Catalysts
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2022
·Vol. 12
·期 5
·509
·
IF 4.501
Chi Li,Yongfu Lian,Qin Zhou
The degradation of a high concentration of organic pollutants has long been a challenge to water restoration, and the development of electro-Fenton catalysis offers a practical approach to solving this problem. In this study, a novel electro-Fenton catalyst, activated fullerene soot-loaded NiO-doped CeO2(0.4(0.4NiO-CeO2)-AFS) nanoparticles, was prepared through the impregnation of 0.4NiO-CeO2particles and activated fullerene soot (AFS). When applied for the degradation of 200 mg/L of tetracycline, this catalyst demonstrated a degradation rate as high as 99%. Even after 20 cycles, the degradation rate was more than 80%. Moreover, it was concluded that AFS could initiate the synergistic effect between Ni and Ce dual active centers in the degradation of tetracycline; this can be ascribed to the extremely large specific surface area of AFS.Keywords:fullerene soot;NiO-doped CeO2;tetracycline;degrading efficiency;electro-Fenton
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JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Yue Chen,Shaobin Li,Li Zhang,Tao Jing,Jianxin Wang,Lijie Zhao,Fengbo Li,Chao Li,Jingyu Sun
Rational design and constructed new electrode material as high performance electrochemical sensor with outstanding selectivity, reproducibility and stability is an urgent demand for trace detection. Herein, a novel Ce-MOF/Ti 3 C 2 T X MXene composite as electrochemical sensor for L-Tryptophan (L-Trp) was constructed by utilizing the three-dimensional straw-sheaf-like Ce-MOF and Ti 3 C 2 T X MXene nanosheets . The combination of Ce-MOF and Ti 3 C 2 T X MXene not only significantly improves the conductivity of metal-organic framework (MOF) but also effectively prevents the stacking of Ti 3 C 2 T X MXene nanosheets. The electrochemical properties of the proposed sensor were investigated by electrochemical techniques in detail. The L-Trp sensor exhibits a wide linear range (0.2 μM–139 μM) and a low limit of detection (0.19 μM, S/N = 3). Moreover, the proposed sensor exhibits excellent selectivity, good reproducibility and long-term stability, as well as satisfactory practical ability in real blood serum samples.
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Journal of Energy Chemistry
·
2022
·
IF 13.599
Meng Li,Xiaodong Wu,Kun Liu,Yifan Zhang,Xuechun Jiang,Dongmei Sun,Yawen Tang,Kai Huang,Gengtao Fu
Urea oxidation reaction (UOR), which has favorable thermodynamic energy barriers compared with oxygen evolution reaction (OER), can provide more cost-effective electrons for the renewable energy systems, but is trapped by its sluggish UOR kinetics and intricate reaction intermediates formation/desorption process. Herein, we report a novel and effective electrocatalyst consisting of carbon cloth supported nitrogen vacancies-enriched Ce-doped Ni 3 N hierarchical nanosheets (Ce-Ni 3 N@CC) to optimize the flat-footed UOR kinetics, especially the stiff rate-determine CO 2 desorption step of UOR. Upon the introduction of valance state variable Ce, the resultant nitrogen vacancies enriched Ce-Ni 3 N@CC exhibits an enhanced UOR performance where the operation voltage requires only 1.31 V to deliver the current density of 10 mA cm −2 , which is superior to that of Ni 3 N@CC catalyst (1.36 V) and other counterparts. Density functional theory (DFT) results demonstrate that the incorporation of Ce in Ni 3 N lowers the formation energy of nitrogen vacancies, resulting in rich nitrogen vacancies in Ce-Ni 3 N@CC. Moreover, the nitrogen vacancies together with Ce doping optimize the local charge distribution around Ni sites, and balance the adsorption energy of CO 2 in the rate-determining step (RDS), as well as affect the initial adsorption structure of urea, leading to the superior UOR catalytic performance of Ce-Ni 3 N@CC. When integrating the Ce-Ni 3 N catalyst in UOR//HER and UOR//CO 2 R flow electrolyzer, both of them perform well with low operation voltage and robust long-term stability, proofing that the thermodynamically favorable UOR can act as a suitable substitute anodic reaction compared with that of OER. Our findings here not only provide a novel UOR catalyst but also offer a promising design strategy for the future development of energy-related devices.
