Enzyme cascade reactions play significant roles in bioelectrochemical processes because they permit more complex reactions. Co-immobilization of multienzyme on the electrode could help to facilitate substrate/intermed...Enzyme cascade reactions play significant roles in bioelectrochemical processes because they permit more complex reactions. Co-immobilization of multienzyme on the electrode could help to facilitate substrate/intermediate transfer among different enzymes and electron transfer from enzyme active sites to the electrode with high stability and retrievability. Different co-immobilization strategies to construct multienzyme bioelectrodes have been widely reported, however, up to now, they have barely been reviewed. In this review, we focus on recent state-of-the-art techniques for constructing co-immobilized multienzyme electrodes including random and positional co-immobilization. Particular attention is given to strategies such as multienzyme complex and surface display. Cofactor co-immobilization on the electrode is also crucial for the enhancement of catalytic reaction and electron transfer, yet, few studies have been reported. The up-to-date advances in bioelectrochemical applications of multienzyme bioelectrodes are also presented. Finally, key challenges and future perspectives are discussed.展开更多
Microalgae biomass is an ideal precursor to prepare renewable carbon materials,which has broad application.The bioaccumulation efficiency(lipids,proteins,carbohydrates)and biomass productivity of microalgae are influe...Microalgae biomass is an ideal precursor to prepare renewable carbon materials,which has broad application.The bioaccumulation efficiency(lipids,proteins,carbohydrates)and biomass productivity of microalgae are influenced by spectroscopy during the culture process.In this study,a bilayer plate-type photobioreactor was designed to cultivate Chlorella protothecoides with spectral selectivity by nanofluids.Compared to culture without spectral selectivity,the spectral selectivity of Ag/CoSO_(4)nanofluids increased microalgae biomass by 5.76%,and the spectral selectivity of CoSO_(4)solution increased by 17.14%.In addition,the spectral selectivity of Ag/CoSO_(4)nanofluids was more conducive to the accumulation of nutrients(29.46%lipids,50.66%proteins,and 17.86%carbohydrates)in microalgae.Further cultured chlorella was utilized to prepare bioelectrode materials,it was found that algal based biochar had a good pore structure(micro specific surface area:1627.5314 m^(2)/g,average pore size:0.21294 nm).As the current density was 1 A/g,the specific capacitance reached 230 F/g,appearing good electrochemical performance.展开更多
The effective elimination of aromatic compounds from wastewater is imperative for safeguarding the ecological environment.Bioelectrochemical processes that combine cathodic reduction and anodic oxidation represent a p...The effective elimination of aromatic compounds from wastewater is imperative for safeguarding the ecological environment.Bioelectrochemical processes that combine cathodic reduction and anodic oxidation represent a promising approach for the biomineralization of aromatic compounds.However,conventional direct current bioelectrochemical methods have intrinsic limitations.In this study,a low-frequency and low-voltage alternating current(LFV-AC)-driven bioelectrode offering periodic in situ coupling of reduction and oxidation processes was developed for the biomineralization of aromatic compounds,as exemplified by the degradation of alizarin yellow R(AYR).LFV-AC stimulated biofilm demonstrated efficient bidirectional electron transfer and oxidation–reduction bifunctionality,considerably boosting AYR reduction(63.07%±1.91%)and subsequent mineralization of intermediate products(98.63%±0.37%).LFV-AC stimulation facilitated the assembly of a collaborative microbiome dedicated to AYR metabolism,characterized by an increased abundance of functional consortia proficient in azo dye reduction(Stenotrophomonas and Bradyrhizobium),aromatic intermediate oxidation(Sphingopyxis and Sphingomonas),and electron transfer(Geobacter and Pseudomonas).The collaborative microbiome demonstrated a notable enrichment of functional genes encoding azo-and nitro-reductases,catechol oxygenases,and redox mediator proteins.These findings highlight the effectiveness of LFV-AC stimulation in boosting azo dye biomineralization,offering a novel and sustainable approach for the efficient removal of refractory organic pollutants from wastewater.展开更多
