JOURNAL OF CATALYSIS
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2025
·
IF 6.5
Juan Chen,Linmeng Wang,Hongyi Gao,Rushuo Li,Zhiyuan Liu,Tao Ban,Shunzheng Zhao,Jichao Yang,Ge Wang
Single-atom catalysts (SACs) catalysts have unique electronic properties and geometric structures, offering maximum atom-utilization efficiency. Noble metal-free SACs anchored within metal–organic frameworks (MOFs) enable precise tuning of electronic structures and significantly enhance catalytic activity beyond conventional porous materials. Herein, we synthesized the synthesis of Cu(I)/Ce-MOF-808-EA by anchoring atomically dispersed Cu(II) species onto the open Ce 6 nodes of the Ce-MOF-808 framework, followed by in situ reduction to Cu(I) via ethanol treatment and thermal activation processes. The atomic dispersion and valence transformation of Cu sites on Ce-MOF-808 were confirmed by X-ray Absorption Spectroscopy (XAS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), and X-ray photoelectron spectroscopy (XPS). The resulting Cu(I)/Ce-MOF-808-EA exhibited outstanding catalytic performance for the hydrogenation of Dicyclopentadiene (DCPD), achieving 100 % conversion, 91.54 % selectivity toward Dihydrodicyclopentadiene (DHDCPD), and 8.45 % selectivity toward Tetrahydrodicyclopentadiene (THDCPD) at 100 °C, 2 MPa. Notably, Cu(I)/Ce-MOF-808-EA outperformed other transition metal catalysts (Co/Ce-MOF-808-EA, Ni/Ce-MOF-808-EA and Zn/Ce-MOF-808-EA). For the first time, Density Functional Theory (DFT) calculations, combined with experimental investigations, revealed a low-energy reaction pathway for DCPD hydrogenation, wherein Cu(I) sites, in cooperation with adjacent oxygen atoms, act as bi-active centers to heterolytically cleave H 2 into proton and hydride species (*H δ+ -H δ- ) for subsequent hydrogenation. This study underscores the potential of MOFs as versatile platforms for engineering single-atom catalysts with enhanced catalytic properties.
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Waste and Biomass Valorization
·
2024
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IF 2.6
Luo Bo,Liu Huiyu,Shan Rui,Zhang Jun,Yuan Haoran,Chen Yong
Purpose This work aims to investigate the thermal behavior and kinetic characteristics of polyethylene (PE) pyrolysis over Cu/Ce modified ZSM-5. The influences of metal types, particles size of active center and interaction of Cu–Ce species on products distribution are elucidated. Methods Metal-modified ZSM-5 catalysts were prepared by negative pressure impregnation method. Catalytic fast pyrolysis and thermogravimetric experiments were conducted using Py–GC/MS and TG/MS for the qualitative and quantitative analysis of pyrolysis products. Results Morphology characterization indicated the interaction of Cu–Ce species facilitated the regulation of active center size into a nanoparticle scale. The final products were restricted to a carbon number of less than 9 over CuCe/ZSM-5. Cu–Ce modification increased the aliphatic content from 58.5 to 76.1%. Kinetic analysis revealed a remarkable reduction in activation energies during both the intermediate and final stages, where an average decrease of 30% was achieved. Conclusion The synergistic effects of Cu 0 and CeO x facilitated the formation of more short chain olefins by enhancing C–C bonds cleavage activity. Undesired polycyclic aromatic hydrocarbons (PAHs) were avoided by the optimal steric hindrance of CuCe/ZSM-5. Graphical Abstract
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JOURNAL OF POWER SOURCES
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2025
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IF 7.9
Jiaxin Huang,Huanbin Gou,Jinming Pan,Yuping Liu,Ming Nie,Bo Shang,Danmei Yu,Guangsheng Huang,Dingfei Zhang,Fusheng Pan
Within the domain of metal-air battery systems, developing the non - precious metal catalysts featuring extraordinary catalytic activity in oxygen reduction reaction (ORR) is crucial to the air-cathode. This work unveils a sol-gel engineered synthesis of La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 perovskite via the co-doping strategy, with targeted exploration of its electrochemical behavior and underlying mechanism in Zn-air and Mg-air battery systems. The perovskite La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 has a wealth of catalytically active ORR sites and a mesoporous architecture. The diffusion-limited current density of La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 successfully achieves a 1.2-fold enhancement relative to commercial Pt/C with a low H 2 O 2 yield of <0.27 %, underscoring its superior mass transport kinetics. The maximum power densities of La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 -based primary/secondary zinc - air batteries are 130 and 83 mW cm −2 , respectively, which are on a par with those of Pt/C - based Zinc - air batteries. Whereas, the open - circuit voltage and maximum power density of the primary magnesium - air battery fabricated with 10 wt% KCl as the electrolyte are 1.85 V and 52 mW cm −2 , respectively, which exhibit superiority over Pt/C catalysts. In combination with DFT analyses, the La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 perovskite emerges as a prospective ORR catalyst for metal-air battery realization.
