CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Peng Liu,Jianyue Yan,Hao Huang,Wenbo Song
Electrochemical reduction of nitrate to ammonia is an eco-friendly strategy to remove the nitrate pollution in waste effluents. Developing new-type electrocatalysts with high activity for NO 3 RR has attracted worldwide attention. Owing to the numerous active single-metal sites, electric conductivity and ordered in-plane porous structure, conductive metal–organic frameworks (cMOFs) are promising alternative to construct the next-generation NO 3 RR electrocatalysts. In this work, a bimetallic cMOF (Cu x Co y HHTP) is proposed for efficient NO 3 – electroreduction to ammonia and the synergy effect between different types of single-metal sites is also revealed. As the result, the optimal Cu 1 Co 1 HHTP exhibits an outstanding electrocatalytic activity with a high NH 3 yield rate of 299.9 μmol h −1 cm −2 and a large Faradic efficiency of 96.4%. Both theoretical and experimental results reveal that the Co sites can affect the electron structure of Cu sites in Cu 1 Co 1 HHTP slab and decrease the ΔG of potential determining step in NO 3 RR process. Moreover, the Co sites bring a higher selectivity to Cu active sites for reducing *NO 2 to *NO, rather than the desorption of NO 2 – . The bimetallic c-MOFs strategy will innovate the design concept of next-generation catalyst, paving the way to investigate catalytic mechanism of single-metal-atom and open up their application prospects.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Xi Peng,Xing Hu,Kai Liu,Deming Gong,Guowen Zhang
Inhibition of advanced glycation end products (AGEs) formed in protein glycosylation is crucial for minimizing diabetic complications. Herein, the anti-glycation potential of hesperetin-Cu (II) complex was investigated. Hesperetin-Cu (II) complex strongly inhibited three stages glycosylation products in bovine serum albumin (BSA)-fructose model, especially for the inhibition of AGEs (88.45%), which was stronger than hesperetin (51.76%) and aminoguanidine (22.89%). Meanwhile, hesperetin-Cu (II) complex decreased the levels of BSA carbonylation and oxidation products. 182.50 µg/mL of hesperetin-Cu (II) complex inhibited 66.71% β-crosslinking structures of BSA, and scavenged 59.80% superoxide anions and 79.76% hydroxyl radicals. Moreover, after incubating with methylglyoxal for 24 h, hesperetin-Cu (II) complex removed 85.70% methylglyoxal. The mechanisms of protein antiglycation by hesperetin-Cu (II) complex may be through protecting structure, trapping methylglyoxal, scavenging free radicals and interacting with BSA. This study may contribute to the development of hesperetin-Cu (II) complex as a functional food additive against protein glycation.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Yinghong Zhu,Guanxuan Guo,Jianping Zhang,Qi Zhang,Ke Chen,Minling Zhou,Youqun Chu
Copper nanoparticles (Cu NPs) modified zinc electrode (Cu-Zn/Cu-foam) is successfully prepared via cathodic electrodeposition followed by a galvanic-exchange procedure and characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), cyclic voltammetry (CV), Tafel curve and galvanostatic electrolysis. With the reconstruction of Zn through the formation of Cu NPs on the surface, the corrosion current and active surface area are increased, and the activity on the electrochemical reduction of tetrabromobisphenol A (TBBPA) is activated. The TBBPA (10 mmol/L) is almost degraded within 1 h, and the yield of the complete debromination product bisphenol A (BPA) reaches 92 % in 3 h. Furthermore, the surface of used Cu-Zn/Cu-foam electrode become more uniform and CuZn 5 is formed, which enabled the stable electro-catalytic activity on the electro-reduction of TBBPA even after ten cycles. Then the degradation mechanism is proposed. The micro galvanic reconstruction of Zn offers a promising strategy for the removal of TBBPA in aquatic environment.
