机构：[1]Hunan Provincial Key Laboratory of Micro & Nano Materials Interface Science, College of Chemistry and Chemical Engineering, Central South University, Changsha, Hunan 410083, China.[2]College of Material, Chemistry and Chemical Engineering, Hangzhou Normal University, Hangzhou, Zhejiang 311121, China.[3]Department of Urology, Xiangya Hospital, Central South University, Changsha, Hunan 410083, China.[4]Department of Oncology, Xiangya Hospital, Central South University, Changsha, Hunan 410083, China.[5]State Key Laboratory for Powder Metallurgy, Central South University, Changsha, Hunan 410083, China.[6]School of Resources and Environment, University of Electronic Science and Technology of China, Chengdu, Sichuan 611731, China.[7]Henan Province Industrial Technology Research Institute of Resources and Materials, School of Material Science and Engineering, Zhengzhou University, Zhengzhou, Henan 450001, China.[8]School of Materials Science and Engineering, Peking University, Beijing 100871, China.
Designing nanozymes that match natural enzymes have always been an attractive and challenging goal. In general, researchers mainly focus on the construction of metal centers and the control of non-metallic ligands of nanozyme to regulate their activities. However, this is not applicable to lactate oxidase, i.e., flavoenzymes with flavin mononucleotide (FMN)-dependent pathways. Herein, we propose a coordination strategy to mimic lactate oxidase based on engineering the electronic properties at the N center by modulating the Co number near N in the Cox-N nanocomposite. Benefitting from the manipulated coordination fields and electronic structure around the electron-rich N sites, Co4N/C possesses a precise recognition site for lactate and intermediate organization and optimizes the absorption energies for intermediates, leading to superior oxidation of the lactate α-C-sp(3)-H bond toward ketone. The optimized nanozyme delivers much improved anticancer efficacy by reversing the high lactate and the immunosuppressive state of the tumor microenvironment, subsequently achieving excellent tumor growth and distant metastasis inhibition. The developed Co4N/C NEs open a new window for building a bridge between chemical catalysis and biocatalysis.
基金：
This work was supported by the National Science Fund for
Distinguished Young Scholars (no. 52025133), the National
Natural Science Foundation of China (nos. 22238013,
21807117, and 22178393), the National Key R&D Program
of China (no. 2017YFA0206701), Tencent Foundation
through the XPLORER PRIZE, the Hunan Provincial Science
and Technology Plan Project, China (nos. 2019TP1001 and
2020JJ3044), and the Fundamental Research Funds for the
Central Universities of Central South University, Changsha,
China (no. 2022ZZTS0397).
语种：
外文
PubmedID：
中科院(CAS)分区：
出版当年[2023]版：
大类|1 区化学
小类|1 区化学：综合
最新[2023]版：
大类|1 区化学
小类|1 区化学：综合
第一作者：
第一作者机构：[1]Hunan Provincial Key Laboratory of Micro & Nano Materials Interface Science, College of Chemistry and Chemical Engineering, Central South University, Changsha, Hunan 410083, China.[2]College of Material, Chemistry and Chemical Engineering, Hangzhou Normal University, Hangzhou, Zhejiang 311121, China.
通讯作者：
通讯机构：[1]Hunan Provincial Key Laboratory of Micro & Nano Materials Interface Science, College of Chemistry and Chemical Engineering, Central South University, Changsha, Hunan 410083, China.[2]College of Material, Chemistry and Chemical Engineering, Hangzhou Normal University, Hangzhou, Zhejiang 311121, China.[8]School of Materials Science and Engineering, Peking University, Beijing 100871, China.[*1]Hunan Provincial Key Laboratory of Micro & Nano Materials Interface Science, College of Chemistry and Chemical Engineering, Central South University, Changsha, Hunan 410083, China[*2]School of Materials Science and Engineering, Peking University, Beijing 100871, China[*3]College of Material, Chemistry and Chemical Engineering, Hangzhou Normal University, Hangzhou, Zhejiang 311121, China
推荐引用方式(GB/T 7714)：
Zhao Senfeng,Li Huihuang,Liu Renyu,et al.Nitrogen-Centered Lactate Oxidase Nanozyme for Tumor Lactate Modulation and Microenvironment Remodeling[J].Journal of the American Chemical Society.2023,doi:10.1021/jacs.3c02005.
APA：
Zhao Senfeng,Li Huihuang,Liu Renyu,Tao Na,Deng Liu...&Liu You-Nian.(2023).Nitrogen-Centered Lactate Oxidase Nanozyme for Tumor Lactate Modulation and Microenvironment Remodeling.Journal of the American Chemical Society,,
MLA：
Zhao Senfeng,et al."Nitrogen-Centered Lactate Oxidase Nanozyme for Tumor Lactate Modulation and Microenvironment Remodeling".Journal of the American Chemical Society .(2023)
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