The high impedance caused by the lack of interfacial hydrogel in dry electrodes seriously affects the quality of acquired electrophysiological signals.Although there are existing strategies to reduce impedance with mi...The high impedance caused by the lack of interfacial hydrogel in dry electrodes seriously affects the quality of acquired electrophysiological signals.Although there are existing strategies to reduce impedance with micro–nanostructures,achieving stretchable and breathable electrodes while ensuring low impedance is extremely challenging.Herein,we successfully prepared a dry textile electrode(nanomesh film(NF)-ZnO–polypyrrole(PPy))with low impedance,high stretchability,and breathability.Wrinkle-nanorod coupled microstructures are constructed to increase the effective surface area and roughness of NF-ZnO–PPy electrode,achieving an exponential reduction in impedance compared with the smooth textile dry electrode(15.64 kΩ·cm^(-2)at 10 Hz,approximately 1/6 of the lowest impedance of reported electrodes).Simultaneously,the wrinkled structure formed by pre-stretching improves electrode’s stretchability(up to 910%strain)and cycle stability(R/R0 is within 1.08 after 1000 cycles at 30%strain).Furthermore,the NF-ZnO–PPy electrode has excellent breathability(2233.52 g·m^(-2)·d^(-1))and good biocompatibility.Finally,as a proof of concept,the 16-channel NF-ZnO–PPy electrode can record electromyography signals in different states and parts of body for a long time((22.03±0.76)dB,which is twice that of the commercial electrode).Notably,we employ ZnO nanorods as a template to reduce impedance.This template strategy overcomes complex and expensive micro–nanomanufacturing technologies(photolithography,laser processing,etc.)and can be suitable for most flexible substrates,showing great potential in the field of soft electronics.展开更多
Conducting polymer hydrogels offer promising electrical interfaces with biological tissues for electrophysio-logical signal recording,sensing,and stimulation due to their favorable electrical properties,biocompatibili...Conducting polymer hydrogels offer promising electrical interfaces with biological tissues for electrophysio-logical signal recording,sensing,and stimulation due to their favorable electrical properties,biocompatibility,and stability.Among them,Poly(3,4-ethylenedioxythiophene):Polystyrene sulfonate(PEDOT:PSS)is widely used as a conductive filler,forming a network of conjugated nanofibers within the hydrogel matrix.This structure enables robust electronic conductivity while preserving ionic transport and biocompatibility in phys-iological environments.However,the mechanical integrity of these hydrogels is often compromised by micellar microstructures in aqueous colloidal dispersions.The absence of interconnected conducting polymer nanofibers to maintain mechanical integrity during swelling hinders the mechanical properties of hydrogels.Here,three modification strategies were explored to enhance the flexibility and stretchability:constructing an inter-penetrating network,phase separation induced by ionic compounds,and pure conductive hydrogels formed through polar solvent additives and dry-annealing.These strategies synergistically enhance conductivity and flexibility by controlling interchain entanglement and redesigning the distribution of conjugated crystal regions and soft regions.The resulting hydrogels exhibit excellent conductivity(1.99-5.25 S/m),softness(elastic modulus as low as 280 Pa),and elasticity(tensile properties up to 800%).When used as epidermal or implantable bioelectrodes,they provided a soft interface,ensuring longer-lasting and more stable electromyo-gram,electrocardiogram,and electroencephalogram signals compared to commercial gel electrodes,with a signal-to-noise ratio of up to 20.0 dB.Therefore,the conducting polymer hydrogels developed in this study leverage the synergy between conductivity and flexibility,paving the way for further transformative applications in bioelectronics.展开更多
开发耐用且可靠的生物电极,用以采集高质量的生物电信号,已成为人体生理状态监测和人机交互领域的关键技术.然而,现有的生物电极多基于传统弹性基底,这导致了机械性能不匹配和低渗透性等问题,并且缺乏与生物皮肤类似的多方面属性和必要...开发耐用且可靠的生物电极,用以采集高质量的生物电信号,已成为人体生理状态监测和人机交互领域的关键技术.然而,现有的生物电极多基于传统弹性基底,这导致了机械性能不匹配和低渗透性等问题,并且缺乏与生物皮肤类似的多方面属性和必要的协同特性.本研究中,我们报道了一种新型的基于自支撑导电全聚合物薄膜的超薄表皮生物电极(ASU-EBE).该电极将超一致性、优异的拉伸性和透气性集成于一体,展现了约475 S cm^(-1)的高导电性,约48%的出色拉伸性,与生物组织界面的超一致性以及优异的透气性.该电极的电子和机械性能得到提升,这归功于在PEDOT:PSS中引入水溶性聚氧化乙烯,以调节分子间π-π堆积距离,并促进纳米纤维结构的形成.因此,ASU-EBE在与皮肤接触时的阻抗远低于标准凝胶电极,使其成为复杂日常环境下长期医疗监测的理想选择.展开更多
基金supported by the National Natural Science Foundation of China(21878324,21706273)the CAS Pioneer Hundred Talent Program(Type C,reference#2016-081)。
文摘Enzyme cascade reactions play significant roles in bioelectrochemical processes because they permit more complex reactions. Co-immobilization of multienzyme on the electrode could help to facilitate substrate/intermediate transfer among different enzymes and electron transfer from enzyme active sites to the electrode with high stability and retrievability. Different co-immobilization strategies to construct multienzyme bioelectrodes have been widely reported, however, up to now, they have barely been reviewed. In this review, we focus on recent state-of-the-art techniques for constructing co-immobilized multienzyme electrodes including random and positional co-immobilization. Particular attention is given to strategies such as multienzyme complex and surface display. Cofactor co-immobilization on the electrode is also crucial for the enhancement of catalytic reaction and electron transfer, yet, few studies have been reported. The up-to-date advances in bioelectrochemical applications of multienzyme bioelectrodes are also presented. Finally, key challenges and future perspectives are discussed.
