JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2026
·
IF 4.6
Cheng Xiong,Liyin Bu,Xue Bai,Yongzhong Fu,Quan Wang
Cts/Ce-UiO-66 was developed for sensitive ratiometric detection of Hg 2+ . • Intrinsic Ce 4+ /Ce 3+ redox couple in MOF provides a stable reference signal. • Chitosan coating promotes Hg 2+ enrichment and stabilizes the modified film. • The sensor showed a 3.73 nM LOD and 95.0%–105.3% recovery in pond water. Mercury pollution remains a serious environmental concern because of its toxicity, persistence, and bioaccumulation in aquatic environments. Herein, a ratiometric electrochemical sensor for Hg 2+ detection was developed using a chitosan/Ce-UiO-66 (Cts/Ce-UiO-66) composite. Ce-UiO-66 was used as a redox-active sensing scaffold. Its porous framework may provide accessible interfacial sites that may contribute to Hg 2+ accumulation, while the intrinsic Ce 4+ /Ce 3+ redox response provides a built-in electrochemical signal for internal normalization under controlled measurement conditions. Chitosan was introduced as a film-forming matrix. The amino and hydroxyl groups of chitosan may contribute to Hg 2+ interfacial preconcentration, while the polymer matrix improves the stability of the modified film. The integration of the proposed Cts-assisted Hg 2+ interfacial accumulation and the intrinsic Ce-related normalization signal enabled ratiometric Hg 2+ quantification. Under optimized differential pulse voltammetry conditions, the sensor exhibited a linear response toward Hg 2+ over the concentration range of 0.10–3.00 μM, with a limit of detection of 3.73 nM. The sensor was further evaluated in a fish-pond water sample, achieving recoveries of 95.00–105.33% at the tested spiking levels. These results support the preliminary feasibility of the Cts/Ce-UiO-66-based ratiometric sensor for Hg 2+ determination in the tested fish-pond water matrix under the present experimental conditions. Scheme 1. Schematic illustration of the preparation and sensing processes of Cts/Ce-UiO-66/GCE. Download: Download high-res image (108KB) Download: Download full-size image
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高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Junfang Ding,Changjin Xu,Xinyi Yao,Kunming Hou,Yinkang Yang,Dan He,Hao Chai,Xiaomin Sun,Shanghong Zeng
The development of ultrafine metal oxide nanoparticles anchored on reducible oxide supports with precisely engineered interfacial active sites has emerged as a critical frontier in heterogeneous catalysis. However, conventional synthesis strategies struggle to reconcile high loading with ultrafine dispersion, often leading to nanoparticle aggregation and compromised stability. Herein, we present a coordination chemistry-driven strategy integrating the hard–soft acid–base principle with a water-etching process to synthesize ultrafine CuOx nanoparticles anchored on CeO2. By exploiting the differential coordination affinities of Ce3+ and Cu2+ with carboxyl ligands in a bimetallic BTC precursor, selective segregation during solvothermal synthesis was achieved. Ce3+ formed a stable framework with carboxyl groups, while Cu2+ underwent a hydrolysis-induced migration to surface defect sites. Regulating the Cu2+/Ce3+ ratio enabled precise control over CuOx dispersion, interfacial Cu–O–Ce bonding, and local structure. The optimized catalyst exhibited a remarkable Cu loading of 21.94% with high dispersion, lattice distortion, and enhanced metal–support interactions. Notably, the designed catalyst demonstrated exceptional stability under H2-rich streams, which achieved a CO conversion enhancement from 67.4 to 77.7% over 40 h through the interfacial stabilization of metastable Cu+-Ov-Ce4+ active configurations. Advanced characterization and density functional theory (DFT) calculations revealed that the enhanced interfacial Cu–O–Ce interactions and unsaturated coordinated CuOx species facilitated electron transfer, oxygen activation, and CO adsorption, synergistically boosting the catalytic performance via the Mars–van Krevelen mechanism. This work establishes a rational coordination chemistry-guided paradigm for designing high-performance catalysts with precisely engineered active sites.