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ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
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2025
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IF 6.1
Fangjing Xiao,Guibin Jiang,Duo Bu,Jianjie Fu,Xiaomei Cui,Qiangying Zhang
A porous aluminum–cerium (Al/Ce) composite oxide was innovatively synthesized via a one-step, template-free evaporation–pyrolysis route, enabling in-situ formation of sulfate-templated mesopores and dual-functional –OH/SO 4 2 ⁻ sites. Designed to address the severe ion interference of geothermal water, this bifunctional adsorbent achieved rapid, simultaneous removal of arsenic (As) and fluoride (F⁻) with high efficiencies (93.8 % As, 91.5 % F⁻) within 15 min. Maximum adsorption capacities reached 251 mg/g (As) and 297 mg/g (F⁻), following pseudo-second-order kinetics and Freundlich isotherms. Thermodynamic analysis confirmed spontaneous, endothermic chemisorption. Structural characterizations (FT-IR, XRD, XPS) revealed ion exchange and surface complexation mechanisms via formation of Al–F, Ce–F, and Ce–O–As bonds. Remarkably, in real geothermal matrices rich in competing ions, removal efficiencies exceeded 96 %, underscoring the composite's strong anti-interference performance. This study demonstrates a scalable, environmentally friendly strategy for fabricating robust, synergistic adsorbents tailored for complex wastewater treatment.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120584
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IF 7.2
Jian Wang,Kejia Lu,Wei Wang,Jianjun Yu,Yaqi Peng,Guanghua Xia,Guanjie Wang
Atomic defects in catalysts (such as vacancies, substituted atoms, or interstitial atoms) are the decisive factors in initiating low-temperature catalytic reactions. The study achieved the selective exposure of Mn-doped CeO 2 (111) crystal planes and facilitated the migration of oxygen species at the interface through the regulation of Mn and Ce precursors, thereby enhancing the low-temperature catalytic performance for chlorobenzene (CB). The Mn: Ce precursor ratio strongly influences activity; Mn 1 Ce 1 shows optimal performance with T 50 ≈ 142 ℃ and T 90 ≈ 192 ℃. Structural analyses confirm Mn incorporation into the CeO 2 lattice across multiple facets, optimizing Mn-O v -Ce interfacial sites, increasing surface acidity, and elevating oxygen‑vacancy (O v ) concentration (3.6 ×10 13 spins/g). CB was nearly completely mineralized to CO 2 at 240 ℃, while chlorine was mainly removed as HCl. Oxygen is crucial for the dynamic generation and cycling of O v , effectively replenishing the consumed adsorbed oxygen (O ads ) during catalysis, whereas the presence of water vapor causes competitive adsorption, reducing catalytic activity. In-situ DRIFTS, in-situ EPR, and DFT calculations demonstrated that surface O ads are the primary active oxygen species. CB trapped by O v is sequentially converted into intermediates (e.g., phenol and benzoquinone) and ring-opening products (e.g., maleic anhydride and formic acid) under the action of O ads , ultimately mineralizing into CO 2 . The Mn-doped CeO 2 (111) crystal facet exhibited the lowest CB adsorption energy (-2.4 eV), O v formation energy (1.1 eV), and HCl formation energy (-1.3 eV). Furthermore, Mn serves as a dechlorination site, effectively promoting C-Cl bond cleavage and inhibiting chlorine poisoning at CeO 2 interface.
