APPLIED SURFACE SCIENCE
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2022
·
IF 7.392
Zhiqiang Zhang,Ruijie Chen,Lei Wang,Xueru Chen,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic reduction of CO 2 to methanol over SrTiO 3 (ST) perovskite oxide is considered as a promising method to alleviate environment and energy problems at the same time. Meanwhile, the inducing of Cu plays an important role in photocatalytic activity and selectivity. Herein, a series of SrTi 1-x Cu x O 3 -H 2 (STCu x -H, x = 0.04, 0.06, 0.08, and 0.1) nanofiber catalysts were prepared by electrospinning combined with in-situ dissolution strategy. Cu x O dissolved in situ on a one-dimensional nanofiber structure could realize more active sites exposed and convenient directional movement of electrons, simultaneously. The unique structure facilitates the enhancement of photocatalytic activity and the improvement of selectivity. The methanol yield of STCu 0.08 -H nanofiber catalyst upped to 5.38 ± 0.19 μmol·g −1 ·h −1 , which was twice that of ST. Moreover, the photocatalytic activity did not decrease significantly after four times of reuse. The characterization further demonstrated that STCu 0.08 -H had stronger light response ability and faster electron transfer ability than ST under the synergistic action of Cu 2+ and Cu + . STCu 0.08 -H had superior CO 2 adsorption, activation ability, and electronic reduction capability by DFT calculation. This study provided a new idea about the design of perovskite oxide nanofiber for photocatalytic CO 2 reduction.
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Polymers
·
2022
·Vol. 14
·期 19
·4187
·
IF 4.967
Jia Qu,Liangliang Chang,Mingbao Liu,Baoyue Cao,Meilan Li,Qiang Yang,Wei Gong
Beneficiation wastewater contains various types of pollutants, such as heavy metal ions and organic pollutants. In this work, a silica-based amphiphilic block copolymer, SiO2–g–PBMA–b–PDMAEMA, was obtained by surface-initiated atom transfer radical polymerization (SI-ATRP) for Cu(II) and sodium oleate adsorption in beneficiation wastewater, using butyl methacrylate (BMA) as a hydrophobic monomer and 2-(dimethylamino)ethylmethacrylate (DMAEMA) as a hydrophilic monomer. FTIR, TGA, NMR, GPC, XRD, N2adsorption–desorption isotherms and TEM were used to characterize the structure and morphology of the hybrid adsorbent. The introduction of PBMA greatly increased the adsorption of sodium oleate on SiO2–g–PBMA–b–PDMAEMA. Adsorption kinetics showed that the adsorption of Cu(II) or sodium oleate on SiO2–g–PBMA–b–PDMAEMA fitted the pseudo-second-order model well. Adsorption isotherms of Cu(II) on SiO2–g–PBMA–b–PDMAEMA were better described by the Langmuir adsorption isotherm model, and sodium oleate on SiO2–g–PBMA–b–PDMAEMA was better described by the Freundlich adsorption isotherm model. The maximum adsorption capacity of Cu(II) and sodium oleate calculated from Langmuir adsorption isotherm equation reached 448.43 mg·g−1and 129.03 mg·g−1, respectively. Chelation and complexation were considered as the main driving forces of Cu(II) adsorption, and the van der Waals force as well as weak hydrogen bonds were considered the main driving forces of sodium oleate adsorption. The adsorbent was recyclable and showed excellent multicomponent adsorption for Cu(II) and sodium oleate in the mixed solution. SiO2–g–PBMA–b–PDMAEMA represents a satisfying adsorption material for the removal of heavy metal ions and organic pollutants in beneficiation wastewater.Keywords:silica;amphipathic;block copolymer;adsorption;beneficiation wastewater;Cu(II);sodium oleate
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Journal of Environmental Sciences
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2022
·
IF 6.796
Xin Yang,Xingyun Hu,Linghao Kong,Xianjia Peng
