BIOSENSORS & BIOELECTRONICS
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2018
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IF 8.173
Hua Yu,Jing Han,Shangjie An,Gang Xie,Sanping Chen
Metal–organic frameworks (MOFs) as a new class of porous materials have attracted increasing attention in the field of biomimetic catalysis . This study firstly reports a mixed valence state Ce-MOF possessing intrinsic catalytic activity towards thionine (Thi), and its application in constructing an amplified electrochemical aptasensor for thrombin detection. As noticed, the novel catalytic process combines the advantages of 3D infinite extension of the Ce(III, IV)-MOF skeleton containing large amounts of catalytic sites and spontaneous recycling of the Ce(III)/Ce(IV) for electrochemical reduction of Thi, thereby presenting amplified electrochemical signals. To further improve the aptasensor performance, the high selectivity of proximity binding-induced DNA strand displacement and high efficiency of exonuclease III-assisted recycling amplification were incorporated into the assay. The aptasensor was employed to detect thrombin in complex serum samples, which shows high sensitivity, specificity, stability and reproducibility. This work offers an opportunity to develop MOF-based electrocatalyst as signal-amplifying tag for versatile bioassays and catalytic applications.
研究领域:
材料科学
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电化学
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生物传感器
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催化
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DOI
PubMed
高影响因子
TALANTA
·
2022
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IF 6.556
He Mei,Qing Wang,Jiahui Jiang,Xiaolei Zhu,Huili Wang,Shugen Qu,Xuedong Wang
Herein, glutathione-capped copper nanoclusters (CuNCs) and graphitic carbon nitride nanosheets (g-C 3 N 4 NSs) were synthesized by a facile one-pot chemical reduction and directly thermal pyrolysis following ultrasonic exfoliation approaches, respectively. The introduction of Ce(III) (Ce 3+ ) played dual functions in constructing a fluorescence-enhanced ratiometric nanoprobe (g-C 3 N 4 NSs-Ce 3+ -CuNCs), i.e., triggering aggregation-induced emission of CuNCs and conjugating g-C 3 N 4 NSs with CuNCs by virtue of electrostatic and coordination interactions. The as-fabricated nanohybrid displayed 460 and 625 nm dual-emitting peaks, attributing to the emission of g-C 3 N 4 NSs and CuNCs, respectively. Upon addition of H 2 O 2 , the 625 nm emission was dramatically quenched, whereas the 460 nm emission remained nearly unchanged, thereby causing obvious color changes from purple to blue under a 365-nm UV lamp. A ratiometric fluorescent assay, based on g-C 3 N 4 NSs-Ce 3+ -CuNCs, was devised for sensitive and visual detection of H 2 O 2 , which spanned the linear range of 2–100 μM with a detection limit of 0.6 μM. In the presence of glucose oxidase , the ratiometric nanoprobe could be simultaneously employed to detect glucose across the linear range of 1.6–320 μM with a detection limit of 0.48 μM. In milk and human serum samples, the fortified recoveries for H 2 O 2 and glucose by the nanoprobe were in the range of 95.5–103.6% with RSDs <3.8%. The real detection levels for glucose are consistent with those by a standard glucometer. As such, the ratiometric nanoprobe offers a promising methodology for several practical applications, such as point-of-care diagnosis and workplace health evaluations.
研究领域:
分析化学
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生物医学工程
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纳米技术
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DOI
高影响因子
CATALYSIS TODAY
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2021
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IF 6.766
Liangliang Zhang,Yang Feng,Huihui He,Yang Liu,Jiena Weng,Peng Zhang,Wei Huang
In this article, we report a series of hexanuclear rare-earth MOFs based on Ce (III) and 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin, namely Ce-PCN-224, with a new zln topology through linker induce strategy. Ce-PCN-224 exhibits permanent porosity, high water and thermal stabilities, and the ability to adsorb dye molecules in the aqueous environment. Moreover, after post-metallation with Fe, Co, and Ni, Ce-PCN-224(Fe) and Ce-PCN-224(Co) were proved to be efficient heterogeneous catalysts for the cycloaddition of CO 2 with epoxides, attributed to the combination of multiple Lewis acidic sites.
