ACS Sensors
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2024
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IF 8.2
Huimin Yang,Zhenming Du,Yazhou Yang,Qirui Wu,Chaofan Ma,Huiyu Su,Xiaoxia Wang,Dawen Zeng
Developing gas sensors capable of efficiently detecting harmful gases is urgent to protect the human environment. Here, an active Ce–Ag bimetallic pair was innovatively introduced into SnS2, which successfully exhibited excellent NO2 gas sensing performance. 0.8% Ce–SnS2–Ag showed a gas sensing response of 5.18 to 1 ppm of NO2 at a low temperature of 80 °C, with a lower limit of detection as low as 100 ppb. DFT calculations revealed that Ce atoms are substituted into the main lattice of SnS2, which opens up the interlayer spacing and serves as an anchor point to fix the Ag atoms in the interlayer. The Ce–Ag bimetallic pairs successfully modulate the electronic structure of SnS2, which promotes the adsorption and charge transfer between NO2 and Ce–SnS2–Ag and thus achieves such an outstanding gas sensing performance. This work opens an avenue for the rational functional modification of SnS2 with an optimized electronic structure and enhanced gas sensing.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Peng Liu,Yeping Liu,Zhexu Gai,Fei Yang,Yanzhao Yang
Despite significant progress in nanozyme research and the advancement of analytical techniques, the inherent lack of specificity for target analytes often limits their utility in analysis. Integrating specific recognition capabilities into inorganic nanomaterials, independent of biological catalysts or adaptors, represents a crucial breakthrough in the field. Detecting Sarcosine (Sar) in human urine has recently emerged as a non-invasive biomarker for prostate cancer (PCa), presenting a valuable diagnostic tool. This study introduces a novel method for embedding molecular imprinting sites directly onto the surface of a Zn/Ce-based zeolitic imidazolate framework (Zn/Ce-ZIF) nanozyme, facilitating the development of a highly specific colorimetric assay for precise Sar measurement. By utilizing the lanthanide metal cerium as the catalytic element and ZIF-8 as the structural scaffold, we synthesized spherical Zn/Ce-ZIF nanozymes with exceptional oxidase-like catalytic efficiency. The efficiency of molecular imprinting experiments and the ability of molecularly imprinted polymers (MIPs) to identify target molecules were significantly enhanced by using theortical calculations to screen suitable functional monomers. The molecularly imprinted nanozyme (Zn/Ce-ZIF@MIP) initiates a colorimetric oxidation reaction of 3,3′,5,5′-tetramethylbenzidine (TMB), wherein the presence of Sar facilitates selective recognition and capture by the MIP shell, modulating the colorimetric response by hindering TMB’s access to the catalytic site. An intelligent color extraction detection device has been developed for the rapid perception of Sar. This colorimetric sensing platform has been validated through the detection of Sar in simulated urine samples. Overall, the application of surface molecular imprinting enhances the functionality of nanozymes in analytical fields.
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Nature Communications
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2024
·Vol. 15
·期 1
·1-11
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IF 14.7
Shen Fengyi,Zhang Zhihao,Wang Zhe,Ren Hao,Liang Xinhu,Cai Zengjian,Yang Shitu,Sun Guodong,Cao Yanan,Yang Xiaoxin,Hu Mingzhen,Hao Zhengping,Zhou Kebin
The state-of-the-art alkaline hydrogen evolution catalyst of united ruthenium single atoms and small ruthenium nanoparticles has sparked considerable research interest. However, it remains a serious problem that hydrogen evolution primarily proceeds on the less active ruthenium single atoms instead of the more efficient small ruthenium nanoparticles in the catalyst, hence largely falling short of its full activity potential. Here, we report that by combining highly oxophilic cerium single atoms and fully-exposed ruthenium nanoclusters on a nitrogen functionalized carbon support, the alkaline hydrogen evolution centers are facilely reversed to the more active ruthenium nanoclusters driven by the strong oxophilicity of cerium, which significantly improves the hydrogen evolution activity of the catalyst with its mass activity up to −10.1 A mg −1 at −0.05 V. This finding is expected to shed new light on developing more efficient alkaline hydrogen evolution catalyst by rational regulation of the active centers for hydrogen evolution.
