GREEN CHEMISTRY
·
2023
·Vol. 25
·期 21
·8645-8651
·
IF 9.8
Jianyue Yan,Jiawen Li,Peng Liu,Hao Huang,Wenbo Song
Electrocatalytic reduction of nitrate represents a carbon-neutral approach to managing wastewater remediation while offering an innovative route for high-value green ammonia synthesis. However, nitrite byproduct is inevitably generated in the electrochemical process, which is more toxic to human beings and limits the conversion efficiency of nitrate to ammonia. Herein, a bimetallic metal–organic framework NixCu(3−x)(HITP)2 (HITP = 2,3,6,7,10,11-hexaiminotriphenylene) is proposed as both a cascade catalyst to eliminate the nitrite and a mechanism platform for the study of the cascade process for nitrate reduction. The bimetallic NixCu(3−x)(HITP)2 platform shows that the Cu sites work as the active sites responsible for the conversion of nitrate to nitrite (NO3− + 2 e− → NO2−). The byproduct NO2− has a tendency to adsorb at Ni sites and further convert to NH3 (NO2− + 6 e− → NH3). By integrating Cu and Ni active centers, the bimetallic MOF strategy synergizes the distinct reaction pathways on heterogeneous metal centers. As a result, compared with monometallic Cu3(HITP)2, the optimal Ni1.5Cu1.5(HITP)2 achieved an outstanding NH3 yield of 130.93 μmol h−1 cm−2 with dramatically enhanced NH3 selectivity. This research elucidates the correlation between structure and activity in bimetallic active sites and cascade catalysis, which offers a high-efficiency nitrate-to-ammonia reduction.
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高影响因子
IONICS
·
2023
·Vol. 29
·期 12
·5491-5503
·
IF 2.8
Ren Shufang,Cao Li,Liu Xiaohang,Cui Wangyong,Lv Rui,Guo Tong,Wang Qingtao,Zheng Zhixiang
The detection of norfloxacin (NOR) is crucial because the overdoes and accumulation may result in residues in environment in animal-derived foods, which can destroy ecology and cause disease for people. A molecularly imprinted electrochemical sensor based on g-C 3 N 4 /Cu-MOF was constructed for the selective detection of norfloxacin in this paper. The g-C 3 N 4 /Cu-MOF was synthesized by melamine pyrolysis and solvothermal method followed by ultrasonic mixing. After drop casting g-C 3 N 4 /Cu-MOF on glassy carbon electrode, the molecularly imprinted film was synthesized by electropolymerization. The composite was analyzed by powder X-ray diffractometer, field emission scanning and transmission electron microscope, and Fourier transform infrared spectroscopy. The electrochemical properties of the sensor were characterized by cyclic voltammetry, electrochemical impedance spectroscopy, and pulse voltammetry. The results show that the composite of g-C 3 N 4 /Cu-MOF efficiently decreased the charge transfer resistance of electrode and improved the electron transfer kinetic between analyte and electrode with the improved current response and increased active area. After optimizing conditions of the ratio of functional monomers to template molecules, the number of polymerization cycles, accumulation time, electrolyte pH, and the sensor exhibits excellent response toward NOR with the linearity range of 0.02–0.1 μmol/L and 1–120 μmol/L and the limit of detection of 6.67 nmol/L. Moreover, it shows good selectivity, anti-interference, and reproducibility properties. In the real sample detection of pharmaceutical formulations, serum and milk, the sensor shows an acceptable recovery rate and standard deviation.
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ChemCatChem
·
2023
·Vol. 15
·期 22
·e202300967
·
IF 4.5
Ting Li,Yuhao Tian,Xiaoli Yan,Weijie Cai
Graphical CO 2 Reforming : Transition metal-based SiO 2 -Ni@CeO 2 catalyst with typical core@shell structure exhibited the better activity/stability in CO 2 reforming with ethanol reaction compared to SiO 2 -Cu@CeO 2 sample. It is of great significance to design the high-performance catalysts with good anti-sintering and coke-resistance properties which can efficiently convert undesirable greenhouse gas CO 2 with bio-ethanol into high value-added syngas. To be addressed this issue, a series of SiO 2 -M@CeO 2 (M: Cu, Ni) catalysts with typical core@shell structure were prepared via a strong electrostatic adsorption technique. Interestingly, Ni-based catalyst exhibited the higher activity towards ethanol dry reforming at the relatively low temperature. Meanwhile, SiO 2 -Ni@CeO 2 catalyst presented good stability after a 50 h tests while a serious deactivation occurred for SiO 2 -Cu@CeO 2 within 20 h reaction due to heavy carbon deposition and reactor blockage. Herein, the higher catalytic performance of SiO 2 -Ni@CeO 2 catalyst compared to SiO 2 -Cu@CeO 2 sample was attributed to the combination effect of its mesoporous structure, higher Ni dispersion as well as stronger Ni-Ce interaction as depicted by BET, TEM, XPS, H 2 -TPR and XRD findings. This work might provide meaningful information to other reforming processes involving coke formation and active metal sintering problems.