研究领域:
材料科学
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化学工程
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环境科学
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催化
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DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Xuwen Chen,Peixin Wang,Fei Peng,Zhou Zhou,Michael Gatheru Waigi,Wanting Ling
Substituted polycyclic aromatic hydrocarbons (SPAHs) are being intensively investigated, considering their high toxicity. Additionally, the mechanism of the effect of substituents on the removal of SPAHs and the activation of Ce(III) ions on peroxymonosulfate (PMS) have not been explored. Here we evaluated the removal efficiency of SPAHs in the oxidation system constructed by Ce(Ⅲ) ions and PMS, with emphasized the effect of substituents on SPAHs degradation. Ce(Ⅲ) has high catalytic performance for PMS, and the degradation percentage of all pollutants was higher than 92%. The significantly negative correlation between the reaction rate constants of SPAHs and the highest occupied molecular orbital-the lowest unoccupied molecular orbital gap, confirms that substituents lead to the differences in the degradation of SPAHs. The generation of reactive oxygen species (SO 4 •− , • OH, and 1 O 2 ) is based on the electron transfer between Ce(Ⅲ) and PMS, and the contribution of ROS to substituted naphthalene varies due to the role of substituents. The Ce(Ⅳ)/Ce(Ⅲ) cycle accelerates the activation of PMS. Based on the transformation products and condensed Fukui function, the possible degradation pathways are inferred. In addition, inorganic anions and organic matter have little effect on the Ce(Ⅲ)/PMS system, which is a prerequisite for applying this system to real-world waste-water for SPAHs removal. This work demonstrates a new model of the degradation mechanism of SPAHs in the Ce(Ⅲ)/PMS system.
研究领域:
环境化学
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水处理
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污染物降解
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催化
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jiaojie He,Qingwang Cai,Ziyi Kang,Jingxin Zhang,Huan Tang,Tinglin Huang
Research on inorganic metal coagulants has largely focused on the Al, Fe, Ti and Zr-based salts, leaving insufficient studies on the metal Ce. This study first attempted to conduct an in-depth investigation into the coagulation effect of Ce-based reagents with different valence states. The CCl was a pure Ce(III)-based salt, while Ce(IV)/Ce(III) in CAN equaled 2.7/1. The results demonstrated that CAN possessed far superior capability of turbidity removal compared with CCl, which was on par with polyaluminum chloride (PAC). And its ability to remove organic matter even surpassed that of PAC. Furthermore, CAN exhibited more remarkable and stable performance across a broad pH range. Mechanism studies confirmed that the Ce(III) had the strongest organic ligand complexing ability but insufficient hydrolysis ability, leading the complex re-stabilized in solution. Whereas, the merits of Ce(IV) was based on the following distinctive properties: (1) the high positive charge, with zeta potential even close to that of PAC under acidic condition, (2) the readily formed hydrolysis products owning film-like structure to enhance sweep flocculation, (3) the high coordination number to offer abundant reaction sites to balance the three effects, electric neutralization, complexation, and sweeping, to fully exploit their respective advantages. Thus, the above three effects were combined to achieve the stable coagulation efficiency in CAN containing both Ce(IV) and Ce(III), which might be insufficient or competitive in PAC or CCl. The clarification of the coagulation mechanisms is conducive to better developing Ce-based coagulants and may offer valuable insights into finding more suitable metal-based reagents.
