摘要
The preparation of high-value fuels and chemicals through the electrochemical carbon dioxide reduction reaction(CDRR)is of great significance to the virtuous cycle of carbon dioxide.However,due to the high overpotential involved in this reaction,high power consumption and high-cost noble-metal-based catalysts are required for driving this process.Herein,the electrochemical CDRR was achieved on biocompatible metal-free nitrogen,phosphorus co-doped carbon-based materials(NP-C)in the microbial fuel cell-microbial electrolysis cell(MFC-MEC)coupling system.As the bioelectrochemistry in MFC supplied power to drive the electrocatalysis in MEC,syngas was spontaneously produced from this coupling system without external energy input.With the NP-C materials as the excellent bifunctional electrocatalyst for the CDRR and oxygen reduction reaction(ORR),the current density of the MEC reached−0.52 mA cm^−2,and the Faradaic efficiencies(FEs)of CO and H2 were 60%and 40%,respectively,at a load resistance of 10Ω.Moreover,the CO/H2 product ratio can be changed by adjusting the load resistance,which will widely meet various demand of syngas usage in further reactions.This study provides a spontaneous and tunable production of syngas in biogas digesters via a electrochemical strategy.
通过二氧化碳的电化学还原来制备高价值的燃料和化学品对二氧化碳的良性循环具有重要意义.然而,由于二氧化碳电化学还原过程中的高过电势,导致驱动该还原反应需要高功耗和高成本贵金属催化剂.在本文中,电化学二氧化碳还原反应是在微生物燃料电池-微生物电解池(MFC-MEC)耦合系统中具有生物相容性的无金属氮磷共掺杂碳基材料上实现的.基于MFC中的生物电化学提供能量以驱动MEC中的电催化作用,无需任何外部能量输入,就可以从该耦合体系中自发产生合成气.在MFC-MEC耦合体系中,对于二氧化碳还原反应和氧还原反应,NP-C材料是一种优良的双功能电催化剂.当负载电阻为10Ω时,MEC阴极的电流密度可达-0.52 mA cm^-2,CO和H2的法拉第效率分别为60%和40%.此外,可以通过调节负载电阻来改变CO/H2产物比,可满足进一步反应中对于合成气使用的各种需求.这项工作为通过沼气池中的微生物系统自发生产合成气提供了一种新的电化学策略.
作者
Wei Wang
Rahul Anil Borse
Jiafang Xie
Yaobing Wang
王玮;Rahul Anil Borse;谢佳芳;王要兵(Key Laboratory of Design and Assembly of Functional Nanostructures,Fujian Provincial Key Laboratory of Nanomaterials,State Key Laboratory of Structural Chemistry,Key Laboratory of Optoelectronic Materials Chemistry and Physics,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences,Fuzhou,350002,China;University of Chinese Academy of Sciences,Beijing,100049,China;Dalian National Laboratory for Clean Energy,Dalian,116023,China)
基金
the National Natural Science Foundation of China(21872147 and 21805277)
the Natural Science Foundation of Fujian Province(2018J05030 and 2019J05152)
the Key Research Program of Frontier Sciences,CAS(ZDBS-LYSLH028)
DNL Cooperation Fund,CAS(DNL201924)
the Strategic Priority Research Program,CAS(XDB20000000)。