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LAB ON A CHIP
·
2023
·Vol. 23
·期 20
·4493-4503
·
IF 6.1
Wei Liu,Yongan Feng,Yapeng Yao,Zihang Liang,Fei Xiao,Zhongliang Ma
Integrating energetic materials with microelectromechanical systems (MEMS) to achieve miniaturized integrated smart energetic microchips has broad application prospects in miniaturized aerospace systems and civil explosive systems. In this work, MEMS compatible [Cu(BODN)·5H2O]n arrays and [Cu(BODN)·5H2O]n@nano-Al composite energetic films were successfully fabricated on copper substrates by the in situ reaction method and drop-coating method. Single crystal X-ray diffraction, powder X-ray diffraction, scanning electron microscopy, infrared spectroscopy, differential thermal analyses, and pulsed laser ignition were employed to characterize the prepared samples. The results show that [Cu(BODN)·5H2O]n arrays formed by the coordination reaction between the Cu(OH)2 template and the BODN ligand exhibit a porous supramolecular structure with excellent thermal and energy properties. Their morphology and composition on a copper substrate can be effectively regulated by adjusting the reaction time and solution concentration. In addition, adjustable energetic properties of [Cu(BODN)·5H2O]n@nano-Al composite films can be achieved after the encapsulation of nano-Al. Their heat release, flame height and ignition duration can reach as much as 1987.5 J g−1, 13.2 mm, and 5900 μs, respectively, indicating that [Cu(BODN)·5H2O]n@nano-Al can be used as an excellent pyrotechnic agent in MEMS ignition chips. Overall, this work provides a reference for the integration and application of energetic materials in MEMS systems.
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高影响因子
RENEWABLE ENERGY
·
2023
·
IF 8.7
Bo Cai,Rui Kang,Junfeng Feng,Thomas L. Eberhardt,Zhongqing Ma,Qingge Zhu,Hui Pan
The catalytic transfer hydrogenation (CTH) of levulinate ester to γ-valerolactone is one of the important reactions for production of renewable fuels from biomass. An efficient and robust bimetallic Cu–Ru catalyst were developed for the hydrogenation of biomass-derived ethyl levulinate to γ-valerolactone. A series of bimetallic catalysts were prepared and characterized in detail. Subsequently, the as-prepared catalysts were evaluated in the hydrogenation system of ethyl levulinate. The results showed that Cu–Ru/ZrO 2 –SO 3 –SiO 2 -450 catalyst provided 100 % GVL yield in 12 h at 180 °C. Meanwhile, it also exhibited high catalytic hydrogenation activity for the various biomass-derived carbonyl compounds. The structure-reactivity relationship of catalysts was investigated in detail, and the results show the interaction between support and metal sites played an important role in the hydrogenation activity. The sulfur species could tune the electronic states of metallic sites to gain optimal activity. Besides, the Cu–Ru/ZrO 2 –SO 3 –SiO 2 -450 catalyst performed excellent recyclability in five reaction runs without an obvious loss of activity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yanming Feng,Xinyue Lv,Xi Ran,Caifeng Jia,Lujie Qin,Maoshen Chen,Ruijuan Qi,Hui Peng,Hechun Lin
Cuprous oxide (Cu 2 O) and cupric oxide (CuO) are widely available and low cost raw materials. Their applications as precursors for wet chemical synthesis of metallic Cu materials are greatly limited due to their insoluble in water and most organic solvents . In this work, copper superfine particles (Cu SPs) are synthesized using Cu 2 O and CuO as precursors via a heating process in monoethanoamine (MEA). Due to the strong coordinating character, Cu 2 O and CuO can be partially dissolved in MEA. The dissolved copper source is reduced by MEA at elevated temperature with the drastically releasing of NH 3 . As the dissolved copper source is reduced, more oxide will be dissolved and finally leads to the full reduction of Cu 2 O and CuO to produce the Cu SPs. The advantage of this synthesis method is that MEA acts as both the solvent and the reducing agent. The antimicrobial properties are investigated to find that the obtained Cu SPs depress the growth of Escherichia coli (E. coli) and Staphylococcus aureus (St. aureus) efficiently. More interesting, the composites produced via curing Cu 2 O and CuO with a small amount of MEA also exhibit excellent antimicrobial activity, indicating the MEA curing method is high-efficiency. The synthesis is low cost, high-efficiency, high atom-economy and up-scale synthesizing easily, which will benefit the wide applications of Cu SPs.