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Solar RRL
·
2023
·Vol. 7
·期 21
·2300493
·
IF 7.9
Xiushuai Guan,Xiaochao Zhang,Changming Zhang,Rui Li,Jianxin Liu,Yunfang Wang,Yawen Wang,Caimei Fan,Zhong Li
The conversion of carbon dioxide to dimethyl carbonate (DMC) is an attractive process, but thermodynamic limitations of the reaction hinder its further development. Herein, a simple solution coprecipitation strategy for the synthesis of a series of Ce–metal organic framework (MOF)-derived CeO 2 nanoparticles is proposed to rapidly break the thermodynamic equilibrium and achieve highly efficient activation of CO 2 /CH 3 OH under photothermal system. The CeO 2 –M–5, Ce(NO 3 ) 3 ·6H 2 O/2-methylimidazoles molar ratio of 1:5, exhibits the highest DMC yield of 2.52 mmol DMC g −1 cat under photothermal system, higher 3.26 times than CeO 2 –C (nanoparticle by high-temperature calcination). Moreover, the DMC yield of CeO 2 –M–5 nanoparticles increases by 10% under the photothermal synergistic system compared to thermocatalytic system. This superior catalytic performance is attributed to the abundant Lewis acid–base sites, excellent light absorption capacity, and hydrophobicity. Besides, in situ diffuse reflectance infrared Fourier transform spectroscopy demonstrates that Ce–MOF-derived CeO 2 nanoparticles can effectively activate CO 2 /CH 3 OH to enhance the formation of the key intermediate methyl carbonate upon light irradiation. Finally, combining characterization and experimental results, the reaction mechanism of photothermal catalysis of CO 2 /CH 3 OH for DMC synthesis over Ce–MOF-derived CeO 2 nanoparticles is proposed. This work would provide new insights into the rational design of an effective catalyst for CO 2 to produce high value-added chemicals.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xia Li,Weiqiang Fan,Yajie Bai,Ying Liu,Fengfeng Wang,Hongye Bai,Weidong Shi
Photoelectrochemical nitrate (NO 3 – ) reduction reaction (PEC NRR) is a promising technology to solve both environmental pollution and traditional energy crisis. However, the fabrication of efficient catalyst with controllable active sites for high selectivity is still challenging. In this work, copper phthalocyanine (C 32 H 16 CuN 8 )/cerium dioxide (CuPc/CeO 2 ) heterostructure has been designed as a model to understand the role of Ce 3+ /Ce 4+ pairs on the formation of oxygen vacancies (OVs), which helps for identifying the key factors to adjust the chemical adsorption and activation of NO 3 – in PEC NRR system. Furthermore, the unique organic–inorganic hybrid matrix significantly strengthens the relationship of solar harvest–carriers’ separation–NO 3 – reduction. CuPc/CeO 2 heterostructure exhibits a high NH 3 yield of 1.16 μmol h −1 cm −2 and Faradic efficiency of 33% (-0.6 V vs.), and the desirable PEC NRR could be well retained for 5 cycles. Therefore, the construction of CuPc/CeO 2 successfully optimizes the thermodynamic and kinetic factors in PEC NRR system, providing a new insight for organic–inorganic hybridization and NH 3 green production.
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Redox Biology
·
2026
·
IF 16.2
Yaping Chen,Kaichen Zeng,Yunxin Ye,Xinyi Sun,Ling Yan,Ziya Lao,Yifan Wu,Tao Luo,Li Yang,Lvhua Guo
In situ integration creates an electronically coupled Ce MOF-CD nanozyme. • Interfacial electron transfer regulates the Ce 3+ /Ce 4+ redox balance. • pH-dependent catalysis switches from ROS generation to superoxide removal. • Ce MOF-CD reduces inflammation and accelerates MRSA-infected wound healing. Infected wounds require therapeutic materials that can control bacterial infection without aggravating oxidative tissue damage. Here, glutathione-derived carbon dots (GSH-CDs) were introduced during the formation of a cerium metal-organic framework (Ce MOF) through an in situ integration strategy to construct a carbon-dot-integrated Ce MOF nanozyme (Ce MOF-CD). Electronic-structure analyses supported interfacial electron redistribution from GSH-CDs toward Ce MOF, accompanied by changes in the local electronic environment and Ce 3+ /Ce 4+ distribution of the Ce active centers. Ce MOF-CD exhibited a distinct pH-dependent redox catalytic preference, with oxidase-like catalysis favored under acidic conditions and superoxide dismutase-like activity becoming more pronounced near neutrality. Accordingly, Ce MOF-CD markedly reduced the viability of MRSA and E. coli and disrupted established biofilms under acidic conditions. Under near-neutral cellular conditions, it reduced intracellular oxidative stress, attenuated inflammatory activation, and promoted repair-associated macrophage polarization. In an MRSA-infected wound model, Ce MOF-CD reduced bacterial burden and local inflammation, promoted tissue reconstruction, and accelerated wound closure with favorable biosafety. Overall, GSH-CDs-mediated interfacial electronic regulation modulates the pH-dependent redox catalytic behavior of Ce MOF, enabling antibacterial activity to be coordinated with oxidative-stress regulation during infected wound healing. Download: Download high-res image (393KB) Download: Download full-size image
