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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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Shuaiqi Zhao,Jiajin Lin,Wenqiang Gong,Aihua Xu,Xiaoxia Li,Yongcai Qiu
Pt-based catalysts are one of the most extensively used heterogeneous catalysts for the degradation of pollutants, and regulating electron-metal-support interaction (EMSI) is an efficient strategy to enhance the performance of Pt-based catalysts. Herein, we introduced a quenching technique for regulating the EMSI of Pt-CuO/CeO 2 catalysts to significantly boost its CO catalytic activity. The EMSI optimized by quenching was determined to promote the electron redistribution between Pt and CuO/CeO 2 via Cu–O-Pt structure, thus forming more electron-rich Pt species and enhancing the surface oxygen species activity. From comprehensive characterization investigations, we confirmed that the superior activity arouse from the moderate Pt 0 /Pt 2+ ratio, in which CO molecules were preferentially adsorbed on the electron-rich Pt sites and reacted with active oxygen species from PtO x or CuO/CeO 2 , accelerating the whole CO catalytic process. Our finding provided a new inspiration to control EMSI of Pt-based catalysts and widened the application of quenching chemistry in heterogeneous catalysis.
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JOURNAL OF NANOPARTICLE RESEARCH
·
2023
·Vol. 25
·期 11
·1-12
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IF 2.5
Li Fangyuan,Yao Niu,Yuan Huiyu,Cui Junyan,Jia Quanli
The redox properties of electrode materials play a vital role in electrochemical performance. Fabrication of electrode materials with multiple oxidation species is highly desired for ultrasensitive glucose sensing. Herein, multivalent Cu/Cu 2 O/CuO/C (Cu/C) nanocomposites were successfully prepared for non-enzymatic glucose sensing by in situ pyrolysis of Cu metal-organic framework (Cu 3 (BTC) 2 ·3H 2 O, Cu-BTC) at a critical temperature. Structure characterizations showed that the nanocomposites maintained the original morphology of Cu-BTC crystals and exhibited mesoporous structures. Meanwhile, multiple Cu species containing Cu, Cu 2 O and CuO were generated simultaneously, which were tightly pinned on the ligand-derived carbon layers. Thus, under the synergistic effect of multivalent Cu species, mesoporous structure and intense interface contact, the sensing platforms based on Cu/C nanocomposites exhibited good glucose detection performance with a wide linear range of 0.005-2.0 mM, ultrasensitivity of 147.65 μA mM -1 cm -2 , low detection limit of 6.31 μM (S/N = 3), and favorable anti-interference properties and stability. Especially, the Cu/C sensing platform showed excellent recoveries of glucose when used to monitor glucose in real sample of honey. The good electrochemical activities of Cu/C nanocomposites render them promising candidates for sensors and other applications. Graphical abstract
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Wentao Hao,Panpan Xu,Li Sun,Ensi Cao
Co-doped TiO 2 ceramics exhibit great potential as high-performance giant dielectric materials. However, their excessively high sintering temperature renders them unsuitable for economical industrial production. The giant permittivity of these ceramics is closely correlated with the concentration of Ti 3+ ions present. Adding a sintering aid to the ceramics is an effective method to reduce the sintering temperature. CuO, a common sintering aid, not only reduces the sintering temperature but also potentially enhances the Ti 3+ ions concentration through the multivalence of Cu element, further optimizing their giant dielectric properties. Therefore, the effects of CuO addition on the sintering condition, microstructure, and dielectric properties of In and Nb co-doped TiO 2 ceramics were investigated. The results indicate that CuO effectively lowers the sintering temperature of the ceramics. However, the presence of a large number of Cu + ions inhibits the formation of Ti 3+ ions, resulting in the disappearance of their giant dielectric properties. Upon annealing at 1150 °C for 2 h in air, the Ti 3+ ions concentration significantly increases in the ceramics, consequently restoring their giant dielectric properties. Additionally, a new dielectric relaxation appears around 100 kHz, likely arising from the conductivity difference between the shallow layers and cores of grains induced by annealing. Furthermore, annealing enhances the grain boundary resistance, thereby reducing the low-frequency dielectric loss of the ceramics.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Yanhong Zhang,Hu Bai,Jiaming Chu,Haiyang Lan,Qi Zhou,Zixian Wang,Weitao Jin,Juan Zhou
A catalyst layer is coated on the fuel electrode in a proton-conducting solid oxide electrolysis cell reactor, which can optimize electrochemical performance and expand the application range of the reactor. In this work, CuO–ZnO catalyst is prepared by oxalate co-precipitation method and combined with a single cell to obtain a reactor with the structure of La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3-δ (LSCF) ǀ BaZr 0.1 Ce 0.7 Y 0.1 Yb 0.1 O 3-δ (BZCYYb) ǀ NiO-BZCYYb (active layer) ǀ NiO-BZCYYb (support layer) | CuO–ZnO (catalyst layer). The electrolysis current density of this reactor with humid air as oxidant and 20%CO 2 –80%H 2 as fuel is 2751 mA cm −2 under 1.3 V at 750 °C. It operates steadily for 138 h under 1.3 V electrolysis at 650 °C, which is better than the reactor without a catalyst layer under this condition. Additionally, CO and CH 4 are detected in the exhaust gas on the fuel electrode side, and the CO selectivity reaches over 90% at 750-550 °C.
