A Cost‐Effective Hemin‐Based Artificial Enzyme Allows for Practical Applications

• Published in: Advanced science Vol. 11; no. 32; pp. e2402237 - n/a
• Main Authors: Qiu, Dehui, He, Fangni, Liu, Yuan, Zhou, Zhaoxi, Yang, Yuqin, Long, Zhongwen, Chen, Qianqian, Chen, Desheng, Wei, Shijiong, Mao, Xuanxiang, Zhang, Xiaobo, Mergny, Jean‐Louis, Monchaud, David, Ju, Huangxian, Zhou, Jun
• Format: Journal Article
• Language: English
• Published: Germany John Wiley & Sons, Inc 01-08-2024; Wiley Open Access; John Wiley and Sons Inc; Wiley
• Subjects: artificial enzyme; Catalysis; Chemical Sciences; Cost-Benefit Analysis - methods; Energy; Enzymes; G-Quadruplexes; G‐quadruplex; hemin; Hemin - chemistry; Hemin - metabolism; histidine analogs; Hydrogen bonds; Molecular Docking Simulation - methods; Nanomaterials; Nanoparticles; Nanostructures - chemistry; Peptides; Spectrum analysis; Wastewater - chemistry; G‐quadruplex; artificial enzyme; histidine analogs; hemin; histidine analogue; Artificial enzyme hemin histidine analogue G-quadruplex; Artificial enzyme; G-quadruplex
• ISSN: 2198-3844; 2198-3844
• DOI: 10.1002/advs.202402237

Nanomaterials excel in mimicking the structure and function of natural enzymes while being far more interesting in terms of structural stability, functional versatility, recyclability, and large‐scale preparation. Herein, the story assembles hemin, histidine analogs, and G‐quadruplex DNA in a catalytically competent supramolecular assembly referred to as assembly‐activated hemin enzyme (AA‐heminzyme). The catalytic properties of AA‐heminzyme are investigated both in silico (by molecular docking and quantum chemical calculations) and in vitro (notably through a systematic comparison with its natural counterpart horseradish peroxidase, HRP). It is found that this artificial system is not only as efficient as HRP to oxidize various substrates (with a turnover number kcat of 115 s−1) but also more practically convenient (displaying better thermal stability, recoverability, and editability) and more economically viable, with a catalytic cost amounting to <10% of that of HRP. The strategic interest of AA‐heminzyme is further demonstrated for both industrial wastewater remediation and biomarker detection (notably glutathione, for which the cost is decreased by 98% as compared to commercial kits).
A nanomaterial comprising hemin, histidine analogs, and G‐quadruplex (G4)‐forming sequences is assembled and its peroxidase‐like enzymatic activity is investigated. The resulting catalytic nanoparticles, referred to as assembly‐activated hemin enzyme (AA‐heminzyme), are readily synthesized, at low cost, exhibit excellent catalytic activity, heat resistance, and recyclability, and are found quite active in two representative applications.