研究领域:
环境科学
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化学工程
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Mei Li,Zhixiang Shan,Rugeng Liu,Meng Zhang,Wei Han
The electrochemical investigation of Ce(III) was carried out on W, Sn film and liquid Sn electrodes in LiF-LiCl eutectic by a variety of electrochemical methods. It was determined that Ce(III) was reduced to metallic Ce on W electrode via a one-step three-electron transfer, which was a reversible process controlled by diffusion. The diffusion coefficient of Ce(Ⅲ) in LiF-LiCl eutectic was estimated by CV and CP, while the diffusion activation energy was calculated to be 20.86 kJ mol −1 and 20.95 kJ mol −1 , respectively. The electrochemical behavior of Ce(Ⅲ) was studied on Sn film electrode by CV and OCP. Eight alloy compounds Ce x Sn were obtained due to the underpotential deposition of Ce on the pre-deposited Sn film electrode. The activities of Ce in Ce x Sn and standard Gibbs formation energies of Ce x Sn were evaluated, respectively. Moreover, on Sn film electrode, the electrochemical extraction of Ce was performed at −1.5 V. XRD, SEM and EDS results exhibited the formation of CeSn 3 and Ce 2 Sn 5 . On liquid Sn electrode, the reduction current of Ce appeared at about −1.2 V and reached a peak at about −1.4 V. The electrochemical extracting Ce was also conducted on liquid Sn electrode at −1.3 V and CeSn 3 was obtained. The extraction rates and efficiencies of Ce on liquid Sn electrode were estimated using ICP-AES at different durations. It was found that as the extraction proceeded, the extraction rate decreased, while the extraction efficiency increased. The extraction efficiency reached over 98 % after electrolysis for 10 h.
研究领域:
冶金学
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电化学
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DOI
高影响因子
Small
·
2023
·Vol. 19
·期 49
·2304644
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IF 13.3
Ping Lu,Zhaoyang Qi,Jie Chen,Changshen Ye,Ting Qiu
High-efficiency adsorption of aromatic sulfur-containing compounds from liquid hydrocarbon fuels over metal-organic frameworks (MOFs) is challenging because of inert metal sites. A new method, the Ce-enhanced modulation of MOFs’ microenvironment, is proposed to modulate the –COO···Cu(II)– coordination microenvironment of Hong Kong University of Science and Technology (HKUST-1) using Ce(III) as a molecular scalpel for fabricating abundant high-efficiency Cu(I) and Cu-coordination-unsaturated sites and improving the pore structures around adsorptive sites. The optimal CH-250 thus exhibits adsorptive capacities for 20.2, 28.0, and 58.3 mg S g –1 of thiophene, benzo-thiophene, and dibenzothiophene, respectively, which are superior to most reported MOFs, zeolites, and nanoporous carbons. The constructed Cu(I) sites show stronger affinity for dibenzothiophene (−0.86 eV) than the initial Cu(II) (−0.74 eV) for out-of-plane adsorption. Further, they are far stronger in-plane adsorption interactions in DBT/CH-250 (−0.90 eV) than those in DBT/HKUST-1 (−0.37 eV). Thus, molecular engineering for modulating the coordination microenvironment of MOFs shows great potential for adsorption desulfurization.