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CHEMICAL ENGINEERING SCIENCE
·
2025
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IF 4.3
Wenbin Huang,Kaining Wang,Han Yang,Tianyu Bai,Yasong Zhou,Qiang Wei,Minghan Han
CO 2 hydrogenation to methanol emerges as a promising strategy, offering a dual advantage of carbon dioxide fixation and the production of a valuable liquid fuel and chemical feedstocks. However, its industrial application is limited by the high stability of the CO 2 molecule, resulting in low CO 2 conversion and methanol selectivity. In this work, a series of Ce-doped Cu-ZrO 2 catalysts were synthesized by an oxalic acid gel co-precipitation method, and the effect of Ce/Zr molar ratios on catalyst structure and catalytic performance were investigated. Comprehensive characterization techniques, including XRD, N 2 physical adsorption–desorption, HRTEM, H 2 -TPR, XPS, CO 2 /H 2 -TPD and DFT calculation were employed to analyze the influence of Ce doping on oxygen vacancy concentration, surface basicity distribution, electron transfer, and catalytic performance. The results demonstrate that the CC 0.4 Z catalyst (n(Ce)/n(Zr) = 0.4) forms a Ce 0.4 ZrO solid solution structure, significantly enhancing CuO dispersion and generating abundant Cu δ+ -Ce 0.4 ZrO interfacial sites and oxygen vacancies. These features synergistically promote CO 2 /H 2 adsorption and activation while stabilizing Cu + species. Under optimized reaction conditions (260 ℃, 3.0 MPa, 9000 h −1 ), the CC 0.4 Z catalyst exhibits outstanding performance: CO 2 conversion of 14.6 %, methanol selectivity of 74.1 %, and a methanol yield of 10.8 %. Compared to the unmodified catalyst, this represents an increase of 5.8 percentage points in CO 2 conversion and 6.3 percentage points in methanol yield, providing a novel catalyst design strategy for efficient CO 2 conversion.
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Journal of Materials Chemistry B
·
2016
·Vol. 4
·期 22
·3903-3910
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IF 4.872
Genxing Zhu,Ruibo Zhao,Yaling Li,Ruikang Tang
Multifunctional Gd,Ce,Tb co-doped β-tricalcium phosphate (TCP) porous nanospheres are prepared by a facile solvothermal strategy with trimethyl phosphate as the phosphorus source. The as-prepared nanomaterial (average diameter of 100 nm) has a multiple level pore size distribution with the specific surface area of 124.33 m2 g−1, which benefits drug loading. Its photoluminescent and magnetic multifunctions are realized by the co-doping of Gd3+, Ce3+ and Tb3+ ions, which make the nanomaterial promising for both fluorescence and magnetic resonance imaging techniques. Furthermore, the nanomaterial exhibits excellent cytocompatibility and a relatively high doxorubicin loading capacity as well as sustained pH-sensitive drug release behaviour. It is suggested that the Gd,Ce,Tb co-doped β-TCP porous nanospheres are promising for applications in the biomedical fields such as multifunctional drug delivery systems and tissue engineering scaffolds with bioimaging guidance.
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Applied Sciences-Basel
·
2021
·Vol. 11
·期 5
·2018
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IF 2.679
Yang Chen,Qi Tian,Yongsheng Tian,Jiawei Cui,Guanghui Wang
A mesoporous silica-supported molybdenum oxide catalyst with a cerium(Ce) modifier was prepared by in situ synthesis and used in a hydrogen peroxide (H2O2) system for the desulfurization of dibenzothiophene (DBT), benzothiophene (BT), and 4,6-dimethyldibenzothiophene (4,6-DMDBT) fuel oils. The catalytic performance of the catalyst was studied. The catalyst was characterized by Fourier Transform Infra-Red (FT-IR), X-ray diffraction (XRD), Brunner−Emmet−Teller (BET), and X-ray Photoelectron Spectroscopy (XPS). The influences ofm(catalyst)/m(fuel oil),v(H2O2)/v(fuel oil), reaction temperature, and reaction time were investigated. The catalyst had excellent catalytic oxidation desulfurization performance under moderate operational conditions. The catalytic performance was in the order DBT > 4,6-DMDBT > BT. The kinetic analysis results showed that the reaction was a pseudo first-order kinetics process and the apparent activation energies of DBT, BT, and 4,6-DMDBT were 46.67 kJ/mol, 56.23 kJ/mol, and 55.54 kJ/mol, respectively. The reaction products of DBT, BT, and 4,6-DMDBT were DBTO2, BTO2, and 4,6-DMDBTO2, respectively. The recycling experiments indicated that DBT, BT, and 4,6-DMDBT removal could still reach levels of 94.0%, 63.0%, and 77.9% after five cycles.
