Synergistic Effect of Bimetallic Bioelectrocatalysis and Endogenous Soluble Electron Mediators for Functional Regulation of Electroactive Biofilms

IF 9.7 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Journal of Cleaner Production Pub Date : 2025-01-22 DOI:10.1016/j.jclepro.2025.144789

Xu Pan, Ye Chen, Qing Wen, Cunguo Lin, Haiping Gao, Zhenghui Qiu, Liuqingying Yang

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引用次数: 0

Abstract

Microbial fuel cells (MFCs) are green power generation devices that convert chemical energy into electricity. The energy conversion efficiency and power generation performance of MFCs are primarily influenced by the extracellular electron transfer (EET) process mediated by electroactive bacteria. In this study, Zr, N-codoped carbon (Zr-NC) and Fe, Zr, N-codoped carbon (Fe-Zr-NC) materials were derived from amino-modified Zr and Fe-Zr metal organic frameworks (MOF), respectively, and were considered as high-performance bioelectrocatalysts to optimize the multi-electron EET pathway and the interfacial charge transfer kinetics. Compared to Zr-NC MFC, the maximum power density of Fe-Zr-NC MFC increased from 3.62 to 5.25 W/m², and the coulombic efficiency increased from 18.23% to 26.37%. In addition, Fe-Zr-NC improved the total capacitive behavior contribution of bioanode, increasing the limiting storage capacity of biocapacitor from 4207.46 to 10582.28 C/m². Furthermore, the exchange current density of the Fe-Zr-NC bioanode increased from 0.65 to 1.43 mA/cm², while the charge transfer resistance decreased from 3.72 Ω to 1.08 Ω. Electrochemical measurements and density functional theory (DFT) suggested that the charge redistribution of Fe atoms at the bimetallic catalytic sites increased the interfacial potential difference of the terminal conductive protein and the strong adsorption of flavin species, thus regulating the dominant EET pathway and charge transfer kinetics. High-throughput sequencing results and PICRUSt2 indicated the affinity of Fe-Zr-NC bioelectrocatalyst for functional microorganisms, facilitating the enrichment of exoelectrogens and the secretion of soluble electron mediators. Fe-Zr-NC can serve as a novel bioelectrocatalyst with high performance and stability for the improvement of MFCs or biocapacitors, leading to higher power output and energy conversion efficiency.

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双金属生物电催化与内源性可溶性电子介质在电活性生物膜功能调控中的协同作用

微生物燃料电池（mfc）是一种将化学能转化为电能的绿色发电装置。mfc的能量转换效率和发电性能主要受电活性菌介导的胞外电子转移（EET）过程的影响。本研究分别从氨基修饰的Zr和Fe-Zr金属有机骨架（MOF）中制备了Zr， n共掺杂碳（Zr- nc）和Fe， Zr， n共掺杂碳（Fe-Zr- nc）材料，并将其作为高性能的生物电催化剂，优化了多电子EET途径和界面电荷转移动力学。与Zr-NC MFC相比，Fe-Zr-NC MFC的最大功率密度从3.62 W/m2提高到5.25 W/m2，库仑效率从18.23%提高到26.37%。此外，Fe-Zr-NC提高了生物阳极的总电容行为贡献，使生物电容器的极限存储容量从4207.46 C/m2提高到10582.28 C/m2。Fe-Zr-NC生物阳极的交换电流密度从0.65 mA/cm2增加到1.43 mA/cm2，电荷转移电阻从3.72 Ω降低到1.08 Ω。电化学测量和密度泛函理论（DFT）表明，Fe原子在双金属催化位点的电荷重分布增加了末端导电蛋白的界面电位差和黄素的强吸附，从而调节了EET的优势途径和电荷转移动力学。高通量测序结果和PICRUSt2表明，Fe-Zr-NC生物电催化剂对功能微生物具有亲和力，有利于外电的富集和可溶性电子介质的分泌。Fe-Zr-NC可以作为一种高性能稳定的新型生物电催化剂，用于mfc或生物电容器的改进，从而提高功率输出和能量转换效率。

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来源期刊

Journal of Cleaner Production 环境科学-工程：环境

CiteScore

20.40

自引率

9.00%

发文量

4720

审稿时长

111 days

期刊介绍： The Journal of Cleaner Production is an international, transdisciplinary journal that addresses and discusses theoretical and practical Cleaner Production, Environmental, and Sustainability issues. It aims to help societies become more sustainable by focusing on the concept of 'Cleaner Production', which aims at preventing waste production and increasing efficiencies in energy, water, resources, and human capital use. The journal serves as a platform for corporations, governments, education institutions, regions, and societies to engage in discussions and research related to Cleaner Production, environmental, and sustainability practices.