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高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2021
·Vol. 133
·期 1
·55-71
·
IF 2.081
Yu Jun,Liang Jiezhen,Chen Xiaopeng,Wang Linlin,Wei Xiaojie,Qin Yanmin,Li Youqi,Ling Youkang
The reaction pathway and kinetics of cellulose hydrogenolysis to ethylene glycol (EG) catalyzed by nickel and tungsten combined with copper supported on magnesium aluminum spinel (NiO x -WO y -Cu/MgAl 2 O 4 ) were studied. Cellulose was hydrolyzed to glucose, which followed either the retro-aldol condensation to glycolaldehyde and erythrose or isomerized to fructose followed by retro-aldol reaction to dihydroxyacetone and glyceraldehydes. The derived glucose can also be hydrogenated to sorbitol. The intermediate products were subsequently converted to EG, erythritol, glycerol and 1,2-propanediol. The cellulose conversion, yields of EG and C 2,3 polyols were achieved 100, 53.1 and 62.7%, respectively. The simplified kinetic models were proposed and validated with the experimental results, indicating that the simpler first-order model could perfectly describe the hydrogenolysis of cellulose in the catalytic system. Hydrolysis of cellulose was demonstrated as the rate determining step independent of the reaction pathway, and high temperatures were favorable to the hydrolysis of cellulose to glucose. Activation energies results showed that high temperatures were favorable to the hydrolysis of cellulose to glucose.
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ANALYST
·
2021
·Vol. 146
·期 19
·5951-5961
·
IF 4.616
Hong Cui,Shuaishuai Cui,Siyuan Zhang,Qiuju Tian,Yunfeng Liu,Ping Zhang,Mingxiu Wang,Jialing Zhang,Xiangjun Li
The stability, repeatability and sensitivity of an electrochemical biosensor material are closely connected with the dispersibility of metal organic frameworks (MOFs) in aqueous media. Herein, a nanocomposite based on Cu–MOF/hemin, which is not only highly water-soluble but also simple and efficient in synthesis, was used for the construction of a non-enzymatic sensor to detect hydrogen peroxide (H2O2). The Cu–MOF/hemin was characterized via scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy dispersive X-ray spectroscopy (EDS)-mapping, X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and thermal gravimetric analysis (TGA), which indicate that hemin and the Cu–MOF were successfully combined. As a H2O2 electrochemical biomimetic enzyme, the Cu–MOF/hemin exhibited excellent electrocatalytic performance, which was confirmed by the electrochemical experiments and chromogenic reactions, and the possible mechanism of the reactions has been deduced. The electrochemical sensor based on the biomimetic enzyme exhibited an extended linear detection range from 0.01–5.0 mM (R = 0.998), low detection limit of 4.14 μM, and high selectivity and stability under the optimized conditions. More importantly, the practical application ability of the sensor was verified by the test of H2O2 in human serum samples and it could be used for the real-time detection of H2O2 released from living cells with satisfactory results. Therefore, this novel nanocomposite has certain potential in preparing electrochemical sensing platforms for nonenzymatic biosensing and provides a new method for clinical diagnosis and real-time monitoring.