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高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·124457
·
IF 7.5
Xiaoliang Li,Jingyu Luo,Quanfang Wei,Songling Han,Yongwu He
The development of photocatalysts that combine rapid remediation, broad applicability, and robustness in complex aqueous environments remains a significant challenge. Herein, a novel cerium oxide/carboxyl-rich graphene oxide (CeO 2 /cGO) nanocomposite was rationally synthesized, in which cGO acted as a favorable matrix for the uniform immobilization and dispersion of CeO 2 nanoparticles. Benefiting from the reversible Ce 3+ /Ce 4+ redox couple, the optimized CeO 2 /cGO delivered a narrowed bandgap and highly accelerated charge separation and migration. Under natural sunlight, it realized ultrafast and broad-spectrum elimination of dyes, antibiotics and refractory organic pollutants. Impressively, the catalyst maintained outstanding activity over wide pH ranges, practical water matrices and 18 consecutive cycles. Mechanistic investigations unveiled an “adsorption-first, catalysis-second” cascade effect. Pollutants were pre-concentrated within the confined interfacial microenvironment via π–π stacking and coordination with exposed Ce 3+ /Ce 4+ sites, drastically reducing mass transfer distances. Photogenerated charge carriers were efficiently separated through the reversible Ce 3+ /Ce 4+ redox cycle, with dissolved O 2 acting as a terminal electron acceptor to sustain catalytic turnover. While EPR detected the in situ generation of •OH, •O 2 − , and 1 O 2 , substrate-specific quenching experiments and the "scavenger-resistant" nature of the catalyst revealed a dominant non-radical pathway. For dyes, degradation was synergistically mediated by multiple reactive species, whereas recalcitrant pollutants relied predominantly on selective oxidation by surface-confined 1 O 2 and direct interfacial electron transfer. Complete mineralization into CO 2 and H 2 O was confirmed by TOC and mass spectrometry analyses. This work provides a rational design strategy for constructing highly efficient, non-radicaldominated photocatalysts with strong potential for practical water remediation.
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高影响因子
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 14
·3911-3919
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IF 9.405
Yanlong Qi,Shijun Liu,Long Cui,Quanquan Dai,Jianyun He,Wei Dong,Chenxi Bai
The synthesis of functionalized 1,3-dienes has received increasing attention due to their importance in the practical development of high-performance elastomers. In the present work, furfural and acetone, acting as renewable feedstocks, are first employed to produce a functionalized 1,3-diene containing a furan group (1-(2-furyl)-1,3-butadiene, F-diene). After selective hydrogenation of the CO group, the aldol adduct (4-(2-furanyl)-3-buten-2-ol, FAH) shows a nearly complete conversion, with an excellent selectivity (as high as 92%) towards F-diene over ceria-based catalysts in a fixed bed. BET, TEM, XRD, XPS, Raman, TPD, TPR and TGA were conducted to identify the relationship between the catalytic performance and catalyst structure. A plausible reaction pathway for the dehydration of FAH over ceria-based catalysts was proposed using a radical mechanism, which suggested the importance of the Ce4+–Ce3+ redox cycle for the dehydration of FAH to F-diene. Furthermore, the ceria-based catalysts exhibited a notable carbon resistance.
研究领域:
化学工程
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催化
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可再生化学
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材料科学
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高影响因子
Analytical Methods
·
2023
·
IF 3.1
Xin-Xin Dong,Tao-Li Chen,Xiangjuan Kong,Shuang Wu,Fang-Fang Kong,Qiang Xiao
In this work, a facile fluorescence Eu3+-based metal organic frameworks (Eu MOF) sensor for ascorbic acid (AA) and ascorbate oxidase (AAO) detection was developed. The fluorescence of Eu MOF could be effectively quenched by Ce3+ but not Ce4+ at an appropriate concentration, thus, when the reductant AA was added into the solution containing Ce4+, Ce4+ was chemically reduced to Ce3+, which induced the decreased fluorescence signal of Eu MOF. However, when AAO was introduced, AA was effectively oxidized to dehydroascorbic acid (DHAA) under the catalysis of AAO, thus, Ce4+ could not be reduced, resulting in the fluorescence restore of Eu MOF. Hence, the concentration of AA and AAO could be determined by the fluorescence decrease and restore of Eu MOF. The fluorescent platform showed high sensitivity with the limit of detection of 0.32 µM for AA and 1.18 U/L for AAO, respectively. Moreover, the proposed method was successfully applied for AA and AAO determination in real samples, indicating great potential for biomedical application in complex matrices.
