JOURNAL OF MATERIALS SCIENCE
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2022
·Vol. 57
·期 1
·526-537
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IF 4.682
Xu Lin-Wei,Qian She-Liang,Dong Bao-Xia,Feng Li-Gang,Li Zong-Wei
Molecular complexes with active metal centers exhibit high activity and selectivity for electrochemical CO 2 reduction reaction (CO 2 RR), which represents a promising method for transforming greenhouse gas into valuable chemicals and feedstock. Using metal–organic frameworks (MOFs) to load the active molecular complexes then employing the combination with the carbonic conducting material may exhibit a beneficial effect for CO 2 RR. Herein, we obtained a composite catalyst named PCN-222(Fe)/CNTs, which was in situ synthesized through the solvothermal method that loads iron porphyrin-centered PCN-222(Fe) molecules onto CNTs. The catalyst PCN-222(Fe)/CNTs exhibits excellent electrocatalytic performance for CO 2 RR with a FE CO of 95.5% (m(Fe-TCPP):m(CNTs) = 1:30, written as PCN-222(Fe)/CNTs-30) and an overpotential ( η ) of 494 mV. In addition, the turnover frequency (TOF) is high as 448.76 h −1 (3.011 site −1 s −1 ) and the hydrogen evolution reaction (HER) is indistinctive. After long-term electrocatalysis of 10 h at −0.6 V vs. RHE, PCN-222(Fe)/CNTs-30 remained its high catalytic performance with average FE CO = 90%. This work provides a solid foundation for further research in the high-efficiency transformation of CO 2 to CO. Graphical abstract
研究领域:
电化学
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材料科学
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催化
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环境科学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry B
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2021
·Vol. 9
·期 34
·6811-6817
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IF 6.331
Xiao Liang,Yingxuan Chen,Kai Wen,Haobo Han,Quanshun Li
In the past two decades, the number of reports on the construction of uric acid (UA) sensors has increased dramatically, as it is a vital factor in the diagnosis of physiological functions and diseases. Among these sensors, cascade colorimetric detection based on peroxidase mimics has received great attention owing to the advantages of easier operation and more intuitive results. Herein, we report a simple UA detection method via the integration of urate oxidase (UOx) and PCN-222(Fe) with peroxidase-like activity, in which UOx is immobilized in PCN-222(Fe) by physical adsorption. UOx could catalyze the UA oxidation to produce H2O2, and then PCN-222(Fe) catalyzed the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) in the presence of H2O2 to generate a blue product with a maximum absorbance at 652 nm. Under optimal conditions, the increasing absorbance at 652 nm was proportional to the UA concentration. The linear range for UA detection was 10–800 μM with a limit of detection of 3.5 μM, and the cascade system has been successfully utilised for the detection of UA in human serum samples to demonstrate the accuracy of the proposed method. In conclusion, the cascade catalytic system based on the immobilization of UOx in PCN-222(Fe) has the potential to be used as a rapid and sensitive sensor for UA detection.
研究领域:
分析化学
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生物传感器
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医学诊断
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Desen Zhou,Xuan Zhang,Zheng Li,Jun Zhang,Tielin Wang,Shaowen Cao
Photocatalytic conversion of CO 2 to usable fuels provides a new strategy for solving energy problems and the greenhouse effect. Porphyrin-based metal-organic frameworks (MOFs) are promising in photocatalysis due to their remarkable light harvesting ability, and the metal active site and its coordination environment can be further adjusted to achieve the high activity. In this work, g-C 3 N 4 /PCN-222 composites with different porphyrin metal centers were fabricated and the g-C 3 N 4 /PCN-222(Fe III ) catalyst showed the highest photocatalytic CO 2 reduction performance than that of g-C 3 N 4 /PCN-222(Fe II ) and other g-C 3 N 4 /PCN-222( M , M = Co, Ni, Cu, Zn) composites. Experimental studies and theoretical calculations showed that the axial coordination in g-C 3 N 4 /PCN-222(Fe III ) distorts the square planar field (Fe-N4) to quasi-octahedral coordination, which led to the moderate adsorption ability of CO 2 reduction intermediate (*CO), resulting in the high photocatalytic activity.
研究领域:
材料科学
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环境科学
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化学工程
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催化
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
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2018
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IF 0
Bao-Xia Dong,She-Liang Qian,Fan-Yan Bu,Yi-Chen Wu,Li-Gang Feng,Yun-Lei Teng,Wen-Long Liu,Zong-Wei Li
Heterogeneous electrocatalysis provides better control of the chemical surroundings of the catalyst’s active site for improved performance, offers the possibility of overcoming drawbacks of deactivation caused by aggregation or dimerization in homogeneous condition, and permits the use of benign aqueous solutions. Employing metal–organic frameworks (MOFs) or covalent–organic frameworks (COFs) to support the active molecular catalyst of porphyrin for electrochemical conversion of CO2 to CO is a promising strategy. We have rationally introduced a 3D highly stable porphyrin-based MOF of PCN-222(Fe) into heterogeneous catalysis through the simple dip-coating method. The composite catalyst PCN-222(Fe)/C (mass ratio = 1:2) exhibited high catalytic performance for electrochemical conversion of CO2 to CO with 494 mV overpotential (where j = 1.2 mA cm–2) and maximum 91% FECO in a CO2-saturated 0.5 M KHCO3 aqueous solution, achieving a TOF of 0.336 site–1 s–1. The catalyst was found to retain its crystallinity and stability after 10 h of electrolysis at −0.60 V versus RHE (average FECO 80.4%; RHE, reversible hydrogen electrode), which generates 334 μmol of CO with the TOF of 0.012 s–1 (0.286 site–1 s–1). These results indicate that the PCN-222(Fe)/C has a substantial catalytic effect on the electrochemical reduction of CO2 due to the combination of the intrinsic activity of the porphyrin molecule, and the promising CO2 adsorption ability endowed by the conserved porosity, as well as the high conductivity of carbon black.
研究领域:
电化学
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催化
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材料科学
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环境化学
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产品关联
DOI
SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Tianyu Zeng,Shuai Wu,Qizhi Liang,Hai Shi,Jue Gong,Ningjun Duan,Wei Li,Genxi Li,Yongmei Yin
The emergence of antibody-drug conjugates (ADCs) targeting trophoblast cell-surface antigen-2 (Trop-2) has reshaped the therapeutic landscape of advanced breast cancer. Accurate profiling of the Trop-2 status of tumor cells can facilitate the identification of patients who will benefit from Trop-2-targeting therapy; however limited analytical method has hindered this process. In this study, we have proposed a specific and sensitive biosensor for visual tracking of the Trop-2 status of breast cancer cells based on tetrahedral DNA nanostructure (TDN)-decorated Fe-based metal-organic framework nanoparticles (TDN-PCN-222 (Fe)). In the design, a dual-aptamer-assisted biomimetic capture strategy shows high capture efficiency while maintaining the viability and original phenotype of captured cells, ensuring the accurate profiling of the Trop-2 status. Meanwhile, by using the high intrinsic peroxidase activity and excellent targeting ability of Trop-2-specific aptamer-linked TDN-PCN-222 (Fe), specific detection of Trop-2-positive tumor cells can be achieved with a limit of detection (LOD) of 10 cells/mL, and the Trop-2 status of tumor cells can be visually tracked. Moreover, the proposed biosensor has been successfully used for tracking the Trop-2 status of tumor cells in breast cancer tissues, suggesting that our method has great promise for clinical applications.
研究领域:
生物技术
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癌症生物学
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纳米技术
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分子诊断
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）