MOLECULES
·
2023
·Vol. 28
·期 14
·5554
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IF 4.6
Sheli Zhang,Yuerong Yan,Wei Hu,Yunchang Fan
Metal oxide nanoparticles (NPs) have been widely used as catalysts in the chemical industry, but their preparation is usually limited by strict conditions such as high temperature, elevated pressure, and the use of volatile and highly toxic organic solvents. To solve this problem, this work developed an environmentally benign method using green solvents, i.e., natural deep eutectic solvents (NADESs), as a reaction medium to prepare copper oxide (CuO) particles. The experimental results suggested that the synthesized CuO particles were sheet-like mesoporous NPs, and they exhibited excellent catalytic performance towards the photodegradation of rhodamine B (RhB) in the presence of potassium monopersulfate (PMS). The catalytic activity of the synthesized CuO NPs was better than that of the reported metal oxide-based catalysts. Reactive species such as photoexcited holes, superoxide radicals, and singlet oxygen were involved in the RhB degradation. These results indicated that NADESs are good media for the preparation of CuO NPs, and exhibit the potential for application to the preparation of other metal oxides.Keywords:natural deep eutectic solvents;photocatalytic degradation;copper oxide;rhodamine B;photoexcited holes
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2023
·
IF 3.8
Umsalama Abuelgasim Abubakr Yasin,Zhixin Jia,Ziwen Qin,Tianyu Guo,Ruihua Zhao,Jianping Du
A series of MoS 2 -modified CuO (CuO/MoS 2 ) heterostructures were successfully fabricated. The photodegradation properties of organic dyes were explored in detail under visible light. The photocatalytic results demonstrate that the CuO/MoS 2 -3 heterostructure delivers superior degradation rates towards methyl violet dye (MV) and rhodamine B (RhB), reaching 99.8% and 95.3% within 30 min, respectively. The decent photodegradation activity is due to improved visible light adsorption and faster transfer of electron-hole pairs. The radical trapping experiments show that superoxide radicals (· O 2 - ) and holes (h + ) are the main active species in the removal of MV. Furthermore, the CuO/MoS 2 -3 composite possesses the prominent stability and recyclability. This work offers a highly sustainable technique for designing a high-efficiency photocatalyst to remove environmental pollutants.
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Catalysts
·
2023
·Vol. 13
·期 9
·1246
·
IF 3.9
Jianhui Zhao,Huan Li,Yuanzhou Wang,Jingjie Yu,Ning Li,Shaopo Wang
Biochar (BC) usually has abundant surface functional groups, well-developed pore structures and high specific surface areas, which can combine with transition metals for peroxymonosulfate (PMS) activation to degrade organics. In this paper, BC modified with Cu/CuO was prepared by a modified impregnation pyrolysis method using peanut shells as raw materials. The morphology, structure and physicochemical properties were analyzed. Results showed that the originally smooth BC surface was modified into a rough structure with distributed metal particles, and the specific surface area of the modified Cu/CuO-BC700 (i.e., Cu/CuO-BC) increased from the initial 22.57 to 192.64 m2/g. The Cu/CuO-BC was employed for PMS activation and tetracycline (TC) degradation, achieving a removal efficiency of 93.2% at TC initial concentration 20 mg/L, PMS concentration 0.5 mM and catalyst dosage 0.1 g/L after 30 min. The influence of co-existing anions in the actual water on TC degradation followed the order of HCO3−> H2PO4−> Cl−, and HA had an inhibitory effect on TC degradation. A variety of active species participated in TC degradation, and the free radical pathway played a dominant role. Furthermore, the Cu/CuO-BC could maintain the degradation efficiency of TC up to 80% even after five consecutive cycles. The Cu/CuO-BC maintained high activity through redox reactions between catalytically generated active species and the cycling of metal ions (Cu+/Cu2+).Keywords:Cu/CuO;modified biochar;peroxymonosulfate;active species;tetracycline
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AICHE JOURNAL
·
2023
·Vol. 69
·期 10
·e18158
·
IF 3.7
Han Han,Xue Ye,Jie Yao,Xinhua Gao,Jinghao Yu,Lisheng Guo,Jie Li
The application of heterogeneous catalysts in dimethyl carbonate (DMC) synthesis from methanol is hindered by low activation efficiency of methanol to methoxy intermediates (CH 3 O*), which is the key intermediate for DMC generation. Herein, a catalyst of alkali metal K anchored on the CuO/ZnO oxide is rationally designed for offering Lewis acid–base pairs as dual active centers to improve the activation efficiency of methanol. Characterizations of CO 2 -TPD, NH 3 -TPD, XPS, and DRIFTS revealed that the addition of Lewis base K observably boosted the dissociation of methanol and combined with Lewis acid CuO/ZnO oxide to adsorb the formed CH 3 O* stably, thus synergistically promoted the transesterification. Finally, the CuO/ZnO-9%K 2 O catalyst exhibited the optimal catalytic activity, achieving a high yield of 74.4% with an excellent selectivity of 98.9% for DMC at a low temperature of 90°C. The strategy of constructing Lewis acid–base pairs provides a reference for the design of heterogeneous catalysts.
