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POLYMER SCIENCE SERIES B · 2016 ·Vol. 58 ·期 5 ·594-600 · IF 0.737

Preparation and characterization of luminescent cellulose–Y4Si2O7N2:Ce4+ hybrid hydrogels

Wang Yan,Wei Nuo,Feng Qingling,Li Sha,Yang Chang,Liu Zhiqiang,Zhang Wenming,Li Qing

Novel luminescent bio-based hydrogels comprising cellulose and Y 4 Si 2 O 7 N 2 :Ce 4+ (YC) were prepared in an alkali/urea aqueous system using epichlorohydrin as a cross-linker. The structure, characteristics and properties of the hydrogels were investigated by various techniques, including FTIR spectroscopy, wideangle X-ray diffraction, scanning electron microscopy, etc. The results showed that when the content of YC was less than 0.05 g, the YC particles were tightly embedded in the macro porous of cellulose matrix, which not only supplied cavities for YC immobilization, but also supplied the pore wall to protect the structure and character of YC. Hence, the cellulose–YC hybrid hydrogels exhibited strong cyan fluorescence under a UV lamp. However, excess of YC particles were enshrouded in the cellulose matrix resulted in smaller pores, weaker fluorescence intensity, lower swelling ratio and higher mechanical properties.

研究领域: 材料科学 · 生物材料
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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 30 ·12962-12966 · IF 3.288

Convenient and sensitive colorimetric determination of alendronate sodium with Ce4+-triggered oxidation of TMB

Jing Sun,Rui Wang,Meng Xia,Shuyun Zhu,Xian-En Zhao

As alternatives to nanozymes, some metal ions have been used in chemical/biochemical sensors owing to their facile acquisition avoiding tedious preparation and purification. Ce4+ has been reported to possess oxidase-like activity. Ascribed to its strong oxidative ability, Ce4+ can trigger the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to its blue product oxTMB without the requirement of H2O2. When ALDS is added, the oxidation ability of Ce4+ can be reduced because of the redox reaction between Ce4+ and ALDS. The absorbance intensity ascribed to oxTMB decreases followed by the fading of the solution. On the basis of such a mechanism, a simple method is proposed for monitoring ALDS in two linear ranges of 0.1–10.0 μM and 10.0–60.0 μM. The detection limit is low to 0.05 μM. Furthermore, this method exhibits great potential for ALDS detection in real biological body fluids and pharmaceutical samples.

CAS / MDL: 13590-82-4 54827-17-7
研究领域: 分析化学 · 药物分析
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Surfaces and Interfaces · 2024 · IF 5.7

Accelerating Ce3+/Ce4+ Conversion in CeO2 via Mn doping to Endow Scaffolds with Chemodynamic Therapy Properties

Cijun Shuai,Kangdong Wang,Shuping Peng,Jun Zan,Jiang Xiao,Shun Hu,Qi Zhong

CeO 2 nanozymes have garnered significant attention in chemodynamic therapy due to their peroxidase-like activity and ability to deplete glutathione. However, their catalytic efficiency is constrained by the low conversion rate of Ce 3+ /Ce 4+ . To overcome this limitation, the electron transfer was accelerated by introducing the transition metal Mn atom as a valence electron donor through lattice charge transfer. In detail, we introduced Ce 1-x Mn x O 2 into the poly-L-lactic acid (PLLA) scaffold fabricated by selective laser sintering. The conversion from Ce 3+ to Ce 4+ promoted the decomposition of H 2 O 2 within the tumor microenvironment to generate hydroxyl radicals with high oxidative activity, consequently inducing oxidative stress. The conversion from Ce 4+ to Ce 3+ depleted intracellular antioxidant glutathione, disrupting redox balance in tumor cells. This continuous redox cycle ultimately triggered apoptosis in tumor cells. Using a first-principles Hubbard-corrected approximate density-functional method, the analysis of the electron band structure revealed the presence of donor energy levels within the bandgap of Ce 1-x Mn x O 2 , enabling electron transfer channels around 0.645 eV. Electrochemical experiments confirmed that Ce 0.8 Mn 0.2 O 2 significantly reduced the activation overpotential from 0.907 V to 0.646 V, enhancing its redox capacity. As a result, the scaffold exhibited a threefold increase in tumor-killing rate. These findings highlight the immense potential of CeO 2 nanozymes in enhancing chemodynamic therapy for effective tumor treatment.