基金This work was supported by the Key Research and Development Project of Jiangsu Province(BE2019009-4)the National Natural Science Foundation of China(52106091)the Qing Lan Project of Jiangsu Province。
文摘Microalgae biomass is an ideal precursor to prepare renewable carbon materials,which has broad application.The bioaccumulation efficiency(lipids,proteins,carbohydrates)and biomass productivity of microalgae are influenced by spectroscopy during the culture process.In this study,a bilayer plate-type photobioreactor was designed to cultivate Chlorella protothecoides with spectral selectivity by nanofluids.Compared to culture without spectral selectivity,the spectral selectivity of Ag/CoSO_(4)nanofluids increased microalgae biomass by 5.76%,and the spectral selectivity of CoSO_(4)solution increased by 17.14%.In addition,the spectral selectivity of Ag/CoSO_(4)nanofluids was more conducive to the accumulation of nutrients(29.46%lipids,50.66%proteins,and 17.86%carbohydrates)in microalgae.Further cultured chlorella was utilized to prepare bioelectrode materials,it was found that algal based biochar had a good pore structure(micro specific surface area:1627.5314 m^(2)/g,average pore size:0.21294 nm).As the current density was 1 A/g,the specific capacitance reached 230 F/g,appearing good electrochemical performance.
基金supported by the National Natural Science Foundation of China(52170054,51608467,and 52200202)the“Qing Lan Project”of Colleges and Universities in Jiangsu Province。
文摘The effective elimination of aromatic compounds from wastewater is imperative for safeguarding the ecological environment.Bioelectrochemical processes that combine cathodic reduction and anodic oxidation represent a promising approach for the biomineralization of aromatic compounds.However,conventional direct current bioelectrochemical methods have intrinsic limitations.In this study,a low-frequency and low-voltage alternating current(LFV-AC)-driven bioelectrode offering periodic in situ coupling of reduction and oxidation processes was developed for the biomineralization of aromatic compounds,as exemplified by the degradation of alizarin yellow R(AYR).LFV-AC stimulated biofilm demonstrated efficient bidirectional electron transfer and oxidation–reduction bifunctionality,considerably boosting AYR reduction(63.07%±1.91%)and subsequent mineralization of intermediate products(98.63%±0.37%).LFV-AC stimulation facilitated the assembly of a collaborative microbiome dedicated to AYR metabolism,characterized by an increased abundance of functional consortia proficient in azo dye reduction(Stenotrophomonas and Bradyrhizobium),aromatic intermediate oxidation(Sphingopyxis and Sphingomonas),and electron transfer(Geobacter and Pseudomonas).The collaborative microbiome demonstrated a notable enrichment of functional genes encoding azo-and nitro-reductases,catechol oxygenases,and redox mediator proteins.These findings highlight the effectiveness of LFV-AC stimulation in boosting azo dye biomineralization,offering a novel and sustainable approach for the efficient removal of refractory organic pollutants from wastewater.
基金support from the National Natural Science Foundation of China(Grants No.52173237)Nationally Funding Postdoctoral Researcher Program(Grants No.GZC20233469)+4 种基金The Fundamental Research Funds for the Central Universities(Grants No.HIT.OCEF.2022018HIT.NSRIF 202315)Natural Science Foundation of Heilongjiang Province,China(LH2022E051,LH2021B009)Interdisciplinary Research Foundation of HIT(IR2021207)The Open Project Program of Key Laboratory for Photonic and Electric Bandgap Materials,Ministry of Education(PEBM202107).