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FUEL PROCESSING TECHNOLOGY
·
2023
·
IF 7.5
Weicong Xu,Peijun Li,Nan Wang,Xiaowen Ding,Yujia Chen,Beichen Xue,Tao Li,Chao Liu,Rui Xiao
Electrocatalytic reduction is a promising strategy for CO 2 utilization, while the conversion of CO 2 to C 2 products usually suffers from the low selectivity. Herein, we report several high-performance Cu-OCN catalysts for electroreduction CO 2 -to-C 2 H 4 , which are prepared through the in-situ calcination of nanocube Cu 2 O and urea. The highest C 2 H 4 faradaic efficiency from Cu-OCN-10 reaches 55.97%, much higher than that from the pristine CuO counterpart (38.31%), with a partial current density of −12.83 mA cm −2 . Catalyst characterizations and first-principles density functional theory calculations reveal that the superior performance of CuO-OCN is attributed to the introduced nitrogen (N) species and oxygen (O)-vacancies. With the assistance of N species and O-vacancies, the adsorption of CO 2 on Cu-OCN-10 is thermodynamically favorable with the absorption energy of −0.69 eV. Meanwhile, the activation of CO 2 is promoted and the generated *CO intermediate on Cu-OCN-10 is stable, whose release needs to overcome an energy of 2.26 eV, thereby enhancing the C C coupling to produce C 2 H 4 . In general, the synergistic effects of N species and O-vacancies in Cu-OCN catalysts facilitate CO 2 electroreduction to C 2 H 4 .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yaru Xi,Zuoyi Xiao,Hui Lv,Haodong Sun,Shangru Zhai,Qingda An
Copper oxide (CuO) and copper (Cu) have been viewed as the prospective pseudocapacitive electrode materials for supercapacitors. Nevertheless, the poor electron transfer capacity, loading amount, and cycling stability limit their wide applications, which can be addressed by developing the CuO based heterojunction on conductive carbons. Here, a CuO/Cu@C comprising CuO/Cu nanoflowers and chitosan-derived N -doped porous carbon was compounded by simple mechanical mixing, freeze-drying, and carbonization. The composite heated at 700 °C exhibited a high specific capacitance of 2479F/g at 0.5 A/g and excellent cycling stability with capacitance retention of 82.43 % after 10 000 charge–discharge cycles. In addition, the asymmetric supercapacitor (ASC), i.e., CuO/Cu@C-700//AC assembled by CuO/Cu@C (as a positive electrode) and activated carbon (AC, as a negative electrode) displayed a great energy density of 76.87 W h kg −1 at 374.5 W kg −1 and kept as high as 25.83 W h kg −1 even at 14998 W kg −1 . Our work provides a new pathway to preparing transition metal oxide-based electrode materials with distinguished electrochemical performances.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Qinghe Liu,Sen Wang,Fei Han,Shupei Lv,Zairong Yan,Yunfei Xi,Jing Ouyang
Highly efficient three-dimensional (3D) kaolinite/MnO2–CuO (KM@CuO–NO3) catalysts were synthesized by a mild biomimetic strategy. Kaolinite flakes were uniformly wrapped by ultrathin tremelliform MnO2 nanosheets with thicknesses of around 1.0–1.5 nm. Si–O and Al–O groups in kaolinite hosted MnO2 nanosheets to generate a robust composite structure. The ultrathin MnO2 lamellar structure exhibited excellent stability even after calcination above 350 °C. Kaolinite/MnO2 exhibited abundant edges, sharp corners, and interconnected diffusion channels, which are superior to the common stacked structure. Open channels guaranteed fast transportation and migration of CO and O2 during CO oxidation. The synthesized KM@CuO–NO3 achieved a 90% CO conversion efficiency at a relatively low temperature (110 °C). Furthermore, the abundant oxygen vacancies