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ANALYTICAL CHEMISTRY
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2018
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IF 6.042
Jiqing Yang,Xiaotong Hu,Jia Xu,Xin Liu,Li Yang
A novel capillary electrophoresis-integrated immobilized enzyme reactor (CE-integrated IMER) is developed using single-step in situ acetylcholinesterase (AChE)-mediated alginate hydrogelation and enzyme encapsulation. Alginate hydrogelation with “egg-box” structure is triggered inside a capillary with releasing of Ca2+ by changing the pH of the sol solution, which is accomplished in situ by AChE-catalyzed hydrolysis reaction of acetylthiocholine to produce acetic acid. AChE and any other enzyme initially contained in the sol solution [e.g., xanthine oxidase (XO)] are efficiently encapsulated as the hydrogel network grows, forming CE-integrated IMERs without any additional manipulation process. The proposed method facilitates the analysis of different kinds of enzymes using the same IMER depending on the substrate injected for CE analysis. Approximately 68% of the original enzyme in the sol mixture can be encapsulated, indicating high loading capacity for the CE-integrated IMERs. The IMERs exhibit excellent intraday and interday stability and batch-to-batch reproducibility, and these characteristics imply the reliability of the proposed IMERs for accurate online enzyme assays. Enzymatic activities and inhibition of immobilized AChE and XO are analyzed, and the results are compared with those using free enzymes. The feasibility of the proposed method for potential application in real sample analysis is demonstrated by the successful application of the IMERs in detecting organophosphorus pesticides in apple juice samples using AChE-catalyzed reactions. The proposed method is a simple, efficient, and universal approach for online CE assays with immobilized enzymes, which can be widely applied in bioanalysis.
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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.
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ACS Applied Materials & Interfaces
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2024
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IF 8.3
Baihe Sun,Guanghui Li,Yue Wu,Junwei Gai,Min Zhu,Weiwei Ji,Xiaoying Wang,Fenghua Zhang,Wanting Li,Jingjin Hu,Yuxin Lou,Gusheng Feng,Xijun Han,Jinwen Dong,Jiayuan Peng,Jiawei Pei,Yakun Wan,Yanfei Li,Linlin Ma
Apolipoprotein A1 (Apo-A1) is a well-recognized biomarker in tissues, closely associated with cardiovascular diseases such as atherosclerosis, coronary artery disease, and heart failure. However, existing methods for Apo-A1 determination are limited by costly equipment and intricate operational procedures. Given the distinct advantages of electrochemical immunosensors, including affordability and high sensitivity, along with the unique attributes of nanobodies (Nbs), such as enhanced specificity and better tissue permeability, we developed an electrochemical immunosensor for Apo-A1 detection utilizing Nb technology. In our study, Ce-MOF@AuNPs nanocomposites were synthesized by using ultrasonic methods and applied to modify a glassy carbon electrode. The Nb6, screened from an Apo-A1 immunized phage library, was immobilized onto the nanocomposite material, establishing a robust binding interaction with Apo-A1. The recorded peak current values demonstrated a logarithmic increase corresponding to Apo-A1 concentrations ranging from 1 to 100,000 pg/mL, with a detection limit of 36 fg/mL. Additionally, the developed immunosensors demonstrated high selectivity, good stability, and reproducibility. Our methodology was also effectively utilized for serum sample analysis, showing good performance in clinical assessments. This electrochemical immunosensor represents a promising tool for Apo-A1 detection, with significant potential for advancing cardiovascular disease diagnostics.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Yuhong Zhang,Yanchang Liu,Junlong Liu,Zhihao Qu,Siye Tian,Hang Liu
Here, Ce-doped ZnO flower-like nanosheets are prepared by one-step hydrothermal method . The sensor based on Ce–ZnO composite exhibits excellent gas-sensing properties to acetone. Compared with pure ZnO, the response of Ce–ZnO composite is increased by 5.5 times, and the optimum operating temperature is reduced by 60 °C. The gas-sensing properties of the sensor to acetone under different humidity conditions are investigated. The redox reaction of Ce element increases the anti-humidity of Ce–ZnO sensor. Finally, the gas sensing mechanism of Ce–ZnO nanomaterial and anti-humidity principle are discussed in detail. The result can provide a new material for develop high sensitivity acetone sensor and a new anti-humidity strategy for designing gas sensing materials.