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ACS Catalysis
·
2023
·
IF 12.9
Nana Gong,Tao Zhang,Minghui Tan,Liyan Wang,Jiaqian Yang,Li Tan,Guohui Yang,Peng Wu,Yingquan Wu,Yisheng Tan
CO hydrogenation to isobutyl alcohol is a promising route for CO transformation to high value-added products. However, the formation mechanism of isobutyl alcohol is complex, and its synthesis requires complex catalysts and harsh reaction conditions, which hinders the identification of active sites. Herein, we efficiently synthesized isobutyl alcohol under mild conditions over a simple Cu–ZrO2 catalyst by decreasing the Cu loading. The space–time yield (STY) of isobutyl alcohol using an optimal CZ-0.11 catalyst was as high as 61.3 g·Lcat–1·h–1 with a CO conversion of 19.2%, far surpassing the STY of the state-of-the-art isobutyl alcohol synthesis (44.6 g·Lcat–1·h–1) under harsh conditions. Decreasing the Cu loading increased the distribution of smaller Cu particles and clarified the structure–activity relationship of Cu–Zr interactions for isobutyl alcohol synthesis. The enhanced Cu–Zr interaction led to the formation of more electron-deficient Cu species on the CZ-0.11 catalyst, which enriched the linearly adsorbed CO on Cu, as demonstrated by in situ diffuse reflectance infrared Fourier-transform spectroscopy. Experimental and theoretical results revealed that coupling of the bicarbonate species on ZrO2 with the linearly adsorbed CO species on electron-deficient Cu clusters promoted the formation of C2 intermediates and finally produced isobutyl alcohol through rapid β-addition. These insights into the active sites for CO hydrogenation to isobutyl alcohol may guide further catalyst designs.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Jinxian Feng,Junyan Li,Lulu Qiao,Dong Liu,Pengfei Zhou,Jun Ni,Hui Pan
Zn-based materials are regarded as a family of promising electrocatalysts for electrochemical CO 2 reduction reaction (e-CO 2 RR), especially for the CO 2 -to-CO conversion. However, their electrocatalytic performances should be improved and the conversion mechanism needs to be further studied. In this work, we fabricate Cu-incorporated ZnO (Cu 25 Zn-A) on Zn plate for e-CO 2 RR catalyst by a facile annealing method. We find that Cu 25 Zn-A achieves a high CO Faraday efficiency > 90% with a CO yield rate of 0.49 mmol cm −2 h −1 . The improved catalytic activity on Cu 25 Zn-A is mainly attributed to the Cu steps on the reconstructed surface in the reaction: (1) that weakens the OH - /CO 3 2- adsorption, leading to the anti-poisoning surface by preventing the formation of Zn hydroxide/carbonates; and (2) that enhances the adsorption/activation of reactants and stabilizes the intermediates. Additionally, the density of defects in Zn oxide is increased by the Cu-incorporation, resulting in improved deoxygenation step. Our findings may provide insightful understanding on the mechanism and guide the design of novel electrocatalyst for effective CO 2 reduction.
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CATALYSIS TODAY
·
2023
·
IF 5.3
Hangjie Li,Liang Wang,Feng-Shou Xiao
Cu/ZnO/Al 2 O 3 catalyst has been widely studied in the hydrogenation of CO 2 to methanol, but it still suffers from insufficient catalyst stability and methanol selectivity. Herein, we overcome these issues by introducing the silica promoter to the catalyst, achieving the Cu/ZnO/Al 2 O 3 /SiO 2 (CZAS) catalysts with significantly improved methanol selectivity and catalyst durability. Characterizations of samples showed that the silica species efficiently hindered the sintering of Cu nanoparticles during the catalysis, exhibiting constant performances in the continuous tests. In addition, the silica also electronically modulated the Cu nanoparticles that result in abundant Cu δ+ species in the catalyst, which minimized the methanol decomposition to improve the methanol selectivity, compared with the silica-free Cu/ZnO/Al 2 O 3 catalyst. As a result, the CZAS exhibited CO 2 conversion at 12.6 % and methanol selectivity at 85.1 %, giving a one-pass methanol yield at 10.7 %. The strategy in this work might provide an efficient route for enhancing the current industrial catalysts.
