkali-PEI-HC, and pristine HC fitted the pseudo second order kinetic and Freundlich model well, and was dominated by chemisorption . Among these adsorbents, the adsorption capacity of alkali-PEI-HC to metal ions was the maximum, which was 207.6 mg/g to Zn(II) and 56.1 mg/g to Cu(II) at 298 K. Regeneration tests showed a result of no less than 60% of its removal capacity was achieved after five cycles. Therefore, alkali-PEI-HC performed as a promising composite sorbent for metal ions. In addition, the study described here has provided a new basis for the utilization of hydrochar (1.08 kWh kg −1 ) derived from agricultural resources as a promising adsorbent precursor.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Yuzhou Wu,Xubin Zhang,Fumin Wang,Yi Zhai,Xianbao Cui,Guojun Lv,Tao Jiang,Jiaqi Hu
Direct hydroxylation of benzene to phenol is an effective and environment-friendly route to obtain phenol. Herein, Fe-doped and cupric acetylacetonate [Cu(acac)2]-grafted mesoporous silica (Cu/Fe-SBA-15) with highly dispersed metallic sites has been synthesized and used as a heterogeneous catalyst in the hydroxylation of benzene. The physiochemical properties of the synthesized materials as well as the reciprocity between iron and copper sites were analyzed by several characterization techniques including nitrogen adsorption–desorption, X-ray diffraction, transmission electron microscopy, UV–vis diffuse reflectance spectroscopy, Fourier transform infrared spectroscopy, and X-ray photoelectron spectroscopy. In direct hydroxylation of benzene with H2O2 as the oxidant, the prepared Cu/Fe-SBA-15 material showed great catalytic activity. Moreover, the synergistic effect between doped Fe sites and grafted Cu sites was also investigated. In this catalyst, Fe and Cu species both played the role of active sites. Excessive activity of iron would lead to benzene peroxidation, while the presence of copper sites could effectively hinder benzene peroxidation.
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WATER RESEARCH
·
2021
·
IF 11.236
Jingxin Yang,Yujie Luo,Xianghui Fu,Zijun Dong,Chuan Wang,Hong Liu,Chengchun Jiang
Transition metal catalyzed sulfite auto-oxidation is a promising technology used in water and wastewater treatment for the elimination of contaminants. In the literature, this process has been reported to be efficient only in the presence of oxygen. However, in this study, we unexpectedly found that the degradation of diatrizoate (DTZ) by a system based on the combination of copper ion and sulfite (Cu(II)/S(IV)) reached over 95% under anaerobic conditions , but was considerably retarded under aerobic conditions at pH 7. Furthermore, it was found that Cu(I), generated from the cleavage of the CuSO 3 complex, was the main reactive species responsible for the degradation of DTZ by the Cu(II)/S(IV) system under anaerobic conditions. In fact, the absence of oxygen promoted the accumulation of Cu(I). The concomitant release of the iodide ion with the degradation of DTZ indicated that the anaerobic degradation of DTZ by the Cu(II)/S(IV) system mainly proceeded through the deiodination pathway, which was also confirmed by the detection of deiodinated products. The anaerobic degradation of DTZ was favored at higher initial concentrations of Cu(II) or sulfite in this system. Since the CuSO 3 complex, the precursor of Cu(I), was formed mainly at pH 7, the highest anaerobic degradation of DTZ was achieved at pH 7. An increase in reaction temperature considerably enhanced the degradation of DTZ by the Cu(II)/S(IV) system with an apparent activation energy of 119.4 kJ/mol. The presence of chloride, bicarbonate and humic acid slightly influenced the anaerobic degradation of DTZ. The experiments with real water samples also demonstrated the effectiveness of the degradation of DTZ by the Cu(II)/S(IV) system under anaerobic conditions.
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