The selective recovery of copper from strongly acidic wastewater containing mixed metal ions remains a significant challenge. In this study, a novel reagent zinc dimethyldithiocarbamate (Zn(DMDC) 2 ) was developed for the selective removal of Cu(II). The removal efficiency of Cu(II) reached 99.6% after 120 min reaction at 30°C when the mole ratio Zn(DMDC) 2 /Cu(II) was 1:1. The mechanism investigation indicates that the Cu(DMDC) 2 products formed as a result of the displacement of Zn(II) from the added Zn(DMDC) 2 by Cu(II) in wastewater, due to the formation of stronger coordination bonds between Cu(II) and the dithiocarbamate groups of Zn(DMDC) 2 . Subsequently, we put forward an innovative process of resource recovery for strongly acidic wastewater. Firstly, the selective removal of Cu(II) from actual wastewater using Zn(DMDC) 2 , with a removal efficiency of 99.7%. Secondly, high-value CuO was recovered by calcining the Cu(DMDC) 2 at 800°C, with a copper recovery efficiency of 98.3%. Moreover, the residual As(III) and Cd(II) were removed by introducing H 2 S gas, and the purified acidic wastewater was used to dissolve ZnO for preparation of valuable ZnSO 4 ·H 2 O. The total economic benefit of resource recovery is estimated to be 11.54 $/m 3 . Accordingly, this study provides a new route for the resource recovery of the treatment of copper-containing acidic wastewater.
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ACS Omega
·
2022
·
IF 4.132
Feiyu Yang,Jiamin Wang,Kailiang Yin,Huan Pang
Control and detection of sunset yellow (SY) are an utmost demanding issue due to its high risk of detrimental effects on living systems caused by excessive ingestion. In this study, we reported the synthesis of Cu@Cu2O nanoparticle-decorated B and N codoped porous carbon (BNPC) and its use in developing a novel electrochemical sensor for SY. The Cu@Cu2O-BNPC catalyst was fabricated through single-step polymerization, followed by carbonization. Scanning electron microscopy, transmission electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy characterization results showed that Cu@Cu2O anchored on the porous BNPC successfully. Compared with the BNPC-modified electrode, it was found that the Cu@Cu2O-BNPC-modified electrode showed superior electrocatalytic activity in both electrochemical impedance spectroscopy and cyclic voltammetry tests. The as-prepared Cu@Cu2O-BNPC catalyst directly acted as a sensor for amperometric detection of SY without further assembling, which exhibited an ultrahigh sensitivity of 0.09 μA nM–1 cm–2, a low limit of detection (2.4 nM), and a wide linear detection ranging from 10 nM to 8 μM. To further validate its possible application, the proposed method was successfully used for the determination of SY in Fanta drinks with satisfactory results.
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RSC Advances
·
2022
·Vol. 12
·期 35
·22806-22814
·
IF 4.036
Shengnan Li,Ziteng Niu,Yuke Jiao,Peng Jin,Desheng Yang,Chaofei Bai,Jiaran Liu,Guoping Li,Yunjun Luo
Cu nanoparticles are more active catalytically than CuO nanoparticles, which have been widely studied as catalysts for organic synthesis, electrochemistry, and optics. However, Cu nanoparticles are easily agglomerated and oxidized in air. In this research, columnar, flower-like, bubble-like and teardrop-shaped Cu/GO nanocomposites were fabricated via a water-solvent thermal method and high temperature calcination technique using deionized water (H2O), methanol (CH3OH), ethanol (CH3CH2OH) and ethylene glycol (EG) as the solvent, respectively. The structures, the morphology and the catalytic performance and catalytic mechanism for thermal decomposition of ammonium perchlorate (AP) of the Cu/GO nanocomposites have been studied by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), scanning electron microscopy (SEM), nitrogen adsorption tests (BET), simultaneous thermogravimetry-differential scanning calorimetry (TGA/DSC) and thermogravimetric couplet with Fourier transform infrared spectroscopy (TGA–FTIR), respectively. The experimental results show that the morphology of the Cu/GO nanocomposites has a significant effect on the surface area