on KM@CuO-NO3 assisted the adsorption and activation of oxygen species and thus enhanced the oxygen mobility and reactivity in the catalytic process. The mechanism results suggest that CuO introduced to the catalyst not only acted as CO active sites but also weakened the Mn–O bond, subsequently improved the mobilities of the oxygen species, which was found to contribute to its high activity for CO oxidation. This study provides new conceptual insights into rationally regulating structural assembly between transition metal oxides and natural minerals for high-performance catalysis reactions.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Kunlin Li,Jiayu Feng,Xingguang Hao,Xin Song,Changbin Zhang,Ping Ning,Kai Li
In this study, CuO@SiO 2 core-shell catalysts were successfully synthesized and applied to efficiently remove hazardous gaseous pollutant arsine (AsH 3 ) by catalytic oxidation under low-temperature and low-oxygen conditions for the first time. In typical experiments, the CuO@SiO 2 catalysts showed excellent AsH 3 removal activity and stability under low-temperature and low-oxygen conditions. The duration of the AsH 3 conversion rate above 90 % for the CuO@SiO 2 catalysts was 39 h, which was markedly higher than that of other catalysts previously reported in the literature. The considerable catalytic activity and stability were attributed to the protection and confinement effects of the SiO 2 shell, which resulted in highly dispersed CuO nanoparticles . Meanwhile, the strong interaction between the CuO core and SiO 2 shell further facilitated the formation of active species such as coordinatively unsaturated Cu 2+ and chemisorbed oxygen. The accumulation of oxidation products (As 2 O 3 and As 2 O 5 ) on the interface between the CuO core and SiO 2 shell and the pore channels of the SiO 2 shell is the main cause of catalysts deactivation . Furthermore, through combined density functional theory (DFT) calculations and characterization methods, a reaction pathway including gradual dehydrogenation (AsH 3 *→AsH 2 *→AsH*→As*) and gradual oxidation (2As*→As*+AsO*→2AsO*→As 2 O 3 ) for the catalytic oxidation of AsH 3 on CuO (111) surface was constructed to clarify the detailed reaction mechanism. The CuO@SiO 2 core-shell catalysts applied in this study could provide a powerful method for developing AsH 3 catalysts from multiple know AsH 3 removal systems.
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FUEL
·
2022
·
IF 8.035
Xiang Lv,Yi Gao,Yueshuai Cui,Chen Wang,Gangchui Zhang,Fang Wang,Peijin Liu,Wen Ao
The ignition and combustion properties of n -Al/CuO/kerosene nanofluid fuels are examined, with a focus on the formulation effects of the n -Al/CuO nano-thermite. The DSC data shows the addition of CuO facilitates the exothermic process of n -Al particles, which then promote the n -Al/CuO/kerosene droplets to evaporate. There are two exothermic peaks on the DSC curve of n -Al/CuO (5 %) at 249.3 ℃ and 463.8 ℃, respectively. The burning of n -Al/CuO/kerosene droplets consists of four stages: ignition, d 2 -law combustion, vapor flame extinguishment, and agglomerate burning. During the agglomerate burning stage, n -Al/CuO (5 %)/kerosene shows the minimum ignition delay at 0.057 s and the highest emission spectral intensity. Droplet combustion conforms well to the d 2 -law, and the maximum combustion rate is found for n -Al/CuO (20 %)/kerosene, at 1.287 mm 2 s −1 . The particle size of combustion residues is uniform, and the overall appearance smoothens as the CuO content increases. A new nanofluid fuel with better ignition and combustion properties than traditional nanofluid fuels is proposed.