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RSC Advances
·
2019
·Vol. 9
·期 14
·7786-7794
·
IF 3.049
Zhuang Xu,Wenjing Lou,Gaiqing Zhao,Dongdong Zheng,Junying Hao,Xiaobo Wang
Tungsten disulfide–polydopamine–copper (WS2–PDA–Cu) nanocomposites were first prepared by a green and effective biomimetic strategy and then used as a lubricant additive in polyalkylene glycol (PAG). The biomimetic strategy is inspired by the adhesive proteins in mussels. WS2 nanosheets were decorated by uniformly dispersed Cu nanoparticles (Cu NPs). The WS2–PDA–Cu nanocomposites with good dispersion stability, showed better friction reducing and anti-wear properties than WS2, Cu NPs and WS2–Cu dispersed in PAG base oil. The average friction coefficient and wear volume were reduced by 33.56% and 97.95%, respectively, at 150 °C under a load of 100 N for the optimal concentration of 0.9 wt%. The lubrication mechanism was discussed.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Quanfa Zhong,Qintie Lin,Runlin Huang,Hengyi Fu,Xiaofeng Zhang,Haoyu Luo,Rongbo Xiao
A nitrogen and copper codoped biochar (N-Cu/biochar) material was prepared and used to activate persulfate (PS) for tetracycline (TC) degradation. The material was characterized by SEM, FT-IR, XRD and XPS. The results showed that the N-Cu/biochar had a flaky carbon structure with urchin-like copper growing on the carbon surface, a large specific surface area of 352.43 m 2 /g that provided sufficient active sites for catalytic reaction, and abundant functional groups. Quenching experiments and electron paramagnetic resonance (EPR) experiments verified the reaction pathway mechanisms. The main free radical in the system was HO ; another possible mechanism is the nonradical pathway of electron transfer between TC and PS on the surface of the catalyst, and this electron transfer could lead to TC degradation. All the TC was removed within 120 min at a catalyst dosage of 200 mg/L, PS dosage of 0.5 mM, and pH of 7.0. Chloride and bicarbonate ions had little effect on the degradation of TC. HPLC-MS was used to investigate the main degradation intermediates and the possible transformation pathways were proposed. The toxicity of TC and its intermediates were evaluated by bioluminescence inhibition method. The high catalytic efficiency and low consumables of the N-Cu/biochar/PS system could provide a new strategy for the remediation of wastewater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2019
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IF 3.131
Nana He,Lili Li,Panpan Wang,Junhao Zhang,Jiaqi Chen,Jie Zhao
Herein, titanium dioxide/chitosan/poly(lactide-co-caprolactone) (TiO 2 /CS/P(LLA-CL)) composite membranes with highly efficient adsorption of copper ions (Cu(II)) in aqueous solution were developed, through a facile electrospinning method. First, TiO 2 nanoparticles were ultrasonically dispersed in CS/P(LLA-CL) solution to get a uniform suspension. Afterwards, the mixture was applied for electrospinning to generate the smooth and bead-free composite membranes. The high adsorption capability of the composite membranes on Cu(II) was mainly attributed to the combination of TiO 2 nanoparticles, CS/P(LLA-CL) matrix and nanosized membrane. Among those, the TiO 2 /CS/P(LLA-CL) composite membrane with 2% TiO 2 content demonstrated the maximum adsorption capability (˜190.5 mg g −1 ) for Cu(II) from aqueous solution. Their adsorption behaviors were well conformed to pseudo-second-order kinetic model and Langmuir isotherm model. Moreover, FTIR and XPS results confirmed the existed chelation and ion exchange between the membrane and the Cu(II) during adsorption process. Due to its simplicity, effectiveness and stability in water, this type of composite membrane may serve as a promising environmentally-friendly and non-toxic adsorbent for removal of Cu(II) in aqueous.