and the teardrop-shaped Cu/GO nanocomposites have the largest specific surface area and the best catalytic performance among them. When 5 wt% of the Cu/GO nanocomposites was added, the decomposition temperature of AP decreased from 426.3 °C to 345.5 °C and the exothermic heat released from the decomposition of AP increased from 410.4 J g−1 to 4159.4 J g−1. In addition, the four morphological Cu/GO nanocomposites exhibited good stability, their catalytic performance for thermal decomposition of AP remained stable after 1 month in air. Excellent catalytic performance and stability were attributed to the strong catalytic activity of pure metal nanoparticles, and GO can accelerate electron movement and inhibit the agglomeration of nanoparticles, as well as the multiple effects of inhibiting the oxidation of Cu nanoparticles in air. Therefore, it has important application potential in high-energy solid propellant.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Guoqiang Li,Siqi Chai,Guojie Zhang,Jun Liu,Yongfa Zhang,Yongkang Lv,Ying Wang,Yuqiong Zhao
In this paper, Ce-modified Cu-based carbon materials (Cu-Ce/AC) were prepared by impregnation method using walnut shell as the carbon precursor, Cu-ammonia solution as Cu source and Ce as modifier. The catalytic wet air oxidation (CWAO) degradation of phenol wastewater was carried out in a self-assembled fixed-bed reactor. The stability of Cu-Ce/AC catalyst under different pH conditions was studied. This study combines XRD, BET, FT-IR, ICP-OES and XPS characterization techniques to study the main reasons for the deactivation of Cu-Ce/AC catalysts. The reaction mechanism of Cu-Ce/AC catalytic wet air oxidation degradation of phenol was clarified. The result indicates that although phenol was completely converted in the CWAO process, the acidic intermediate product produced were difficult to completely degraded. Therefore, the pH of the solution gradually decreased. In acidic environment, the interaction between active component Cu and carbon carrier is weak, resulting in a large amount of metal leaching into the solution. As a result, the COD conversion gradually decreases. The alkaline environment can effectively slow down the leaching of catalyst Cu while maintaining its high catalytic activity . In addition, the incompletely degraded intermediate products are easy to accumulate and deposit on the Cu-Ce/AC surface, block the micropores and cover the surface-active sites, which reduces the catalyst activity. The study also found that there is a redox cycle between Cu + , Cu 2+ Ce 3+ and Ce 4+ during phenol degradation, which enables Cu and Ce to form a strong interaction. The redox cycle can also promote the formation of oxygen vacancy (h + ), O 2 − ·, and HO·, making the degradation of phenol more thorough. At the same time, the mutual conversion between metal lattice oxygen and surface chemisorbed oxygen can generate high concentration of oxygen defect sites, which can improve the oxygen storage capacity of Cu-Ce/AC. These oxygen vacancies also provide more reactive sites to further promote adsorption and catalytic oxidation degradation of phenol and intermediate products.
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Water
·
2022
·Vol. 14
·期 12
·1864
·
IF 3.53
Shanli Wang,Lu Zhang,Mingyan Zhang,Licong Xu,Qian Hu,Tao Yang,Kaili Tu,Minghua Wu,Deyou Yu
Metal–organic frameworks (MOFs) featuring porous structures and large specific surface areas have shown great potential in removing organic pollutants from wastewater via adsorption processes. Although the particle size of MOFs determines the adsorption performance (something known as the size-dependent effect), engineering it into desirable dimensions for enhancing the adsorption performance is a great challenge. Here, we develop a practical and facile approach to regulate the particle size of copper benzene-1,3,5-tricarboxylate (Cu-BTC) adsorbents with high tunability by screening the functional modulator of various