研究领域:
材料科学
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能源化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xinyu Yang,Bing Hou,Mingjing Shi,Muhammad Akram,Xinxin Li,Lei Wang,Jingwen Pan
Excessive fluoride (F − ) in water environment is a widespread concern, and economical and efficient adsorption is widely used defluorination technology. In this study, a series of cerium-based adsorbents (Ce@C) with different structural properties were synthetized by adjusting the calcination conditions to explore their effect on the F − adsorption capacity of Ce@C and intrinsic mechanism. Results indicated that the best performing Ce@C had the maximum adsorption capacity (340.71 mg/g) and a wide pH working range (2–12). The adsorption process of F − conformed to the pseudo-second-order model and the Temkin model, proving that F − adsorption onto Ce@C was mainly dominated by chemisorption. Different calcination conditions altered the content of Ce(III) and oxygen vacancies in Ce@C, and their contents exhibited a significant effect on the F − adsorption performance of Ce@C, which showed a strong positive correlation (R 2 = 0.982 and 0.933). Density functional theory (DFT) calculations further proved that the presence of Ce(III) and oxygen vacancies could provide richer coordination numbers to promote the complexation of F − and Ce@C. This work re-reveals the F − adsorption behavior and intrinsic mechanism onto cerium-based adsorbents, and also provides a theoretical basis for the subsequent design of cerium-based adsorbent materials for defluorination.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Jiaqi Shen,Yuxin Gu,Yue Yang,Jiaojie He,Chuanliang Zhao,Yan Sun,Junfeng Li,Liwei Yang
The metal organic frameworks (MOFs) are considered as the effective adsorbents for phosphate removal , while their ultrafine powders limit their practical application. In this study, we fabricate two chitosan (CS) gel beads added with different cerium-based MOFs and coated with PDA for phosphate adsorption. The MOFs doped in beads are CM1 and CM2, in which the Ce(III)/Ce(IV) ratio is 0.36 and 1.46, indicating CM2 is Ce(III) dominated and more suitable for phosphate removal. However, during the process of preparing gel beads, the mixture of chitosan and CM1/CM2 are added drop-by-drop to NaOH solution, leading to the decrease of Ce(III) contents in both of the two beads on account of oxidization. On this basis, in order to improve the phosphate uptake performance and enhance the mechanical strength, polydopamine (PDA) is applied to be coated on the outside. The adsorption capacities of CS-CM1 and CS-CM2 are no more than 20 mg/g higher than that of pure CS, which is also quite equal with the phosphate uptake of CS@PDA (63 mg/g). Due to the reduction of PDA, the content of Ce(III) increasing evidently in the two adsorbents. The maximum phosphate adsorption capacities are 146.8 mg/g and 114.8 mg/g for CS-CM1@PDA and CS-CM2@PDA, respectively. CS-CM2@PDA exhibits the largest treatment volume of ∼1166 BV in the fix-bed column study, much higher than that of CS-CM1@PDA (976 BV). The main reason is that Ce(III) could form binding with phosphate through ligand exchange and precipitation. Those inner-sphere interactions are much stronger than the electrostatic attraction between Ce(IV) and phosphate. Thus, due to this strong affinity, CS-CM2@PDA possessing a higher content of Ce(III) can capture phosphate more easier at low concentration. In summary, owing to reduction of PDA, the Cerium-based MOFs are successfully introduced in CS to realize excellent phosphate removal and exhibit a great prospect in application.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Chao Wang,Jinshan Zhang,Xinxin Zhu
Incorporation of lanthanide atom into the titanium−oxo cluster structure is an effective strategy for exploring novel photoelectrode materials. Herein, we synthesized and characterized three lanthanide-doped titanium−oxo clusters (Ln-TOCs): [Ti 4 La(μ 3 -O) 3 (O i Pr) 2 (C 6 H 5 COO) 11 ]·3CH 3 CN ( 1 ), [Ti 4 Eu 2 (μ 3 -O) 4 (acac) 2 (C 6 H 5 COO) 13 ] ( 2, acac = acetylacetonate), and [Ti 7 Ce(μ 2 -O) 2 (μ 3 -O) 5 (O i Pr) 2 (C 6 H 5 COO) 15 ]·CH 3 CN ( 3 ). These Ln−TOCs display strong UV-light absorption and extended visible light absorption, which can be ascribed to the doping of lanthanides and benzoates. As electrode precursors for photoelectric responses, these Ln doped clusters exhibit clear photocurrent responses. Moreover, cluster 3 shows the highest photocurrent intensity because of Ce(IV)/Ce(III) redox reaction . This work not only enriches the Ln−TOCs family, but also promotes the development of novel titanium-based photoelectric active materials.