研究领域: 生物医学工程 · 肿瘤治疗学
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CORROSION SCIENCE · 2024 · IF 7.4

Thermal cycling behavior of Yb3+-Ce4+ co-doped La2Zr2O7-based TBCs: Experimental and theoretical research

Pengsen Zhao,Haizhong Zheng,Guifa Li,Yongxiang Geng,Yixin Xiao,Hongbo Guo,Gang Wang,Shixian Zhao,Ping Peng

The thermal cycling behavior of Yb 3+ -Ce 4+ -La 2 Zr 2 O 7 /YSZ (LYZCO/YSZ) TBCs was systematically investigated via experiment and first-principles calculation. Results suggest that ceramic grain boundary cracking is the root cause of LYZCO/YSZ TBCs thermal cycle failure. Compared to La 2 Zr 2 O 7 /YSZ TBCs, LYZCO/YSZ TBCs own an outstanding thermal cycle life at 1100 ℃, which is attributed to LYZCO's higher TEC (10.431×10 −6 /K, 1100 ℃) and lower thermal conductivity (1.299 W/(m·K), 1100 ℃). Furthermore, Griffith's separation work of the LYZCO/YSZ interface is merely −0.576 J/m 2 , implying that the LYZCO/YSZ TBCs are particularly prone to cracking at this interface. Weakly bonded La-O is the first site at this interface cracking.

研究领域: 材料科学 · 计算物理学
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JOURNAL OF MATERIALS SCIENCE · 2022 ·Vol. 57 ·期 28 ·13541-13559 · IF 4.682

Bifunctional modulation of Ce4+ doping for ZnWO4 morphological structure and bandgap width to enhance photocatalytic degradation and electrochemical energy storage

He Geping,Wang Di,HuangFu Huijun,Zhang Cunshe,Zhang Ben,Mi Yuanmei,Zheng Donghao

ZnWO 4 nanomaterials are gaining attention as a kind of multifunctional material in the field of electrochemical energy storage and photocatalysis. However, the controllable adjustment of their nanomorphology and bandgap width limit their wide application. So the nanostructured bifunctional Zn 1− x Ce x WO 4 ( x  = 0.020, 0.022, 0.030) with tunable nanomorphology and bandgap width were prepared by a simple one-step hydrothermal method in this work. On the one hand, the microscopic morphology of the Zn 1− x Ce x WO 4 was changed from clusters to nanosheets with the addition of Ce 4+ . On the other hand, the doping of Ce 4+ generated oxygen vacancies and formed defect states in the ZnWO 4 semiconductor, reducing the energy bandgap width. Zn 1− x Ce x WO 4 ( x  = 0.022) with the optimal doping ratio (nCe/(nCe + nZn) = 0.022) obtained a specific capacitance of 267.091 F g −1 at a current density of 1 A g −1 and an electrolyte of 6 M KOH, which is 3.7 times as great as the specific capacitance of ZnWO 4 (70.545 F g −1 ). In addition, the catalytic efficiency of Zn 1− x Ce x WO 4 ( x  = 0.022) for Rhodamine B (RhB) reached 99.541% in 4.5 h. The doping of Ce 4+ can achieve the dual modulation of the morphology and bandgap width of ZnWO 4 , thus enhancing the electrochemical performance and photocatalytic degradation performance of ZnWO 4 . Graphical abstract

研究领域: 材料科学 · 环境科学 · 电化学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2022 · IF 4.831

Nitrogen and boron co-doped carbon dots as a novel fluorescent probe for fluorogenic sensing of Ce4+ and ratiometric detection of Al3+

Xin Li,Liuxi Zhao,Yuhan Wu,Ao Zhou,Xuanfeng Jiang,Yuan Zhan,Zhengguang Sun

Carbon dots have been widely focused on the field of metal ion detection due to their excellent optical property. Herein, novel orange fluorescent nitrogen and boron co-doped carbon dots (NB-CDs) are obtained by one-pot solvothermal using p-phenylenediamine and boric acid as raw materials. The NB-CDs exhibit excitation-independent emissions and the maximum emission wavelength is 597 nm at 420 nm excitation. The fluorescence can be quenched by Ce 4+ effectively and selectively, and the detection range of Ce 4+ is gained from 0.14 to 180 μM with a detection limit of as low as 0.14 μM. Furthermore, Al 3+ can also recombine with NB-CDs surface functional groups, which shows a detection range from 1.07 to 100 μM and a detection limit of as low as 1.07 μM, accompanied with a blue-shift to 527 nm.