研究领域:
化学工程
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环境科学
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International Journal of Environmental Research and Public Health
·
2019
·Vol. 16
·期 8
·1439
·
IF 2.468
Yue Teng,Ke Yao,Wenbin Song,Yongjun Sun,Haoliang Liu,Zhiying Liu,Yanhua Xu
Cu-Mn-Ce@γ-Al2O3was prepared by incipient wetness impregnation and used to catalyze ozonation in a coal chemical wastewater-biotreated effluent. The preparation factors that considerably affected the catalytic performance of Cu-Mn-Ce@γ-Al2O3, specifically metal oxide loading percentage, calcination temperature, and calcination time, were examined. The catalyst was characterized by scanning electron microscopy, energy dispersive spectrometry, X-ray diffraction, and Brunauer-Emmett-Teller analysis. The optimal catalytic ozonation operating parameters, such as ozone dosage, catalyst dosage, pH, and reaction time, were also investigated. Results showed that an optimized catalyst consisted of 17.0% CuO, 3.0% MnO2, and 2.0% CeO2(wt.%). The optimal calcination temperature and calcination time were 600 °C and 5 h. The optimal catalytic ozonation operating parameters, including ozone dosage, catalyst dosage, pH, and reaction time, were 7, 80.0 mg/L, 20.0 mg/L, 7 and 50 min, respectively. The COD removal of biotreated effluent increased to 61% under these optimal operating conditions. Meanwhile, ozonation alone resulted in only 20% removal. This work proposes the use of easily available Cu-Mn-Ce@γ-Al2O3catalyst and might drive the advancement of catalytic ozonation for chemical wastewater purification.Keywords:catalyst;catalytic ozonation;coal chemical wastewater;advanced treatment
研究领域:
环境科学
·
化学工程
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Xixi Zhao,Pengheng Li,Min Lin,Xing Zhu
A “hydroxyl-transition metal synergistic” strategy was developed to enhance Cu-Ce oxygen carriers for chemical looping preferential oxidation (CL-PROX). Among synthesized MCuCe (M = Mn, Fe, Co) samples, MnCuCe exhibited superior performance. Mn doping strengthened strong interfacial interactions via oxygen vacancy-mediated charge compensation, yielding the highest surface Cu + (77.44%), Ce 3+ (20.94%), and oxygen vacancies (35.30%). Consequently, MnCuCe achieved >99% CO conversion at 180 °C with <3% H 2 consumption, showing no deactivation after 30 cycles. In situ FTIR verified that Cu + serves as the pivotal active site within a Mars-van Krevelen (MvK) mechanism. DFT calculations confirmed that the synergistic construction of stable M−Cu + −O v −Ce 3+ sites results in the most negative CO adsorption energy (−3.00 eV). This study provides a novel paradigm for designing high-performance CL-PROX oxygen carriers.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2026
·
IF 4.6
Li Ding,Jiayu Lin,Zhiqiang Wang,Aixue Jia,Changwu Cai,Zhong Xie,Yongde Yan
The recovery of cerium via molten salt electrolysis with the liquid zinc (Zn) cathode is considered a highly promising strategy for rare earth resource recycling. To reveal the electrochemical reduction of cerium (Ce) ions and the alloy formation process on the Zn electrode, in this work, multiple electrochemical methods were adopted to study the electrode reactions and thermodynamic properties during the Ce deposition process at high temperatures. A concentration-dependent test of the co-deposition reaction indicated that the alloying behaviour of reduced Ce was affected by ion concentration. The electrochemical results showed that four Ce Zn alloys were formed in the electrode reaction. The Gibbs free energy of alloy formation was determined. Furthermore, in order to understand the reaction kinetics on the liquid electrode and the thermodynamic behaviour of the reduced Ce in the electrode, the exchange current density and activity coefficient during electrodeposition were determined by Tafel analysis and coulometric titration, respectively. The temperature dependence of both exchange current density and activity coefficient was further revealed
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.9
Yifei Huang,Hongliang Dai,Hongye Bai,Weiqiang Fan
Biomass materials as an abundant renewable resource could replace traditional fossil fuels and non-renewable materials, providing a new solution to achieve sustainable development. In this paper, Ce-modified Co(OH) 2 /Cu 2 O composite catalysts were prepared by an electrodeposition method, and the CoOOH/CuOOH dual active sites were successfully obtained through an electrochemical reconfiguration strategy, and the experimental results showed that the incorporation of Ce induced the formation of high-valent Co and Cu species, which improved the activity of electrocatalytic HMF oxidation. At 0.55 V vs Hg/HgO, the HMF conversion reached 100%, the FDCA yield was 95.04% and the Faraday efficiency was up to 98.47%. These results confirm the effectiveness of Ce-based non-precious metal catalysts in electrochemical reconstruction strategies and demonstrate their potential application in the high-value conversion of biomass derivatives. This finding not only provides a solid research basis for the development of highly efficient catalysts, but is also expected to promote the development of related technological fields.
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