研究领域:
材料科学
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化学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
·
IF 9
Xuepeng Wang,Yongde Yan,Yanghai Zheng,Jing Pan,Qingguo Zhang,Yun Xue,Milin Zhang,Kai Zhu
The efficient recovery of the radioactive elements uranium (U) and plutonium (Pu) from radioactive calcium fluoride slag is of great significance for the sustainable utilization of nuclear resources and environmental protection. Molten salt electrolysis technology based on pyrometallurgy, characterized by a streamlined process and the absence of secondary waste generation, is widely regarded as the most promising approach for the treatment of such radioactive residues. However, the physicochemical properties of molten salts and the underlying electrode reaction mechanisms under high-temperature conditions remain insufficiently understood and lack systematic investigation. In this study, by comparing the electrochemical parameters and physical-chemical properties of different molten salt systems, it was found that the CaCl 2 -CaF 2 molten salt system is a suitable choice for treating radioactive calcium fluoride waste. Due to the high radioactivity of plutonium (Pu), cerium (Ce) was employed as a chemical analogue of plutonium to investigate the electrochemical extraction of actinides in CaCl 2 -CaF 2 molten salt systems. The electrochemical behavior of Ce(III) on a W electrode and related kinetic parameters were investigated. Electrochemical analysis reveals that Ce(III) undergoes a quasi-reversible and diffusion-controlled reduciton on inert W electrode. The process shows distinct adsorption and desorption, likely attributable to the coexistence of Cl − and F − ions. To better extract Ce, nickel (Ni) ions were introduced into the molten salt. The co-deposition behavior of Ce(III) and Ni(II) on the W electrode was investigated by electrochemical methods. The thermodynamic parameters of Ce-Ni intermetallic compounds at the experimental temperature were calculated. The results show that CeNi 5 has a distinct thermodynamic advantage in formation. X-Ray Diffraction (XRD)， Scanning Electron Microscopy (SEM) and Energy Dispersive Spectrometer (EDS) characterization analyses confirmed the successful extraction of Ce in the form of the CeNi 5 intermetallic compound.
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高影响因子
ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Jiayi Chen,Wei Han,Yixuan Cai,Xudong Wang,Rugeng Liu,Meng Zhang,Mei Li,Weiqun Shi
Studied the electrochemical behavior of Ce(III) ions on Bi film electrodes and liquid Bi electrode. • Studied the effect of Ce (III) ions on the electrochemical behavior of UO 2 2+ at Bi film electrode and liquid Bi electrode. • Ce(III) ions and UO 2 2+ ions were separated via potentiostatic and galvanostatic electro-deposition on a liquid Bi electrode. • Found that better separation of Ce(III) ions and UO 2 2+ can be achieved at relatively low potentials. • The extraction efficiency and separation efficiency were calculated for electrolytic separation at lower potentials. To achieve the separation of uranium and fission products, a liquid Bi electrode was employed to study the electrochemical separation of the fission product Ce(III) ions and UO 2 2+ ions. The electrochemical reduction mechanism of Ce(III) ions was investigated at a Bi film electrode using three electrochemical testing methods: CV, SWV and CP, The results showed that a series of reduction peaks related to the formation of Ce-Bi intermetallic compounds appeared at potentials more positive than the reduction potential of Ce(III) ions. Meanwhile, the electro-reduction mechanism of Ce(III) ions at a liquid Bi electrode was also explored. A reduction peak associated with the formation of Bi-Ce solid solution was recorded. The impacts of Ce(III) ions on the electro-reduction mechanism of UO 2 2+ at a Bi film electrode were examined, and found that the electro-reduction of UO 2 2+ was two-step single-electron transfer process before and after the addition of Ce(III) ions. Furthermore, electrochemical separation of UO 2 2+ and Ce(III) ions was performed at a liquid Bi electrode at -0.7 V/-1.3 mA cm -2 . XRD results confirmed that the separation product included not only UO 2 , but also Ce 2 O 3 and Bi-Ce alloy. Nevertheless, constant potential electrolysis experiment was conducted at the potential of -0.3 V, and the product analyzed by XRD, SEM and EDS demonstrated that only spherical UO 2 with a regular morphology was obtained. The separation factor between UO 2 2+ and Ce(III) ions and extraction efficiency of UO 2 were calculated to be 34.4 and 97.76 %, respectively. Download: Download high-res image (184KB) Download: Download full-size image
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高影响因子
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