surfactants adding in hydrothermal synthesis procedure. The effect of surfactant type and concentration on the particle size of Cu-BTC was systematically investigated. The results show that the nonionic surfactant polyvinylpyrrolidone (PVP) demonstrated the greatest ability to control the particle size of Cu-BTC among other counterparts (e.g., N, N, N-trimethyl-1-dodecanaminium bromide (DTAB), polyethylene glycol (PEG1000), sodium dodecyl sulfate (SDS), sodium dodecyl benzene sulfonate (SDBS) and hexadecyl trimethyl ammonium bromide (CTAB)). By increasing the PVP concentration to 0.14 mmol L−1, the average particle size of Cu-BTC could be correspondingly reduced by more than ten times, reaching to a comparative smaller value of 2.4 μm as compared with the reported counterparts. In addition, the PVP allowed a large increase of the surface area of Cu-BTC according to porosity analysis, resulting in a great enhancement of methylene blue (MB) adsorption. The PVP-modulated Cu-BTC showed fast adsorption kinetics for MB removal accompanied with a maximum adsorption capacity of 169.2 mg g−1, which was considerably competitive with most of the analogs reported. Therefore, our study may inspire concepts for engineering the particle size of Cu-BTCs with improved properties for more practical applications.Keywords:Cu-BTC;particle size;adsorption;surfactant;modulator
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RSC Advances
·
2022
·Vol. 12
·期 26
·16688-16695
·
IF 4.036
Gengqi Xing,Cheng Wang,Ke Liu,Bin Luo,Peichen Hou,Xiaodong Wang,Hongtu Dong,Jianshu Wang,Aixue Li
Methyl jasmonate (MeJA) is an important phytohormone which can regulate plant growth and stress tolerance. It is very necessary to develop sensitive and accurate detection methods for MeJA. In this work, a probe-free electrochemical immunosensor for MeJA detection was developed based on a Cu-MOF–carboxylated graphene oxide (COOH-GO) platform. The Cu2+ in the Cu-MOFs was used to provide redox signals, which avoids the application of an external redox probe in the electrolyte solutions as conventional immunosensors. COOH-GO was used to improve the structural stability and provide more sites for binding MeJA antibodies. The linear range of the MeJA immunosensor is from 10 pM to 100 μM, which can cover the whole concentration range of MeJA in most plants. And its detection limit is very low (0.35 pM), and it can detect very low concentrations of MeJA. This immunosensor is simple, low cost, and does not need redox probe solutions for measurements. It shows remarkable potential for on-site application in precision agriculture.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Hongai Zheng,Yao Zhou,Derui Wang,Meilin Zhu,Xin Sun,Shuangyan Jiang,Yankun Fan,Daquan Zhang,Lizhi Zhang
Catalytic membrane reactors (CMR) based on the sulfate-based advanced oxidation processes (SR-AOPs) have exhibited fantastic applications prospects in water treatment. We synthesized Cu-MOF-74 by an environmentally friendly and facile method, then used it as PVDF (polyvinylidene fluoride) membrane surface modification layer. The results presented that Cu-MOF-74 can significantly improve anti-fouling ability of PVDF membrane (60.9% and 64.1% anti-adsorption of dye and protein). The modified membranes exhibited relatively low flux loss. Simultaneously the modified membrane catalyzed peroxymonosulfate (PMS) to achieve 97.1% degradation efficiency of Rhodamine B (RhB) within 60 min and 90.2% dye penetration recovery within 30 min. Cu-MOF-74 exhibited greater catalytic activity than homogeneous Cu (II) and showed a wide range of pH adaptation. Finally, XPS and ESR proved that it was the redox of Cu (II)/Cu (I) in the Cu-MOF-74 structure making PMS mainly produce SO 4 - • and •OH to oxidize pollutant molecules. The modus proposed in this study may provide a more promising strategy for the preparation of high-efficiency catalytic membranes and their practical applications in wastewater treatment processes .
