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古志远教授课题组在JOURNAL OF THE AMERICAN CHEMICAL SOCIETY发表研究论文

发布时间:17-08-04 15:32:07 文章来源:1 浏览次数: [ 字号:


Two-Dimensional Metal-Organic Framework Nanosheets as an Enzyme Inhibitor: Modulation of the alpha-Chymotrypsin Activity
Xu, M (Xu, Ming)[ 1 ] ; Yuan, S (Yuan, Shuai)[ 2 ] ; Chen, XY (Chen, Xin-Yu)[ 1 ] ; Chang, YJ (Chang, Yu-Jie)[ 1 ] ; Day, G (Day, Gregory)[ 2 ] ; Gu, ZY (Gu, Zhi-Yuan)[ 1 ]*(古志远); Zhou, HC (Zhou, Hong-Cai)[ 2,3 ]*

[ 1 ] Nanjing Normal Univ, Coll Chem & Mat Sci, Jiangsu Collaborat Innovat Ctr Biomed Funct Mat, Jiangsu Key Lab Biofunct Mat, Nanjing 210023, Jiangsu, Peoples R China
[ 2 ] Texas A&M Univ, Dept Chem, College Stn, TX 77843 USA
[ 3 ] Texas A&M Univ, Dept Mat Sci & Engn, College Stn, TX 77842 USA

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,201706,139(24),8312-8319

Two-dimensional metal organic framework (MOP) nanosheets are utilized as effective enzyme inhibitors, providing an inspiring means to enhance the control of cellular processes as well as improve our understanding of the surface chemistry between MOFs and enzymes. In this paper, we demonstrated that the activity of alpha-chymotrypsin (ChT) can be effectively inhibited with 96.9% inhibition by 2-D Cu(bpy)(2)(OTf)(2) nanosheets, while Zn-2(bim)(4) nanosheets show no significant inhibition effect toward ChT. Kinetic studies revealed that the material acts as a competitive inhibitor toward ChT. Furthermore, fluorescence and circular dichroism spectroscopy reveal that the 2-D MOF nanosheets do not change the secondary structure of the enzyme. The Cu(II) center of the 2-D nanosheets binds the 4-(2-hydroxyethyl)-1-piperazineethanesulfonic acid (HEPES) molecules in the buffer, leading to an electrostatic interaction between the nanosheets and the enzyme. In addition, the irreversible coordination interactions between Cu(II) center and His-57 played an important role during the inhibition process, as supported by ionic strength experiments and UV absorbance changes of Cu(II) d-d transitions. As a result, the substrate is prevented from reaching the active sites of the enzyme causing enzyme inhibition. The modulation of enzyme activity by 2-D MOF nanosheets opens up a new direction for the exploration of the MOF-bio interface in physiological and catalytic systems.


文章链接:
http://pubs.acs.org/doi/abs/10.1021/jacs.7b03450
 


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