文摘The high impedance caused by the lack of interfacial hydrogel in dry electrodes seriously affects the quality of acquired electrophysiological signals.Although there are existing strategies to reduce impedance with micro–nanostructures,achieving stretchable and breathable electrodes while ensuring low impedance is extremely challenging.Herein,we successfully prepared a dry textile electrode(nanomesh film(NF)-ZnO–polypyrrole(PPy))with low impedance,high stretchability,and breathability.Wrinkle-nanorod coupled microstructures are constructed to increase the effective surface area and roughness of NF-ZnO–PPy electrode,achieving an exponential reduction in impedance compared with the smooth textile dry electrode(15.64 kΩ·cm^(-2)at 10 Hz,approximately 1/6 of the lowest impedance of reported electrodes).Simultaneously,the wrinkled structure formed by pre-stretching improves electrode’s stretchability(up to 910%strain)and cycle stability(R/R0 is within 1.08 after 1000 cycles at 30%strain).Furthermore,the NF-ZnO–PPy electrode has excellent breathability(2233.52 g·m^(-2)·d^(-1))and good biocompatibility.Finally,as a proof of concept,the 16-channel NF-ZnO–PPy electrode can record electromyography signals in different states and parts of body for a long time((22.03±0.76)dB,which is twice that of the commercial electrode).Notably,we employ ZnO nanorods as a template to reduce impedance.This template strategy overcomes complex and expensive micro–nanomanufacturing technologies(photolithography,laser processing,etc.)and can be suitable for most flexible substrates,showing great potential in the field of soft electronics.
基金supported by the National Natural Science Foundation of China(22278241)a grant from the Institute Guo Qiang,Tsing-hua University(2021GQG1016).
文摘Conducting polymer hydrogels offer promising electrical interfaces with biological tissues for electrophysio-logical signal recording,sensing,and stimulation due to their favorable electrical properties,biocompatibility,and stability.Among them,Poly(3,4-ethylenedioxythiophene):Polystyrene sulfonate(PEDOT:PSS)is widely used as a conductive filler,forming a network of conjugated nanofibers within the hydrogel matrix.This structure enables robust electronic conductivity while preserving ionic transport and biocompatibility in phys-iological environments.However,the mechanical integrity of these hydrogels is often compromised by micellar microstructures in aqueous colloidal dispersions.The absence of interconnected conducting polymer nanofibers to maintain mechanical integrity during swelling hinders the mechanical properties of hydrogels.Here,three modification strategies were explored to enhance the flexibility and stretchability:constructing an inter-penetrating network,phase separation induced by ionic compounds,and pure conductive hydrogels formed through polar solvent additives and dry-annealing.These strategies synergistically enhance conductivity and flexibility by controlling interchain entanglement and redesigning the distribution of conjugated crystal regions and soft regions.The resulting hydrogels exhibit excellent conductivity(1.99-5.25 S/m),softness(elastic modulus as low as 280 Pa),and elasticity(tensile properties up to 800%).When used as epidermal or implantable bioelectrodes,they provided a soft interface,ensuring longer-lasting and more stable electromyo-gram,electrocardiogram,and electroencephalogram signals compared to commercial gel electrodes,with a signal-to-noise ratio of up to 20.0 dB.Therefore,the conducting polymer hydrogels developed in this study leverage the synergy between conductivity and flexibility,paving the way for further transformative applications in bioelectronics.
基金supported by the National Key Research and Development Program of China(2023YFB3608904)the National Natural Science Foundation of China(21835003 and 61704077)+7 种基金the Natural Science Foundation of Jiangsu Province(BE2019120 and BK20191374)the Foundation of Key Laboratory of Flexible Electronics of Zhejiang Province(2023FE002)the Natural Science Foundation of Jiangsu Higher Education Institutions of China(18KJB150025)the Program for Jiangsu SpeciallyAppointed Professor(RK030STP15001)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX21_0778,SJCX21_0298)the NUPT Scientific Foundation(NY219021 and NY219109)the Leading Talent of Technological Innovation of National Ten-Thousands Talents Program of Chinathe Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)。
文摘开发耐用且可靠的生物电极,用以采集高质量的生物电信号,已成为人体生理状态监测和人机交互领域的关键技术.然而,现有的生物电极多基于传统弹性基底,这导致了机械性能不匹配和低渗透性等问题,并且缺乏与生物皮肤类似的多方面属性和必要的协同特性.本研究中,我们报道了一种新型的基于自支撑导电全聚合物薄膜的超薄表皮生物电极(ASU-EBE).该电极将超一致性、优异的拉伸性和透气性集成于一体,展现了约475 S cm^(-1)的高导电性,约48%的出色拉伸性,与生物组织界面的超一致性以及优异的透气性.该电极的电子和机械性能得到提升,这归功于在PEDOT:PSS中引入水溶性聚氧化乙烯,以调节分子间π-π堆积距离,并促进纳米纤维结构的形成.因此,ASU-EBE在与皮肤接触时的阻抗远低于标准凝胶电极,使其成为复杂日常环境下长期医疗监测的理想选择.