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Environmental Science-Nano
·
2023
·
IF 7.3
Jinli Qiu,Huifang Chan,Wenting Zheng,Yao Feng,Fuqiang Liu
The design of metal–organic framework-derived metal oxides/sulfides is an effective approach for water remediation. A series of Fe–Ce composites (Fe–Ce–S–N) with cluster-like morphology were prepared with prussian blue analogue (PBA) as the precursor in a hydrothermal process. S doping promoted the conversion of Fe(III) to Fe(II), which greatly improved the performance of the Fenton-like reaction. The optimized Fe–Ce–S–N catalyst exhibited superior catalytic activity towards sulfamethoxazole (SMZ) degradation (18.63 mgSMZ gcat−1 min−1), showing the largest k value (0.1862 min−1), which was 2.1 and 8.1 times higher than that of Fe–Ce–S–H and Fe–Ce–N, respectively. Moreover, the Fe–Ce–S–N catalyst displayed a remarkable reusability, stability and adaptability in Fenton-like systems. Overall, this work provides new insights into extending novel PBA-derived catalysts to significantly improve heterogeneous Fenton-like performances.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yang Li,Feifei Yang,Jing Xiong,Kejia Liu,Wanhai Xiao,Tao Qi,Zhipeng Dong,Yong Wang
Rare earth polishing powder waste (REPPW) usually contains lanthanum (La) and cerium (Ce) with content over 50 %, thus its recovery is important for the cyclic utilization of rare earth. In the traditional acid leaching process, La and Ce are simultaneously leached and required further separation. Based on their leaching behavior difference, a two-stage hydrochloric acid leaching process was proposed in this study to recover and primarily separate La and Ce in REPPW. With the optimal operation conditions, La enriched solution with a relative purity of 91.11 % and Ce enriched solution with a relative purity of 92.85 % were obtained and their recovery ratio were 59.47 and 85.15 %, respectively. After precipitation and calcination, products of La 2 O 3 with purity of 83.67 % and CeO 2 with purity of 93.38 % were obtained. Besides, individual leaching kinetics of La and Ce in low-acid leaching were studied using various shrinking core models. Based on the analysis of phase components and micromorphology evolution of REPPW during the leaching process, the leaching mechanism of REPPW was determined. Combined the leaching regularity with the fitting results, the leaching process of La was controlled by interfacial transfer and product layer diffusion, and the Ce was by product layer diffusion. The apparent activation energies of the LaOF and CeO 2 leaching reactions were 89.97 kJ/mol and 79.03 kJ/mol, respectively.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Jun-Wei Huang,Xiao-Feng Dong,Xiao-An Lv,Xiao-Na Ren,Chang-Chun Ge
The Si 3 N 4 ceramics with ternary ZrN–AlN–Re 2 O 3 (Re=Yb, Y, Nd, Ce, La) and ZrN–AlN system as sintering additives were prepared by hot-pressed sintering with vacuum environment at 1750°C-30min–30MPa. Subsequently, the effect of the ternary additives system with 2 wt% Re 2 O 3 on phase transformation, grain boundary phases, microstructure, and mechanical properties of the Si 3 N 4 ceramics were investigated firstly. All samples achieved the high β-Si 3 N 4 phases transformation (≥98.86%), while the grain boundary phases Re x Zr 1-x O (4-x)/2 and Yb 2 Si 2 O 7 were detected in the sintered Si 3 N 4 ceramics with Re 2 O 3 additives. Additionally, compared with Si 3 N 4 ceramic not contain Re 2 O 3 additives, the Si 3 N 4 ceramics added Re 2 O 3 additives presented the textured microstructure with more elongated rodlike β-Si 3 N 4 grains based on the XRD and SEM results. Consequently, the sample S-Ce with added CeO 2 additive shows the highest relative density of 99.85% and optimal fracture toughness of 8.75 ± 0.36 MPa m 1/2 . The sample S–Nd with added Nd 2 O 3 additive presented a highest bending strength of 1061.78 ± 41.76 MPa. Sample S–Yb with added Yb 2 O 3 additive presented the maximum Vickers hardness of 16.35 ± 0.07 GPa. The results of this study can provide a helpful reference for the preparation of high-performance Si 3 N 4 ceramics.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2020