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Gas Science and Engineering
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2024
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IF 0
Xuebi Du,Dawei Shao,Yinhua Wan
Metal-organic frameworks (MOFs) have shown potential as nanofillers for the selective capture of specific gases in mixed matrix membranes (MMMs). This study introduces an efficient method, utilizing a mild (100 °C) reaction condition and a short reaction time (20 min), for the synthesis of MOF-808(Ce) nanocrystals. The MOF-808(Ce) that is obtained exhibits porous characteristics, a notable affinity for CO 2 , and robust intermolecular interactions with PIM-1. Furthermore, this study pioneers the incorporation of MOF-808(Ce) as a filler into PIM-1, with varying loadings, to create PIM/MOF-808 MMMs for the purpose of CO 2 separation. Consequently, the MMMs containing 2 wt% MOF-808(Ce) demonstrate high CO 2 permeability of 6854 Barrer and CO 2 /N 2 selectivity of 23.2, which is far surpasses 2008 upper bound from Robeson and approaches the refined 2019 upper bound from MeKenow. A comparative analysis demonstrates the efficacy of MOF-808(Ce) as a filler in PIM-1 for the purpose of CO 2 separation.
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JOURNAL OF RARE EARTHS
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2024
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IF 5.2
Yanting Zuo,Shi Cheng,Ziwen Guo,Haolin Liu,Huaicheng Zhang,Ji Wu,Ziwu Fan,Wentao Li,Aimin Li
Sulfamethoxazole (SMZ) is a prevalent and recalcitrant micropollutant in water, posing a significant threat to both aquatic organisms and human health. Therefore, investigating the removal of SMZ is of critical importance. In order to investigate the effect of rare earth metal doping on the performance of activated persulfate oxidative degradation of SMZ, BiFeO 3 with different Ce doping amounts was successfully prepared by a hydrothermal method. Then, it was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), scanning transmission electron microscopy (STEM) and Brunauer–Emmett–Teller (BET) method. The performance of porous Ce/BiFeO 3 in the catalytic activation of persulfate (PMS) for the degradation of SMZ in water was investigated using SMZ solution as a simulated wastewater. The impact of Ce doping rate, catalyst dosage, temperature variations, common anions, natural organic matter, and PMS concentration on SMZ removal was systematically evaluated. The characterization results show that the octahedral rhombic structure of Ce can be observed on the surface of this doped catalyst, and Ce doping does not change the crystalline shape of Ce/BiFeO 3 . The specific surface area of the doped catalyst increases, accompanied by an enlargement of pore size, thereby enhancing the catalyst's adsorption capacity and resistance to contamination by SMZ. Under the optimal conditions of 25 °C, SMZ concentration of 20 mg/L, 0.8 g/L PMS and 0.3 g/L 0.05Ce/BiFeO 3 catalyst, the removal rate of SMZ reaches approximately 95% within 35 min of reaction time. Even after five cycles of reuse, the degradation rate of SMZ remains above 88%, demonstrating the catalyst's good stability and reusability. Bursting experiments show that SO 4 ·– , ·OH, 1 O 2 and O 2 ·– are involved in the catalytic degradation process, with 1 O 2 playing a dominant role.