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高影响因子
TALANTA
·
2021
·
IF 6.057
Hui Huang,Meini Li,Mingwei Hao,Liangli (Lucy) Yu,Yongxin Li
A selective and sensitive colorimetric strategy for sulfide analysis was developed using GMP-Cu nanozymes with a laccase-like activity. This research discovered for the first time that sulfide could significantly enhance the catalytic activity of the GMP-Cu nanozymes by about 3.5 folds. The enhanced laccase activities duo to two reasons. First, Cu 2+ in GMP-Cu nanozymes was reduced to Cu + . The other reason was the formation of Cu–S bond which was beneficial to accelerate the electron transfer rate to improve catalytic activity. Therefore, this method showed an excellent selectivity for sulfide. And it had a linear relationship in the sulfide concentration range of 0–220 μmol/L with a detection limit of 0.67 μmol/L. Furthermore, the proposed method was successfully applied to examine sulfide in the food systems. This new method may be used in sulfide detection to improve food quality and safety.
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NANOTECHNOLOGY
·
2020
·Vol. 32
·期 8
·085101
·
IF 3.551
Yang Sheng,Shuai Li,Yixin Sun,Rong Zhang,Xinyu Zhao,Mei Chee Tan
CuInSe2 quantum dots (QDs) are one of the most important Cd-free fluorescent probes; they usually exhibited low fluorescence intensity, suggesting that a considerable amount of absorbed photon energy was lost as heat. In this study we aimed to improve the fluorescence intensity of CuInSe2 QDs and investigate their photoacoustic (PA) signal resulting from the heat dissipation, which was previously rarely reported. Cu–In–Zn–Se/ZnSe QDs were synthesized by adopting two strategies of Zn doping and ZnSe shell growth. It was found that there was an upper limit for Zn concentration beyond which the fluorescence intensity began to decrease. In addition, a blue shift of the emission peak of Cu–In–Zn–Se/ZnSe QDs was observed at high concentrations of ZnSe precursor due to the diffusion of excessive Zn. To prepare the dual-modal fluorescence and PA imaging probe, poly(maleic anhydride-alt-1-octadecene) (PMAO) modified with polyethylene glycol (PEG) was coated on the QDs, which led to a slight reduction in fluorescence. Cellular labeling on HeLa cells was performed to demonstrate the utility of these probes for fluorescence imaging. We further studied the in vitro PA imaging capabilities of the Cu–In–Zn–Se/ZnSe/PMAO-g-PEG nanoparticles, which showed a distinct PA signal beyond 1.0 mg ml−1. The current work demonstrated that a moderate amount of Zn doping is necessary for enhancing fluorescence and there is a limit beyond which the fluorescence will be diminished. We also demonstrated the proof of concept that Cu–In–Zn–Se/ZnSe QDs are able to serve as a potential PA imaging contrast agent.
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高影响因子
RSC Advances
·
2020
·Vol. 10
·期 58
·35374-35380
·
IF 3.119
Baozhu Zhang,Chunying Wei
A highly sensitive thrombin aptasensor was constructed based on the alteration of the aptamer conformation induced by the target recognition and the turn-on fluorescence due to the proximity of two darkish DNA-templated copper/silver nanoclusters (DNA-Cu/Ag NCs). Two DNA templates were designed as the functional structures consisting of the Cu/Ag NC-nucleation segment located at two termini or one terminus and the aptamer segment in the middle of a DNA template. Two darkish DNA-Cu/Ag NCs came close to each other when the aptamer combined with the target due to the conformational alteration of the aptamer structure, resulting in an increased fluorescence signal readout. Thrombin was sensitively determined as low as 1.6 nM in the range of 1.6–8.0 nM with a high selectivity. Finally, this sensor succeeded in detecting thrombin in a real fetal bovine serum.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Xue-Qi Zhang,Rong-Fang Shen,Xiao-Jing Guo,Xi Yan,Yan Chen,Jiang-Tao Hu,Wan-zhong Lang
Herein, a convenient and environment-friendly grafting and reduction strategy was used to anchor bimetallic Ag-Cu nanoparticles on polypropylene (PP) fabrics. The as-prepared samples were characterized by various techniques including FE-SEM, XRD, EDX, XPS and FT-IR. The as-prepared sample exhibits excellent activity on the catalytic reduction of highly concentrated 4-NP, and the synergistic effect between Ag and Cu nanoparticles was proved. The entire catalytic reduction was generally considered to obey pseudo-order kinetics, affording high conversion even after 15 successive recycles. These results showed that the PP based composite with Ag-Cu nanoparticles effectively provided superb catalytic efficiency and stability in 4-nitrophenol reduction, and the PP based composites were suitable in practical applications for the treatment of diverse waste water.
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危险品化学品经营许可证（带存储）