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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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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Journal of Physical Chemistry C
·
2022
·
IF 4.177
Yun Ling,Ya-ru Chu,Feng Gao,Qing-yun Feng,Hui-qi Xie,Yong Shao,Qing-xiang Wang
The unique chemical and physical properties of metal–organic frameworks (MOFs) endow them with promising applications in the electrochemical sensing field. Herein, a novel label-free electrochemical sensing strategy for cardiac troponin I (cTnI) has been constructed on the basis of immunoaffinity-induced depression of the electrochemical signal of Cu-MOF-74. The electrochemical assay shows that the immunoaffinity reaction between cTnI and anti-cTnI on the electrode surface can effectively inhibit the electrochemical signal of electrode-confined Cu-MOF-74, suggesting that the Cu-MOF-74-based interface may find application in the label-free analysis of cTnI. Thus, Cu-MOF-74 acts as a bifunctional material in this strategy, namely, the immobilization matrix of probe molecules and the signal source of the sensing analysis. In addition, the reason for the electrochemical signal depression of Cu-MOF-74 induced by immunoaffinity reaction is attributed to the increase in the insulation layer and the blocking of the electrolyte diffusion from the bulk solution to the electrode surface. In this strategy, the analytical range of cTnI is from 0.01 pg mL–1 to 1.0 ng mL–1 and the detection limit is 4.5 fg mL–1. The Cu-MOF-74-based sensing interface is also reliable for cTnI analysis in real serum samples, showing that the biosensor has promising application in point-of-care testing (POCT) of myocardial injury-related diseases.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 4
·919-927
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IF 2.726
Zhu Junlun,Cui Qian,Wen Wei,Zhang Xiuhua,Wang Shengfu
Although great progress has been made in the advancement of nanozymes, most of the studies focus on mimicking peroxidase, oxidase, and catalase, while relatively few studies are used to mimic laccase. However, the use of nanomaterials to mimic laccase activity will have great potential in environmental and industrial catalysis. Herein, Cu/CuO-graphene foam with laccase-like activity was designed for the identification of phenolic compounds and the detection of epinephrine. In a typical experiment, the formation mechanism of Cu/CuO-graphene foam was investigated during the pyrolysis process by thermogravimetric-mass spectrometry. As a laccase mimic, Cu/CuO-graphene foam exhibited excellent catalytic activity with a Michaelis-Menten constant and a maximum initial velocity of 0.17 mmol/L and 0.012 µmol·L −1 ·s −1 , respectively. Based on this principle, Cu/CuO-graphene foam nanozyme could differentially catalyze phenolic compounds and 4-aminoantipyrine for simultaneous identification of phenolic compounds. Furthermore, a colorimetric sensing platform was fabricated for the quantitative determination of epinephrine, showing linear responses to epinephrine in the range of 3 µg/mL to 20 µg/mL with the detection limit of 0.2 µg/mL. The proposed Cu/CuO-graphene foam nanozyme could be applied for the identification of phenolic compounds and the detection of epinephrine, showing great potential applications for environmental monitoring, biomedical sensing, and food detection fields.
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FUEL
·
2022
·
IF 8.035
Chengyan Wen,Ke Jin,Luying Lu,Qian Jiang,Jingcheng Wu,Xiuzheng Zhuang,Xinghua Zhang,Lungang Chen,Chenguang Wang,Longlong Ma
Direct conversion of syngas into aromatics (STA) on the tandem catalyst containing Fischer-Tropsch (F-T) synthesis catalysts and acid zeolites, especially Fe-based catalysts and ZSM-5, has been attracting significant attention due to the higher cost efficiency. Even though promoters have frequently been added into the Fe-based part to improve the performance of STA reaction, its motivating mechanism is still unclear in the tandem catalyst system. Herein, the influence of the Cu promoter was evaluated for the catalytic activity of Fe-based/zeolite tandem catalysts in the STA process. Moreover, the working mechanism of the Cu promoter had been systematically investigated by adding different copper amounts and deliberately designed experiments. It was demonstrated that the addition of copper could improve aromatic selectivity because the Cu promoter could facilitate CO to participate in the conversion of olefins into aromatics over the tandem catalyst. In addition, the Cu promoter doped into the Fe-based catalyst drastically suppressed methane formation and enhanced the stability of the catalyst in the STA reaction. These findings provide insights into the effect of the Cu promoter on producing aromatics from syngas over the Fe-based/zeolite tandem catalyst system.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-13
·
IF 17.694
Yang Baiyu,Chen Ling,Xue Songlin,Sun Hao,Feng Kun,Chen Yufeng,Zhang Xiang,Xiao Long,Qin Yongze,Zhong Jun,Deng Zhao,Jiao Yan,Peng Yang
Electrocatalytic reduction of CO 2 into alcohols of high economic value offers a promising route to realize resourceful CO 2 utilization. In this study, we choose three model bicentric copper complexes based on the expanded and fluorinated porphyrin structure, but different spatial and coordination geometry, to unravel their structure-property-performance correlation in catalyzing electrochemical CO 2 reduction reactions. We show that the complexes with higher intramolecular tension and coordination asymmetry manifests a lower electrochemical stability and thus more active Cu centers, which can be reduced during electrolysis to form Cu clusters accompanied by partially-reduced or fragmented ligands. We demonstrate the hybrid structure of Cu cluster and partially reduced O-containing hexaphyrin ligand is highly potent in converting CO 2 into alcohols, up to 32.5% ethanol and 18.3% n- propanol in Faradaic efficiencies that have been rarely reported. More importantly, we uncover an interplay between the inorganic and organic phases to synergistically produce alcohols, of which the intermediates are stabilized by a confined space to afford extra O-Cu bonding. This study underlines the exploitation of structure-dependent electrochemical property to steer the CO 2 reduction pathway, as well as a potential generic tactic to target alcohol synthesis by constructing organic/inorganic Cu hybrids.
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Journal of Environmental Sciences
·
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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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 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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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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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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