·Vol. 99
·期 9
·1962-1975
·
IF 1.687
Haoran Du,Zhaoping Zhong,Bo Zhang,Jimin Fu,Zhaoying Li
To obtain high-value bio-oil, pure ceria (CeO 2 ) and a series of Ce/Fe composite metal oxides were synthesized via precipitation method and were used to enhance hydrocarbons and ketones production during catalytic pyrolysis of bamboo sawdust. The characterization results were comprehensively analyzed and revealed that doping CeO 2 with Fe promoted the formation of a solid solution structure, which further increased the surface area and number of oxygen vacancies of the catalyst for deoxygenation. Experimental consequences demonstrated that, compared to non-catalytic trial, the catalytic pyrolysis over CeO 2 generated lower amounts of acids and aldehydes, and enhanced the conversion of large oxygenates to monofunctional hydrocarbon precursors via decarboxylation, deoxidation, and ketonization. The concentrations of hydrocarbons and ketones obtained over Ce/Fe catalysts were significantly higher than those obtained over CeO 2 , and that was attributed to the higher surface area and oxygen storage capacity of Ce/Fe catalysts. Particularly, the composite catalyst with the Ce/Fe molar ratio of 4 (Ce 0.8 Fe 0.2 ) presented the most optimal deoxidation capacity in this study. The relative concentration of hydrocarbons generated over Ce 0.8 Fe 0.2 was the highest, and monocyclic aromatics and short-chain aliphatic hydrocarbons accounted for 47.13% and 29.72%, respectively, of the total hydrocarbons. Simultaneously, the amount of ketones, the main hydrocarbon precursors, obtained over Ce 0.8 Fe 0.2 was significantly higher than that obtained over CeO 2 , and the fraction of linear and cyclic ketones of the total ketones increased from 45.96% for the non-catalytic pyrolysis to 97.57%. This further confirmed that the mesoporous Ce/Fe composite catalysts efficiently catalyzed the aldol condensation and ketonization reactions.
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ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Da-Wei Yang,Ya-Lan Liu,Tai-Qi Yin,Shi-Lin Jiang,Yu-Ke Zhong,Lin Wang,Mei Li,Zhi-Fang Chai,Wei-Qun Shi
To study the application perspectives of binary Ga–Al alloy electrodes in pyroprocessing, the utilization of Ga–Al alloy electrode for the separation of U from Ce was studied in this work. Specifically, the reduction behaviors of U (III) on Ga, Al and Ga–Al alloy electrodes was first explored in LiCl–KCl eutectic at 773 K. The cathode peak potential of U (III) at the Ga–Al alloy electrode was 0.44 V (vs. Li/Li 3 Bi), and less affected by the Ga/Al ratio. Moreover, potentiostatic electrolysis at 0.55 V (vs. Li/Li 3 Bi) was conducted on the Ga–Al alloy electrode for 4 h to separate U from Ce. X-ray diffraction (XRD) analysis indicated the co-existence of Al 3 U and Ga 3 U with an identical crystal structure in the deposits. Scanning electron microscopy coupled with energy dispersive spectroscopy (SEM-EDS) illustrated a good diffusion of U metal in Ga–Al alloy electrodes. Inductive coupled plasma optical emission spectrometry (ICP-OES) determinations exhibited an excellent separation performance of the Ga–Al alloy electrode.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2020
·
IF 4.495
Qinghong Meng,Xuejiao Wang,Qi Zhu,Ji-Guang Li
A series of phase-pure [(Gd 0.6 Lu 0.4 ) 0.99 Ce 0.01 ] 3 [Al 1- z (Mg/Si) z ] 5 O 12 ( z = 0-0.10) garnet phosphor powders were prepared via gel-combustion, which were then sintered into ceramics (up to 1550 °C) under atmospheric pressure. Dilatometry revealed that equimole of Mg 2+ /Si 4+ substitution for Al 3+ accelerates densification and lowers the activation energy for grain boundary diffusion in the intermediate stage of sintering (∼1150–1370 °C), which was assayed to be ∼353 kJ/mol for z = 0 and ∼289 kJ/mol for z = 0.10. The acceleration effects of Mg 2+ /Si 4+ on sintering and grain growth were further demonstrated by the results of ramp and holding sintering. Firing at 1550 °C for 4 h also produced ∼99 % dense ceramics for the Mg 2+ /Si 4+ codoped garnet powders. Through considering crystal splitting of the Ce 3+ 5d energy level, photon-phonon coupling, and crystal structure/microstructure, the influences of Mg 2+ /Si 4+ content and material form on Ce 3+ luminescence, including intensity, external/internal quantum efficiencies, emission wavelength, CIE color coordinates and decay time, were clarified in detail.
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