Journal of Cleaner Production
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2021
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IF 9.297
Fengjiao Lai,Feng Yan,Pengju Wang,Fan Qu,Xuehua Shen,Zuotai Zhang
Efficient conversion of biomass-derived carbohydrates to alkyl levulinates is an important goal of biorefinery process, but is still challenging on applicable catalyst. Ce–Si pillared montmorillonite (CeSiM) clay heterostructures , incorporated with Wells-Dawson tungstophosphoric acid (H 6 P 2 W 18 O 64 , DPW), were prepared for the first time and used as the multifunctional catalyst for direct production of ethyl levulinate (EL) from various biomass-derived sugars. The DPW introduced by sol-gel method (DPW-CeSiM) has been effectively incorporated into the framework of porous CeSiM, while part of DPW was just absorbed on the surface of CeSiM by impregnation method (DPW-CeSiM-I). The DPW-CeSiM catalyst has large specific surface area owing to the insertion of Ce–Si pillars, and possesses strong Brønsted acidity and moderate Lewis acidity originated from the incorporated DPW and the Ce-doping, respectively. Due to the well synergistic effect of porous structure and dual acid, the DPW-CeSiM catalyst efficiently catalyzed the conversion of glucose into EL with 56.2% yield and nearly 100% conversion at 170 °C for 4 h. The recyclability studies certified that DPW-CeSiM catalyst showed higher stability than DPW-CeSiM-I over cycles and could be easily recovered from consecutive alcoholysis of biomass-derived sugars. The DPW-CeSiM catalyst also displayed high activity toward the conversion of other biomass-derived carbohydrates (fructose, sucrose, cellobiose and cellulose) into EL. Therefore, this work provides an instructive strategy for the design of efficient and stable DPW-based catalysts with dual acid sites uniformly distributed over the porous structure, which is obviously potential for industrial production of alkyl levulinates from carbohydrates and biomass.
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CANADIAN JOURNAL OF CHEMICAL ENGINEERING
·
2020
·Vol. 99
·期 9
·1962-1975
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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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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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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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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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
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IF 14.229
Zhi Zhu,Changchang Ma,Kesheng Yu,Ziyang Lu,Zhi Liu,Pengwei Huo,Xu Tang,Yongsheng Yan
In the present study, we constructed the Ce-doped biomass carbon-based mesoporous g-C 3 N 4 photocatalyst via alternanthera philoxeroides griseb growing guide using calcination method. The Ce-C@g-C 3 N 4 exhibited more superior photocatalytic performance for 2-mercaptobenzothiazole (96 %) degrading than that of pure g-C 3 N 4 (39 %) and C@g-C 3 N 4 (60 %). As a consequence, the improved degradation efficiency of Ce-C@g-C 3 N 4 attributed to the biomass carbon can significantly enhance the mass transport channels of electron-hole pairs. Meanwhile, the doped Ce 4+ ions acting as the redox center can sufficiently utilize the photogenerated carriers for generating more active radicals. Also, the possible photocatalytic reaction mechanisms including transfer behaviors of charge carriers, generation of reactive species, intermediate degradation products are also discussed in detail. This work may provide a promising approach for synthesizing g-C 3 N 4 -based photocatalyst by the plant growing guide and application in wastewater treatment.
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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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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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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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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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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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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Xixiang Meng,Caizhi Lv,Xiaohui Wen,Xiandeng Hou,Chenghui Li,Juan He
A new bimetallic-centered MOFs, NH 2 -MIL-125(Ti/Ce), was synthesized by partially replacing Ti with Ce. The doping of Ce endowed the MOFs oxidase-like activity and enabled the construction of a ratiometric fluorescence sensing system in combination with o-phenylenediamine (OPD) for detecting trace Cu 2+ with a limit of detection of 16 nM and a linear range of 0.02–50 μM. Trace Cu 2+ was successfully quantified in real water samples. The doping of Ce also increased the photocatalytic capability of the MOFs by about 2 times, achieving excellent reduction of Cr(Ⅵ) under natural light conditions.
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MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Xiao Teng,Bo Zhang,Luxia Yin,Wanyi Tao,Zhang Wen,Zekai Zhang,Wensheng Ning
A series of PdO/CeO 2 /SiO 2 -z aerogel composites with different molar ratio of Si/Ce were facilely fabricated via sol-gel method combined with atmospheric drying technology, where a major of Ce 3+ species could be oxidized to Ce 4+ species by adding hydrogen peroxide. They were used to remove thiophenics from model fuels and aromatics, compared with PdO/SiO 2 and CeO 2 /SiO 2 aerogel composites. Adding Ce and Pd led to an appearance of weak Lewis acid centers on the surface of adsorbents. Compared with PdO/SiO 2 and CeO 2 /SiO 2 , the adsorption capacity of PdO/CeO 2 /SiO 2 -z significantly increased, in which PdO/CeO 2 /SiO 2 -100 performed best and the adsorption capacity for thiophene was 15.0 mg-S/g ads , which was about the sum of PdO/SiO 2 -636 and CeO 2 /SiO 2 -100. The case was attributed to π-complexation of Pd 2+ and S-M (Pd, Ce, acted as Lewis acid centers) bond (σ) with thiophenics, where the adsorption process was dominated by S–Ce bond. Combined with the same chemical state of Pd and Ce in single metal and bimetal adsorbents verified by XPS , it can be deduced that no synergistic interaction between Pd and Ce species was formed in the adsorption process. PdO/CeO 2 /SiO 2 -100 exhibited a higher resistance for competitive adsorption of aromatics and a good solvent washing regeneration performance. The adsorption process of PdO/CeO 2 /SiO 2 -100 for thiophene was well fitted by Langmuir isothermal and pseudo-secound-order model and were spontaneous and endothermic. The solvents (n-heptane, benzene and p-xylene) have no obvious effect on the adsorption thermodynamics and kinetics of PdO/CeO 2 /SiO 2 -100.
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