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MOLECULES
·
2023
·Vol. 28
·期 14
·5554
·
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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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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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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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 17
·7333-7346
·
IF 4.5
Yasin Umsalama Abuelgasim Abubakr,Ahmed Md. Maruf,Zhang Juan,Jia Zhixin,Guo Tianyu,Zhao Ruihua,Shi Jiahui,Du Jianping
Design and development of high-effective photocatalysts to remove multiple organic pollutants are a great challenge. Herein, the band structure of CuO is regulated by constructing the heterostructures between AgBr and CuO, which is realized by controlling hybrid morphologies. The as-prepared AgBr/CuO material consists of CuO nanoflakes and AgBr nanoparticles. Notably, AgBr nanoparticles are adhering on the surface of CuO nanosheets, which favors the formation of heterojunction with point to plane contact and fasten electron transfer. The photocatalytic results show that the AgBr/CuO photocatalyst, prepared by using the 0.1 mol AgNO 3 and KBr as raw materials, presents superior photodegradation activity toward degradation of multi-pollutants with dye concentration of 15 mg L −1 and pH = 7. The methyl violet removal rate reaches 98% within 60 min in the present of 0.1 g catalyst under visible light, and rhodamine B and methyl blue are degraded to 98 and 78% within 90 min. The radical trapping tests prove that photogenerated superoxide radicals (∙O 2 − ) and holes (h + ) act as the main active species in photodegradation of MV. The result indicates that point to plane-contacted heterostructure of AgBr/CuO material plays a key role and it has potential application in the environment remediation. Graphical abstract
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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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MOLECULES
·
2023
·Vol. 28
·期 10
·4164
·
IF 4.6
Jassim Mohamed Hamed Al-Kurdhani,Huajun Wang
A series of supported CuO-based nanoparticle catalysts were prepared by the impregnation method and used for the synthesis of glycerol carbonate from glycerol and CO2in the presence of 2-cyanopyridine as a dehydrant and DMF as a solvent. The effects of supports (activated alumina, silicon dioxide, graphene oxide, graphene, and activated carbon), CuO loading amount, calcination temperature, and reaction parameters on the catalytic activity of the catalyst were investigated in detail. XRD, FTIR, SEM, BET, and CO2-TPD were used for the characterization of the prepared catalysts. It is found that CuO/Al2O3shows a higher catalytic activity, which depends on the CuO loading amount and calcination temperature. The surface area and number of basic sites of the catalyst exhibit a crucial effect on the catalytic activity of CuO/Al2O3. Furthermore, there is a synergistic effect between the catalyst and 2-cyanopyridine where the former has a higher activation ability for glycerol and the latter acts not only as a dehydrant, but also as a promoter for CO2activation. Recycling experiments reveal that this catalyst can be reused for at least five cycles without any inactivation. Based on the experiment results and FTIR characterization, a possible reaction mechanism for the carbonylation of glycerol and CO2is proposed.Keywords:glycerol;glycerol carbonate;carbon dioxide;2-cyanopyridine;CuO/Al2O3
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高影响因子
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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