LANGMUIR
·
2023
·
IF 3.9
Yang Xiang,Zan Liu,Zhilin Cheng
Herein, we successfully constructed a Cu+-doped PVA-derived mesoporous carbon@diatomite (DE) composite by virtue of N2-suffered carbonization and self-reduction at a high temperature. The structure and composition of C/Cu@DE composite adsorbents were determined by a series of characterizations. The results affirmed that Cu+ species are highly scattered in PVA-derived mesoporous carbon, which covered the DE surface. The effect of carbonization temperature on the structure and composition of the C/Cu@DE composite adsorbents were intensively investigated, indicating that the C/Cu@DE composite at an 800 °C carbonization temperature (C/Cu@DE-800 °C) showed the formation of many Cu+ species and preferable hierarchical pore properties. The adsorption experiments of benzothiophene (BT) indicated that C/Cu@DE-800 °C possessed a better adsorption capacity. The adsorption behavior of BT onto C/Cu@DE-800 °C was investigated by a variety of adsorption times, initial concentrations, and recycle times, of which the largest adsorption capacity for BT attained 34.2 mg/g. Furthermore, the adsorption kinetics, intraparticle diffusion, adsorption isotherms, and adsorption thermodynamics of BT onto C/Cu@DE-800 °C was deeply studied, which contributed to the proposed adsorption mechanism.
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Advanced Energy Materials
·
2023
·Vol. 13
·期 42
·2302692
·
IF 27.8
Qingyu Wang,Yida Zhang,Minxi Lin,Hengwei Wang,Yu Bai,Chengyuan Liu,Junling Lu,Qiquan Luo,Gongming Wang,Hai-Long Jiang,Tao Yao,Xusheng Zheng
Metastable structures are promising candidates for efficient catalysis owing to abundant active electronic states, strong electronic coupling with reactants, and energetic preference. Exerting the value of metastable structures while evading the difficulty in direct synthesis remains challenging. Herein, it is reported that light irradiation enables the generation and maintenance of the metastable state over copper single atoms for efficient carbon dioxide reduction. Under irradiation with light, photogenerated electrons transit to Cu-3 d orbits and initiate d -orbital rearrangement. The initial symmetric Cu 1 ─O 4 coordination converts to the metastable asymmetric structure of Cu 1 ─O 2+1 , and is reversibly restored after removing the light. The photoinduced metastable intermediate of Cu 1 ─O 2+1 promotes the Cu single-atom catalyst to deliver an ethylene yield rate of 60.4 µmol g cat. −1 h −1 . Mechanistic studies reveal that Cu 1 ─O 2+1 possesses stronger adsorption capability for reactants and intermediates. The reaction energy barrier over Cu 1 ─O 2+1 also shows an obvious decline compared to that over Cu 1 ─O 4 .
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Nanomaterials
·
2023
·Vol. 13
·期 17
·2478
·
IF 5.3
Ning Wang,Yuanyuan Zhao,Xuelian Wu,Dapeng Li,Ruguang Ma,Zhigang Chen,Zhengying Wu
In this study, a Cu NPs-incorporated carbon-containing mesoporous SiO2(Cu/C-SiO2) was successfully synthesized through a grinding-assisted self-infiltration method followed by an in situ reduction process. The obtained Cu/C-SiO2was then employed as a Fenton-like catalyst to remove tetracycline (TC) from aqueous solutions. TEM, EDS, XRD, N2adsorption–desorption, FTIR, and XPS methods were used to characterize the crystal structure, morphology, porosity, chemical composition, and surface chemical properties of the catalyst. The effects of initial TC concentration, catalyst dosage, H2O2dosage, solution pH, HA addition, and water media on the TC degradation over Cu/C-SiO2were investigated. Scavenging and electrochemical experiments were then carried out to analyze the TC degradation mechanism. The results show that the Cu/C-SiO2can remove 99.9% of the concentrated TC solution (C0= 500 mg·L−1), and it can be used in a wide pH range (R.E.= 94–99%, pH = 3.0–11.0). Moreover, hydroxyl radicals (•OH) were detected to be the dominant reactive species in this catalytic system. This study provides a simple and promising method for the synthesis of heteroatom-containing mesoporous catalysts for the decomposition of antibiotics in wastewater.Keywords:Cu nanoparticles;mesoporous silica;Fenton-like catalyst;tetracycline