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2019
·Vol. 20
·期 6
·1469
·
IF 4.183
Xuerong Zhou,Ling Zhao,Jie Luo,Huaqiao Tang,Min Xu,Yanyan Wang,Xiaoyu Yang,Helin Chen,Yinglun Li,Gang Ye,Fei Shi,Cheng Lv,Bo Jing
Research has shown that nano-copper (nano-Cu) can cause damage to the spleen and immune system yet their mechanisms of cytotoxicity are poorly understood. Our aim is to explore the potential immunotoxicity in the spleen of rats after nano-Cu exposure. The results of hematologic parameters, lymphocyte subsets, immunoglobulins, and histopathology indicated that copper obviously changed the immune function of the spleen. The levels of antioxidants (SOD, CAT, GSH-Px), oxidants (iNOS, NO, MDA), and anti-oxidative signalling pathway of Nrf2 (Nrf2 and HO-1) were strongly induced by nano-Cu. The expression of mRNA and protein of pro-/anti-inflammatory (IFN-γ, TNF-α, MIP-1α, MCP-1, MIF, IL-1/-2/-4/-6) cytokines were increased by nano-Cu. The expression of regulatory signal pathways, MAPKs and PI3-K/Akt were activated, which might be involved in the inflammatory responses and immunomodulatory processes of sub-acute nano-Cu exposure. The immune function of the spleen was repressed by nano-Cu induced oxidative stress and inflammation.Keywords:nano-Cu;rats;spleen injury;immune system;oxidative stress
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JOURNAL OF NANOPARTICLE RESEARCH
·
2019
·Vol. 21
·期 2
·1-12
·
IF 2.009
Xia Xiaoxiao,Li Wei,Li Song
Ionic liquids/metal-organic framework composites are recognized as promising adsorbents for CO 2 capture due to the outstanding adsorption performance, whereas their water stability, which is critical for the real application of ILs/MOF composites, has not been taken into consideration. In this work, the water stability of two ILs/Cu-BTC composites, i.e., 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM][BF 4 ]) /Cu-BTC and 1-butyl-3-methylimidazolium hexafluorophosphate ([BMIM][PF 6 ]) /Cu-BTC, were investigated. We found that the loading of ILs does not impose remarkable impacts on the crystalline structure of Cu-BTC upon water exposure; whereas the thermal stability and surface area of Cu-BTC were decreased by the incorporation of ILs, thereby leading to the reduced CO 2 uptake in spite of the enhanced CO 2 heat of adsorption. Furthermore, it was revealed that the decomposition of Cu-BTC occurred within the first hour of water exposure. Nevertheless, the loading of ILs retarded the decomposition of Cu-BTC according to the variations in BET surface area upon water exposure.
Graphical abstract
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2018
·
IF 3.909
Xiaonuo Zhang,Xiaoyan Lin,Yu He,Yan Chen,Xuegang Luo,Ran Shang
Widespread concern had been given raise to the pollution of antibiotics including tetracyclines in water environment in recent years. A novel Cu-immobilized alginate adsorbent had been synthesized successfully through a facile fabrication way called sol-gel method, and its adsorption performance had been investigated for the tetracycline removal at various conditions, including the pH, temperature, the dosage of adsorbent, concentration and contact time. The adsorbent was characterized with SEM, EDX, FT-IR and XPS analyses to confirm its properties before and after adsorption. The equilibrium data was fitted well with the Freundlich isotherm model and the maximum adsorption capacity for tetracycline was 53.26 mg·g −1 at pH 3, 318.15 K, and 90 mg·L −1 tetracycline solution. The pseudo-second-order kinetic and Freundlich isotherm models combining with the correlative analysis implied that the tetracycline adsorption onto the Cu-immobilized alginate adsorbent was administrated by the n-π electron-donor-acceptor interaction (n-π EDA interaction), hydrogen bond and the cation bonding bridge. Moreover, thermodynamic study demonstrated that the nature of tetracycline adsorption was endothermic, feasible and spontaneous. Compared with the other adsorbents, the as-prepared adsorbent had an excellent tetracycline adsorption capacity, and was expected to be widely applied in the adsorption treatment of tetracycline wastewater.
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