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ChemElectroChem
·
2022
·Vol. 9
·期 15
·e202200529
·
IF 4.782
Xiao Wang,Qian Liu,Xiaopei Qiu,Yingran Wang,Hanqing Xu,Qingle Liang,Jun Wang,Mingxuan Gao,Jing Bao,Ming Chen
Graphical An ultra-fast and sensitive glucose sensor based on CuO nanoflowers coated stereo-graphene electrode on carbon cloth was developed. This kind of flexible enzyme-free glucose sensor has been successfully applied to the detection of glucose in actual serum samples and shows a good accuracy, which is likely be applied to the medical testing field and the commercial production and has potential to further applied in wearable sensors. Designing a highly sensitive, fast response, cheap, and flexible biosensing platform has important significance in the diagnosis of diabetes. Herein, we developed an ultra-fast and sensitive glucose sensor based on CuO nanoflowers-coated stereo-graphene electrode on carbon cloth. The three-dimensional graphene (3DG) nanostructures were established on the carbon cloth (CC) by radio frequency plasma enhanced chemical vapor deposition (RF-PECVD), and CuO nanoflowers subsequently obtained via chemical deposition. The prepared CuO@3DG@CC electrode with self-assembled structures provided abundant ion diffusion channels, large specific surface area and high conductivity, which shows an ultrasensitive current response to glucose. The detection limit of the sensor is as low as 0.068 μM and the response efficiency is as fast as 0.5 s. The electrode has two linear ranges with 0.5–115.5 μM and 165.5–1165.5 μM and has a strong anti-interference ability and shows an excellent stability. This kind of flexible enzyme-free glucose sensor has been successfully applied to the detection of glucose in actual serum samples and shows a good accuracy, which is likely be applied to the medical testing field and the commercial production and has potential to further applied in wearable sensors.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Yao Chen,Shaopeng Chen,Zhenlan Deng,Xiaoyu Xu,Jun Qin,Xincheng Guo,Zhuyu Bai,Xiaolang Chen,Zongcheng Lu
Adsorption is gaining popularity as an efficient, fast, and low-cost method for the removal of organic dyes in the wastewater treatment . In this work, a novel inorganic-organic adsorbent, polystyrene/CuO/calcined layered double hydroxide (PS/CuO@CLDH) microspheres , was successfully fabricated through the dispersion polymerization method for the efficient removal of Conon red (CR). The structure of the microspheres of products was characterized, and the marked impact of key variables (e.g., adsorbent dosage, pH, contact time, and initial dye concentration) on its adsorption was investigated. PS/CuO@CLDH10 exhibits the highest adsorption capacity compared with other composite materials, in which the adsorption capacity can reach 484.6 mg g −1 when the addition amount is 10 mg. Furthermore, the dynamics and isotherms fit better with the pseudo-second-order and Freundlich model. The adsorption thermodynamic data illustrate that the adsorption process of PS/CuO@CLDH10 on CR is endothermic, spontaneous, and thermodynamically feasible. Moreover, PS/CuO@CLDH10 maintains high removal efficiency and structural composition after four cycles, revealing its excellent recyclability and stability. Therefore, this work provides a novel idea for designing and fabricating inorganic-organic composites for efficient adsorption in wastewater treatment.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Wencheng Ma,Shaobo Zhang,Yiru Chen,Dan Zhong,Qinghui Du,Jinxin Li,Ru Li,Xuan Du,Jingna Zhang,Taiping Yu
In this study, lignite activated coke (LAC) was used as the carrier for the first time, Fe 3 O 4 –CuO composite metal oxide was used as the main active material, and the nano-scale magnetic supported composite metal oxide Fe 3 O 4 –CuO@LAC catalyst was synthesized for the first time, which can effectively activate the active oxygen in peroxodisulfate (PS). XRD, FTIR , BET, SEM , XPS and other analysis results showed that there was particulate matter with spherical structure on the surface of the active coke, and its diffraction peaks matched well with the characteristic peaks of Fe 3 O 4 and CuO, and it was a mesoporous structure with a specific surface area of 619.090 m 2 g −1 . By optimizing the experimental conditions, the results showed that more than 92% of hydroquinone can be removed under the conditions of hydroquinone concentration of 50 mg/L, pH = 5, adding 0.1 g/L catalyst and 3 mmol/L PS. EPR and quenching experiments proved that there were four reactive oxygen species in the reaction system ·OH, SO 4 − ·, O 2 − · and 1 O 2 . According to the degradation products of hydroquinone detected by LC-MS, the possible degradation path was deduced which laid a foundation for solving the problem of difficult treatment of phenol-containing wastewater in coal chemical industry.
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