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Xiaoli Zhuang,Chao Han,Jingrui Zhang,Zhaohu Sang,Wei Meng
Metal/metal oxide heterojunctions with diverse combination is significantly desirable in constructing excellent electrochemical platform in the sensing field. In this paper, a ternary composite of Cu/Cu 2 O@C, in which a Cu/Cu 2 O heterojunctions with “head to head” combination fashion uniformly disperse in the octahedral carbon framework, is in situ generated by treating a copper-metal-organic framework (Cu-MOF) under a relatively mild temperature. The Cu/Cu 2 O@C composite is used as electrode material to modify glassy carbon electrode (GCE) to construct a glucose sensor, which shows excellent sensing behaviors with high detection sensitivities of 621.12 μA mM −1 cm −2 and 372.67 μA mM −1 cm −2 in the glucose concentration of 0.001–1.7 mM and 1.7–9.7 mM, respectively. Meanwhile, the Cu/Cu 2 O@C/GCE also exhibits outstanding selectivity for glucose as well as good stability, repeatability and practicability in the test process. The good sensing performances could attribute to the unique characteristics of Cu/Cu 2 O@C: (i) the highly dispersed Cu/Cu 2 O nanoparticles originating from metal-organic framework provide abundant catalytic-sites for the glucose oxidation ; (ii) the “head to head” combination fashion for Cu/Cu 2 O heterojunctions make Cu and Cu 2 O fully participate in the electrocatalytic oxidation for glucose. (iii) the in situ generated carbon framework promotes the charge transfer in the electrocatalytic process.
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FUEL PROCESSING TECHNOLOGY
·
2021
·
IF 7.033
Xiangchen Kong,Chao Liu,Weicong Xu,Yue Han,Yuyang Fan,Ming Lei,Ming Li,Rui Xiao
Stubborn lignin (SL) is the thermochemically stable fragment generated from biomass utilization (e.g., pyrolysis , hydrolysis, fermentation, pulping), which is comparatively difficult to be further depolymerized into value-added bio-products. The cleavage of the stubborn linkages within the structure of SL, such as C C, α -O-4, and 4-O-5 linkages, is the key for its valorization. Herein, we investigated the depolymerization of SL through catalytic hydroprocessing in supercritical methanol with Cu/CuMgAlO x catalyst. The yield of monomers reached 37.76C% with 240 min at 300 °C. Cyclohexanols were identified as the major monomeric products, indicating the occurrence of hydrodeoxygenation and hydrogenation. GPC , quantitative 13 C NMR, HSQC NMR, and HMBC NMR analyses evidenced the depolymerization of SL and upgrading of its derivatives. Furthermore, the mechanistic studies were carried out to provide insights to the stubborn linkage cleavages. The degrees of difficulty to break up the three involved linkages obeyed the sequence of β -5 > 4-O-5 > α -O-4. The apparent activating energies ( E a ), chemisorption energies ( E c ), and bond dissociation energies (BDE) were determined computationally to support the experimental results from the perspectives of kinetics, chemisorption, and thermodynamics, respectively. This research provides a reliable way for the utilization of SL.
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Journal of CO2 Utilization
·
2021
·
IF 7.132
Ziyi Zhao,Xiaotong Li,Jianghao Wang,Xiangzhou Lv,Hao Bin Wu
Electrochemical reduction of carbon dioxide to value-added fuels offers a promising method to solve increasingly serious environmental problems and alleviate energy crisis. Herein, we report a facile method by coating Cu electrode with CeO 2 nanoparticles to largely enhance the C 2+ products selectivity during CO 2 electroreduction. The Faradaic efficiency of C 2+ products for optimal CeO 2 -coated Cu electrode reached a high value of 61 % at -1.05 V vs RHE, and exhibited good stability for over 9 h of CO 2 electrolysis. The CeO 2 nanoparticles were found to induce oxidative corrosion of the Cu foil, leading to a CuO x layer in contact with the CeO 2 nanoparticles. The interface between CeO 2 nanoparticles and oxide-derived Cu might be attributed to the enhanced catalytic activity for C 2+ products by promoting the C C coupling process.