研究领域: 分析化学 · 材料科学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2019 · IF 2.931

Synthesis and spectral analysis of fluorescent probes for Ce4+ and OCl− ions based on fluorescein Schiff base with amino or hydrazine structure: Application in actual water samples and biological imaging

Fanyong Yan,Keqing Fan,Tengchuang Ma,Jinxia Xu,Jie Wang,Cong Ma

Two Schiff base fluorescein probes (FDA, FDH) based on fluorescein-aldehyde and nitroaniline derivatives were synthesized. The effects of amino and hydrazine substituents in fluorescein backbones were examined via fluorescence and absorbance spectra. In the presence of Ce 4+ , the fluorescence of FDA was quenched due to the ligand to metal charge transfer (LMCT). Hypochloric acid can react with the C N bond, and blocking the photo induced electron transfer (PET) of FDH leads to enhancement of the fluorescence. FDA showed detection limits for Ce 4+ and OCl − as low as 63 nM in concentration range of 0–4 μM. FDH showed detection limits for OCl − as low as 0.8 μM in concentration rang 0–100 μM. Polyvinylidene fluoride (PVDF) membrane containing the probes was prepared for the real-time qualitative detection of Ce 4+ and OCl − in real water samples. The probes were successfully applied to biological imaging in vascular smooth muscle cells (VSMCs) and are expected to find applications in biosensing.

研究领域: 分析化学 · 生物化学 · 环境科学
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Journal of the Taiwan Institute of Chemical Engineers · 2018 · IF 3.849

Synthesis of glycerol carbonate from glycerol and diethyl carbonate over CeO2-CdO catalyst: The role of Ce4+ doped into CdO lattice

Yuanfeng Wu,Xianghai Song,Jiahui Zhang,Shuai Li,Xinghui Yang,Huazheng Wang,Ruiping Wei,Lijing Gao,Jin Zhang,Guomin Xiao

A series of Ce 1- x Cd x O mixed oxide catalysts prepared by co-precipitation method were tested for synthesis of glycerol carbonate (GC) from glycerol and diethyl carbonate (DEC). The microstructural and physicochemical properties of the bimetal catalysts were characterized by XRD, SEM, TEM, XPS, CO 2 -TPD, N 2 -adsorption, TG-DSC and 1 H NMR. The results show that the spherical particles of CdO were uniformly dispersed on the surface of lamellar CeO 2 . Besides, a noticeable increase was observed in the moderate basic sites concentration, because more oxygen atoms were adsorbed on the bimetal sample surface which was attributed to Ce 4+ doped into CdO lattice. The Ce 0.7 Cd 0.3 O sample annealed at 500 °C was observed with the highest catalytic activity. 96.84% of glycerol conversion and 100% selectivity to GC were obtained over this catalyst under the optimized conditions (5 wt.% catalyst of glycerol, 90 °C, 180 min, glycerol/DEC molar ratio of 1:3). Besides, it was found that the conversion of glycerol carbonate was synergistically accelerated by the moderate and strong basic sites.

研究领域: 催化化学 · 材料科学 · 绿色化学
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ACS Nano · 2023 · IF 17.1

Boosting CO2 Electroreduction to C2H4 via Unconventional Hybridization: High-Order Ce4+ 4f and O 2p Interaction in Ce-Cu2O for Stabilizing Cu+

Yanfei Sun,Jiangzhou Xie,Zhenzhen Fu,Huiying Zhang,Yebo Yao,Yixiang Zhou,Xiaoxuan Wang,Shiyu Wang,Xueying Gao,Zheng Tang,Shuyuan Li,Xiaojun Wang,Kaiqi Nie,Zhiyu Yang,Yi-Ming Yan

Efficient conversion of carbon dioxide (CO2) into value-added materials and feedstocks, powered by renewable electricity, presents a promising strategy to reduce greenhouse gas emissions and close the anthropogenic carbon loop. Recently, there has been intense interest in Cu2O-based catalysts for the CO2 reduction reaction (CO2RR), owing to their capabilities in enhancing C–C coupling. However, the electrochemical instability of Cu+ in Cu2O leads to its inevitable reduction to Cu0, resulting in poor selectivity for C2+ products. Herein, we propose an unconventional and feasible strategy for stabilizing Cu+ through the construction of a Ce4+ 4f–O 2p–Cu+ 3d network structure in Ce-Cu2O. Experimental results and theoretical calculations confirm that the unconventional orbital hybridization near Ef based on the high-order Ce4+ 4f and 2p can more effectively inhibit the leaching of lattice oxygen, thereby stabilizing Cu+ in Ce-Cu2O, compared with traditional d–p hybridization. Compared to pure Cu2O, the Ce-Cu2O catalyst increased the ratio of C2H4/CO by 1.69-fold during the CO2RR at −1.3 V. Furthermore, in situ and ex situ spectroscopic techniques were utilized to track the oxidation valency of copper under CO2RR conditions with time resolution, identifying the well-maintained Cu+ species in the Ce-Cu2O catalyst. This work not only presents an avenue to CO2RR catalyst design involving the high-order 4f and 2p orbital hybridization but also provides deep insights into the metal-oxidation-state-dependent selectivity of catalysts.