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Frontiers in Chemistry
·
2022
·
IF 5.545
Jia Hongyan,Lv Qing,Xia Qineng,Hu Wanpeng,Wang Yanqin
Efficient conversion of biomass-derived 5-hydroxymethylfurfural (HMF) to renewable fuels such as 2,5-dimethylfuran (DMF) and 2,5-dimethyltetrahydrofuran (DMTHF) is of significance for sustainable energy supply. For efficient catalyst design, it is important to understand the catalytic behavior and clarify the influence of physico-chemical properties of catalyst on reaction performance. Herein, to study the structure-activity relationships of monometallic Cu catalysts for HMF hydrogenolysis, a series of Cu/SiO2 catalysts with different physico-chemical properties were prepared and compared for their catalytic performance in HMF hydrogenolysis. It was found that Cu/SiO2-HT-8.5 catalyst prepared by hydrothermal method showed excellent activity in HMF hydrohydrolysis reaction. Under the optimal reaction condition, the total yield of liquid fuels reaches 91.6% with 57.1% yield of DMF and 34.5% yield of DMTHF in THF solvent. Characterizations such as XRD, H2-TPR, N2-adsorption/desorption, TEM and XPS revealed that the Cu particles in the Cu/SiO2-HT-8.5 catalyst have uniform size and high dispersion. The Cu species and the SiO2 support have relatively weak interaction and are easy to be reduced to Cu0, which makes it show excellent activity in the hydrogenolysis of HMF.
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Advanced Therapeutics
·
2022
·Vol. 5
·期 7
·2200043
·
IF 5.003
Ying Yang,Min Li,Bixia Zhou,Xulei Jiang,Dou Zhang,Hang Luo,Shaorong Lei
Large-scale bone defects caused by traumatic injury or tumor resection, are accompanied by relatively high bacterial infection rates. Relevant clinical therapy encounters challenges of infection recurrence, poor vascularization, and bone destruction. Engineered substitutes endowed with multiple functions of bacterial eradication, osteoconductivity, and angiogenesis are urgently needed to address these challenges. Herein, graphene oxide/copper (GO/Cu) nanocomposite-decorated polylactide- co -glycolide (PLGA)/β-tricalcium phosphate (TCP) (P/T/GO/Cu) scaffolds are fabricated using 3D printing technology. A comprehensive evaluation of material characteristics and biological activities of these scaffolds is conducted and compared. This novel bone substitute has unique surface characteristics, and the incorporation of GO/Cu nanocomposites into the scaffolds exhibits improved antimicrobial and osteogenic potential and displays acceptable cytocompatibility. A subcutaneous implantation model in rats confirms the effective inhibition of abscess formation and inflammatory reactions, satisfactory neovascularization and tissue integration, and good biosafety of the implanted P/T/GO/Cu scaffolds. Eventually, a bacteria-contaminated bone defect model is established in rabbits and significantly better new cancellous bone formation featuring collagen or osteoid deposition is clearly found in the defect regions implanted with P/T/GO/Cu scaffolds. Thus, this novel bone substitute with excellent bacterial inhibition, osteogenesis, and angiogenesis capabilities represents a promising strategy to satisfy the multiple demands for the repair of bacteria-contaminated bone defects.
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ACS Nano
·
2022
·
IF 18.027
Nannan Meng,Xiaomin Ma,Changhong Wang,Yuting Wang,Rong Yang,Jiang Shao,Yanmei Huang,Yue Xu,Bin Zhang,Yifu Yu
Urea electrosynthesis provides an intriguing strategy to improve upon the conventional urea manufacturing technique, which is associated with high energy requirements and environmental pollution. However, the electrochemical coupling of NO3– and CO2 in H2O to prepare urea under ambient conditions is still a major challenge. Herein, self-supported core–shell Cu@Zn nanowires are constructed through an electroreduction method and exhibit superior performance toward urea electrosynthesis via CO2 and NO3– contaminants as feedstocks. Both 1H NMR spectra and liquid chromatography identify urea production. The optimized urea yield rate and Faradaic efficiency over Cu@Zn can reach 7.29 μmol cm–2 h–1 and 9.28% at −1.02 V vs RHE, respectively. The reaction pathway is revealed based on the intermediates detected through in situ attenuated total reflection Fourier transform infrared spectroscopy and online differential electrochemical mass spectrometry. The combined results of theoretical calculations and experiments prove that the electron transfer from the Zn shell to the Cu core can not only facilitate the formation of *CO and *NH2 intermediates but also promote the coupling of these intermediates to form C–N bonds, leading to a high faradaic efficiency and yield of the urea product.
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