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2021
·Vol. 168
·期 8
·087503
·
IF 4.316
Fangzhao Pu,Zhipeng Yu,Wenjing Lu,Chuncai Kong,Ruijun Lin,Xingyu Bai,Xiaojing Zhang,Jian Lv,Zhimao Yang
Fast, reliable, and low-cost glucose detection methods are of great importance for the control of diabetes. In this study, Cu2O combined with Cu nanoparticles anchored on reduced graphene oxide (RGO), was synthesized to function as the electrode in a non-enzymatic glucose sensor. The synergistic effect between Cu nanoparticles and Cu2O, together with the high conductivity of RGO enabled considerably lower resistivity with greater glucose oxidation activity than pure Cu2O. The RGO@Cu2O@Cu electrode exhibited a high sensitivity of 1.112 mA mM−1 cm−2 with a detection limit of 0.019 μM, and the linear range is up to 4 mM. Additionally, the RGO@Cu2O@Cu electrode displayed good anti-interference performance within human blood and high stability while operating for a long duration. Significantly, the glucose detection capability of the as-designed electrode was comparable to commercial sensors, representing a valuable design for future non-enzymatic glucose sensing.
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Materials Express
·
2020
·Vol. 10
·期 10
·1725-1731
·
IF 1.65
Duan Xiaobo,Ding Yanhong,Yu Meng
Multilayer graphene was prepared in this study by microwave burst method. Cu9S5/CoS/graphene and CuS/CoS2/graphene composites were obtained by hydrothermal method to regulate the molecular structure and combination of Cu and Co metal sulfides on graphene
substrate. Graphite oxide was doped by hydrothermal method, and then Cu9S5/CoS/graphene composite was prepared by microwave explosion method. Raman, SEM and TEM were used to characterize the self-made graphene. Results showed that the multilayer graphene had a bag-like
structure which was beneficial to anchor sulfide. Three graphene-based composites were characterized by scanning electron microscopy, X-ray diffraction, energy spectrum analysis and electrochemical properties. Moreover, results showed that CuS/CoS2/graphene had the best electrochemical
performance, and its specific capacity reached 324 F/g when the current density was 1 A · g–1, which was much higher than that of the other two samples. Capacity retention rate, interfacial charge transfer resistance and electrolyte diffusion resistance also have advantages.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 6
·2280-2291
·
IF 6.119
Qingji Ying,Yue Liu,Yaoyu Zhang,Zhongbiao Wu
Herein, a facile in situ sulfation strategy was employed for modifying Cu/TiO2 catalysts using CuSO4 as the precursor to enhance the performance of dichloromethane (DCM) catalytic combustion. The experimental results revealed that the modified samples exhibited superior DCM conversion and COx yield compared to the pristine Cu/TiO2 catalyst. Among these, the 1CuSO4/TiO2 sample showed the best activity with near 90% conversion during 50 h of reaction at 275 °C. Characterization results showed that the in situ sulfation modification could considerably improve the catalyst acidity, benefiting the dissociative adsorption of DCM with C–Cl rupture. Notably, the surface sulfate groups provided abundant Brønsted acidic sites that release surface Cl species in the form of HCl at relatively low temperatures, preventing the surface Cu species from chloride poisoning. With excess CuSO4 addition, the intermediates derived from DCM dechlorination could not be decomposed in time due to the decreased reducibility, leading to their deactivation due to coke deposition. The superior performance of 1CuSO4/TiO2 is attributed to the balance achieved between acidity and redox capacity for DCM catalytic decomposition. Moreover, it was found that CuSO4/TiO2 could partially replace noble-metal Ru/TiO2 catalysts and achieve comparable performances. The findings of this study will aid the development of CVOCs catalytic combustion catalysts with good activity and stability.