CAS / MDL: 298-14-6
研究领域: 电化学 · 材料科学 · 催化 · 可再生能源 · 环境科学
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SENSORS AND ACTUATORS B-CHEMICAL · 2020 · IF 7.1

Graphene quantum dots combined with the oxidase-mimicking activity of Ce4+ for ratiometric fluorescent detection of Ce4+ and alendronate sodium

Meng Xia,Xian-En Zhao,Jing Sun,Zhenjia Zheng,Shuyun Zhu

A simple ratiometric fluorescent sensing system for Ce 4+ and alendronate sodium (ALDS) detection is developed with graphene quantum dots (GQDs) combined with the oxidase-mimicking activity of Ce 4+ . As oxidase-mimicking, Ce 4+ can catalyze the oxidization of o -phenylenediamine (OPD) directly without the requirement of H 2 O 2 . The oxidation product (oxOPD) not only exhibits a strong emission at 562 nm but also quenches the fluorescence of GQDs at 444 nm significantly through inner filter effect (IFE). Due to its strong oxidative ability, Ce 4+ can also oxidize ALDS. Thus, ALDS can inhibit the oxidization of OPD by Ce 4+ . The fluorescence at 444 nm can be protected from quenching while that at 562 nm decreases. Thus, a ratiometric fluorescent strategy for quantitative analysis of Ce 4+ and ALDS has been developed. The ratiometric sensing platform exhibits a high sensitivity with the detection limits of 1.0 μM and 33 nM for Ce 4+ and ALDS, respectively. This strategy can detect Ce 4+ and ALDS in practical samples with satisfactory recoveries.

研究领域: 分析化学 · 生物医学工程
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2020 · IF 4.939

Kinetics and mechanistic studies of methane dry reforming over Ca promoted 1Co–1Ce/AC-N catalyst

Yinghui Sun,Guojie Zhang,Haizhu Cheng,Jun Liu,Guoqiang Li

The mechanism and kinetic features of dry reforming with methane (DRM) over Ca promoted 1Co–1Ce/AC-N catalyst was investigated. The mechanistic pathway studies have conducted by FTIR and XPS analysis, structure-activity correlations demonstrated the CH 4 and CO 2 could adsorb on catalyst active sites and generate intermediate CH x , OH and CH x O, continue to generate CO and H 2 and then desorbed from active sites. Moreover, CH 4 could also oxidized by Ce 4+ and CO 2 reduced by Ce 3+ , the same content of Ce 4+ and Ce 3+ on promoted catalyst greatly improved the reaction rate. The kinetic of dry reforming with methane was examined for temperature between 650 and 850 at 800 °C. The research was carried out by changing the CH 4 /CO 2 ratios between 0.3 and 3.0. The obtained experiment data were fitted by three typical kinetic models (Power Law, Eley-Rideal and Langmuir-Hinshelwood), the fitting results demonstrated that the best prediction of reforming rates can provided by Langmuir-Hinshelwood model for the reaction temperatures between 650 and 800 °C. Moreover, activation energies of methane and carbon dioxide consumption were −117 and −47 kJ/mol, indicating that much higher energy barrier is needed for methane activation compared to carbon dioxide.

CAS / MDL: 206996-60-3 108-78-1
研究领域: 化学工程 · 催化科学
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2021 · IF 4.098

Ce4+-triggered cascade reaction for ratiometric fluorescence detection of alendronate

Meng Xia,Fengjin Shi,Yinghui Xia,Jing Sun,Xian-En Zhao,Shuyun Zhu

A ratiometric fluorescence assay for alendronate (ALDS) has been designed with Ce 4+ -triggered cascade chromogenic reaction. This strategy involves three processes: (1) Ce 4+ oxidizes ascorbic acid (AA) into dehydroascorbic acid (DHAA), which then condenses with o -phenlenediamine (OPD) to generate fluorescent 3-(dihydroxyethyl)furo[3,4- b ] quinoxaline-1-one (DFQ), presenting the maximum emission at 434 nm; (2) As oxidase-mimics, Ce 4+ can oxidize OPD into fluorescent 2,3-diaminophenazine (DAP) which shows a strong emission at 568 nm; (3) ALDS inhibits the oxidation ability of Ce 4+ towards OPD, thus inhibiting the generation of DAP. Accordingly, a homogeneous ratiometric fluorescence system with dual emission comes into being and the presence of ALDS can change the fluorescence intensity ratio obviously. With F 434 / F 568 as readout, ALDS can be detected sensitively with the detection limit of 30 nM. Moreover, this ratiometric method was used to analyze ALDS in both human serum and pharmaceutical samples.

研究领域: 分析化学 · 药物分析 · 生物医学
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