研究领域:
分析化学
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生物医学工程
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材料科学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Pei Su,Xuedong Du,Yang Zheng,Wenyang Fu,Qizhan Zhang,Minghua Zhou
A bifunctional catalyst with Ce-based metal–organic frameworks deposited on carbon encapsulated Fe 3 O 4 particles (Ce-MOFs/Fe 3 O 4 @C) was prepared for heterogeneous electro-Fenton (EF), which exhibited high H 2 O 2 generation efficiency (over 90% selectivity and 80.7% current efficiency), high sulfamethazine (SMT) removal with very low electric energy consumption (7.65 kWh kg −1 SMT), and wider pH suitability to alkaline environment (pH 9). The highest content of oxygen vacancies (O V ), Ce 3+ and Fe 2+ was simultaneously exhibited when the Fe/Ce ratio in precursor was 2:1. Interface-confined between Ce-MOFs and Fe 3 O 4 @C and presence of O V promoted the O 2 adsorption for oxygen reduction reaction and O 2 ∙- generation, and electron transfer between Fe and Ce. Meanwhile, the presence of Fe 2+ /Fe 3+ and Ce 3+ /Ce 4+ simultaneously facilitated the sequential catalysis induced by H 2 O 2 to generate ∙ OH, and Ce 4+ could promote O 2 ∙- to generate 1 O 2 . This work provides new insight into the design and synthesis of Fe-based catalysts in EF with interface confinement and multi-layered reaction centers to improve the generation and the decomposition of H 2 O 2 at the same time at a low cathode potential.
研究领域:
环境科学
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催化化学
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高影响因子
ELECTROCHIMICA ACTA
·
2025
·
IF 5.6
Ran Tao,Feifei Mu,Jérome Chauvin,Serge Cosnier,Xue-Ji Zhang,Dan Shan
Rational design of highly dispersed CeO 2 nanozymes with abundant oxygen vacancies is critical for achieving efficient and sensitive H 2 O 2 detection. Herein, we report a deep eutectic solvent (DES)-guided engineering strategy to construct an N-doped carbon (NC) framework integrated with mussel-inspired, uniformly dispersed CeO 2 nanoparticles. The DES acts both as a green C/N source and a self-templating medium, regulating heteroatom distribution and graphitization degree to yield a conductive carbon scaffold. Dopamine undergoes oxidative self-polymerization under mild alkaline conditions, and its catechol–amine functionalities strongly chelate Ce 3+ ions, directing homogeneous nucleation and suppressing nanoparticle aggregation. This molecularly engineered architecture produces an oxygen-vacancy-rich interface enriched with redox-active Ce 3+ /Ce 4+ sites, enabling rapid electron transfer and accelerated H 2 O 2 redox kinetics. The optimized CeO 2 /NC electrode delivers a diffusion-controlled amperometric response with dual linear ranges (0.05–60 and 60–300 μM), a low detection limit of 0.036 μM, and sensitivities of 94.8 and 49.3 mA M -1 cm -2 , respectively, surpassing most reported CeO 2 -based sensors. Furthermore, the sensor exhibits excellent selectivity and retains 89 % of its initial response after prolonged operation. This work provides a scalable, eco-friendly pathway for constructing bioinspired, oxygen-vacancy-rich nanozymes, offering broad applicability in advanced electrocatalytic sensing platforms.
研究领域:
材料科学
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电化学
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纳米技术
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传感器与生物传感器
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环境化学
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高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Qi Zhong,Kangdong Wang,Gao Pan,Shuping Peng,Cijun Shuai
CeO2 nanozymes have demonstrated the potential to enhance biological scaffolds with chemodynamic therapy. However, their catalytic efficacy is limited by the slow conversion of Ce4+ to Ce3+ and the lack of substrates like H2O2 and H+. To address these challenges, we adopted a dual-pronged strategy that utilized the plasmonic resonance of Au nanoparticles and their glucose-oxidase mimicry to boost electron and hydrogen transfer. Specifically, we integrated Au/CeO2 nanozymes into poly-l-lactic acid scaffolds via selective laser sintering. This conversion of Ce3+ to Ce4+ in the scaffolds enhanced the reduction of H2O2 to a hydroxyl radical, inducing oxidative stress in tumor cells. The Au nanoparticles played a crucial role in boosting the Ce3+/Ce4+ catalytic cycle by providing both the energy and the catalytic substrates. They recycled Ce4+ back to Ce3+ by exploiting plasmonic-induced hot electrons and catalyzed glucose oxidation to supply H2O2 and H+. Our nanoscale and atomic-scale simulations confirmed that the Au/CeO2 hybrid structure utilized near-field coupling to amplify the plasmonic resonance and the Au–O–Ce bridge reduced the electron transfer barrier. Consequently, the Au/CeO2 scaffold decreased the activation energy from 22.57 to 9.92 kJ/mol. These findings highlight the significant promise of the Au/CeO2 nanozyme scaffold for NIR-enhanced chemodynamic therapy.
研究领域:
纳米技术
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癌症治疗
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材料科学
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生物医学工程
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高影响因子
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