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Journal of Cleaner Production
·
2020
·
IF 7.246
Chengcheng Shi,Dachao Yuan,Luping Ma,Guangsheng Fu,Shufang Wang,Yaguang Li
Sunlight-driven toluene elimination system faces the problems of low reaction rate, secondary pollution, and especially tricky to large-scale production. In this work, we used a PVP assisted spray drying method to synthesize Cu doped CeO 2 microspheres with the merits of zero waste water and solids discharge, kilogram level yield, uniform dispersion of Cu, and high toluene combustion activity. Further, a new photothermal device was constructed to heat catalysts to 295 °C under one standard sunlight irradiation. As a result, the new photothermal device supported Cu doped CeO 2 microspheres showed a full oxidation of toluene at the rate of 59.82 mmol g −1 h −1 under 1 sun irradiation, 150 times higher than the advanced sunlight-driven toluene elimination. An industrial demonstration of this new system was developed, and this system was able to completely deal with 22.2 m 3 h −1 of exhaust with the toluene concentration of 1–10,000 ppm under 1 m 2 of outdoor sunlight irradiation in the daytime of winter, showing the potential on industrial applications.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2020
·Vol. 35
·期 1
·e6066
·
IF 3.14
You Han,Yulian Wang,Yan Wang,Yubing Hu,Yao Nian,Wei Li,Jinli Zhang
A series of Cu-pyrrolidone/spherical activated carbon (SAC) catalysts were prepared via a simple incipient wetness impregnation method and then assessed in acetylene hydrochlorination, and the catalytic evaluation result indicated that the 1-methyl-2-pyrrolidinone (NMP) ligand was found to be the most effective one to significantly improve the activity and stability of Cu catalyst. The catalyst with the optimal molar ratio of NMP/Cu = 0.25 showed 94.2% acetylene conversion at 180°C and an acetylene gas hourly space velocity of 180 h −1 . Moreover, the acetylene conversion of Cu-0.25NMP/SAC remained stable over 99.1% for about 220 h under the industrial condition. Transmission electron microscopy (TEM) analyses proved that NMP ligand improved the dispersion of Cu species. In addition, hydrogen temperature-programmed reduction (H 2 -TPR), X-ray photoelectron spectra (XPS), thermogravimetric analysis (TGA), and Brunner–Emmet–Teller (BET) indicated that the additive of NMP was preferential to stabilize the catalytic active Cu + and Cu 2+ species and inhibit the reduction of Cu α+ to Cu 0 during the preparation process and reaction, hence restraining the coke deposition. Furthermore, the steady coordination structure between Cu and NMP was confirmed by Fourier-transform infrared spectra (FT-IR) and Raman combining with density functional theory (DFT) calculation, which could effectively lower the adsorption energy of catalyst for C 2 H 2 and inhibit the serious carbon deposition caused by excessive acetylene self-accumulation. Our findings suggest that the efficient, well-stabilized cost-effective, and environmentally friendly Cu catalyst has great potential in acetylene hydrochlorination.
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TALANTA
·
2020
·
IF 5.339
Zhixia Yao,Hanmeng Liu,Yaosheng Liu,Yongxing Diao,Guangxing Hu,Qifang Zhang,Zhuang Li
A novel fluorometric strategy is proposed for detecting curcumin by polyvinyl pyrrolidone-templated Cu NCs (PVP–Cu NCs) as a fluorescent probe which exhibits excitation/emission peaks at 380/510 nm. The fluorescent excitation and emission spectra of PVP-Cu NCs have a striking overlap with the UV–vis spectrum of curcumin, and the fluorescence lifetime of PVP-Cu NCs decreases after the addition of curcumin. Curcumin leads to fluorescence quenching based on fluorescence resonance energy transfer . This method allows for the determination of curcumin in the range of 0.1–10 μg mL −1 and the detection limit is 21 ng mL −1 . Furthermore, this method displays good selectivity and is successfully applied for real sample analysis.
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