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RARE METALS
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2024
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IF 9.6
Liu Cheng,Shi Ying-Zhang,Chen Qi,Ye Bing-Hua,Bi Jin-Hong,Yu Jimmy C.,Wu Ling
Defect engineering in metal organic frameworks (MOFs) has captured significant attention in the field of photocatalysis. A series of UiO-66(Ce) (UiO = University of Oslo) MOFs with different contents of missing-linker defects have been developed for the photocatalytic selective oxidation of benzylamine (BA) and thioanisole (TA) under visible light. The introduction of missing-linker defects promotes the formation of unsaturated Ce sites with a high Ce 3+ content. It also generates a high concentration of oxygen vacancies. In situ Fourier transform infrared spectroscopy (FTIR) results revealed that BA and TA molecules were activated on coordinatively unsaturated Ce sites via the H–N···Ce and the C–S···Ce interactions, respectively. Simulated in situ electron paramagnetic resonance (EPR) data indicate that O 2 activation and reduction occur at coordinatively unsaturated Ce 3+ sites to form ·O 2 – . This is accelerated by the Ce 3+ /Ce 4+ redox cycle associated with the photogenerated electrons. The corresponding photogenerated holes are involved in the deprotonation of the activated BA and TA. The most active sample exhibits 98.4% and 95.5% conversion rates for BA and TA oxidation. Mechanisms for the molecular activation are proposed at the molecular level. Graphical abstract
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Aiyong Wang,Jiajia Ding,Mingqi Li,Peiyao Song,Zhiyuan Zhao,Yanglong Guo,Yun Guo,Li Wang,Qiguang Dai,Wangcheng Zhan
Short carbon chain alkanes, as typical volatile organic compounds (VOCs), have molecular structural stability and low molecular polarity, leading to an enormous challenge in the catalytic oxidation of propane. Although Ru-based catalysts exhibit a surprisingly high activity for the catalytic oxidation of propane to CO2 and H2O, active RuOx species are partially oxidized and sintered during the oxidation reaction, leading to a decrease in catalytic activity and significantly inhibiting their application in industrial processes. Herein, the Ru/Ce@Co catalyst is synthesized with a specific structure, in which cerium dioxide is dispersed in a thin layer on the surface of Co3O4, and Ru nanoparticles fall preferentially on cerium oxide with high dispersity. Compared with the Ru/CeO2 and Ru/Co3O4 catalysts, the Ru/Ce@Co catalyst demonstrates excellent catalytic activity and stability for the oxidation of propane, even under severe operating conditions, such as recycling reaction, high space velocity, a certain degree of moisture, and high temperature. Benefiting from this particular structure, the Ru/Ce@Co (5:95) catalyst with more Ce3+ species leads to the Ru species being anchored more firmly on the CeO2 surface with a low-valent state and has a strong potential for adsorption and activation of propane and oxygen, which is beneficial for RuOx species with high activity and stability. This work provides a novel strategy for designing high-efficiency Ru-based catalysts for the catalytic combustion of short carbon alkanes.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Xiaoshun Wei,Xuechun Yang,Yun Guo,Guohao Li,Yinzhong Liu,Lingli Cheng,Zheng Jiao
Being one of toxic and flammable volatile organic compounds (VOC), n-butanol has brought about many potential health risks, there is an urgent demand for highly sensitive detection techniques to monitor its concentration in occupational environments and the air. In this paper, Ce-doped MOF:ZnO sensors under UV activation for room-temperature detection of n-butanol were synthesized by the co-precipitation method and systemically characterized by XRD, SEM, HRTEM, and XPS. The sensitive performances were evaluated by the use of a WS-30A gas sensor measurement system. The results showed that Ce doping has significantly enhanced the sensitivity of the MOF:ZnO sensors, and the response value of the 0.08 % Ce-doped ZnO sensor has achieved to 397.30, which was 9.32 times higher than that of the pristine MOF:ZnO. And the response and recovery times were 17 and 117 s respectively, demonstrating a speedy detection capability. In addition, the sensor gained excellent stability and reproducibility with special selectivity for n-butanol. The comprehensive achievements of this research would be promising to promote the development of volatile organic compound detection technology and beneficial to the well application in the fields of environmental monitoring, industrial safety, and public health.
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