TY - JOUR
T1 - Engineering bio-interfaces for the direct electron transfer of Myriococcum thermophilum cellobiose dehydrogenase
T2 - Towards a mediator-less biosupercapacitor/biofuel cell hybrid
AU - Yan, Xiaomei
AU - Tang, Jing
AU - Ma, Su
AU - Tanner, David
AU - Ludwig, Roland
AU - Ulstrup, Jens
AU - Xiao, Xinxin
N1 - Publisher Copyright:
© 2022 The Authors
PY - 2022/8/15
Y1 - 2022/8/15
N2 - Direct electron transfer (DET) of enzymes on electrode surfaces is highly desirable both for fundamental mechanistic studies and to achieve membrane- and mediator-less bioenergy harvesting. In this report, we describe the preparation and comprehensive structural and electrochemical characterization of a three-dimensional (3D) graphene-based carbon electrode, onto which the two-domain redox enzyme Myriococcum thermophilum cellobiose dehydrogenase (MtCDH) is immobilized. The electrode is prepared by an entirely novel method, which combines in a single step electrochemical reduction of graphene oxide (GO) and simultaneous electrodeposition of positively charged polyethylenimine (PEI), resulting in a well dispersed MtCDH surface. The resulting MtCDH bio-interface was characterized structurally in detail, optimized, and found to exhibit a DET maximum current density of 7.7 ± 0.9 μA cm−2 and a half-lifetime of 48 h for glucose oxidation, attributed to favorable MtCDH surface orientation. A dual, entirely DET-based enzymatic biofuel cell (EBFC) was constructed with a MtCDH bioanode and a Myrothecium verrucaria bilirubin oxidase (MvBOD) biocathode. The EBFC delivers a maximum power density (Pmax) of 7.6 ± 1.3 μW cm−2, an open-circuit voltage (OCV) of 0.60 V, and an operational lifetime over seven days, which exceeds most reported CDH based DET-type EBFCs. A biosupercapacitor/EBFC hybrid was also constructed and found to register maximum power densities 62 and 43 times higher than single glucose/air and lactose/air EBFCs, respectively. This hybrid also shows excellent operational stability with self-charging/discharging over at least 500 cycles.
AB - Direct electron transfer (DET) of enzymes on electrode surfaces is highly desirable both for fundamental mechanistic studies and to achieve membrane- and mediator-less bioenergy harvesting. In this report, we describe the preparation and comprehensive structural and electrochemical characterization of a three-dimensional (3D) graphene-based carbon electrode, onto which the two-domain redox enzyme Myriococcum thermophilum cellobiose dehydrogenase (MtCDH) is immobilized. The electrode is prepared by an entirely novel method, which combines in a single step electrochemical reduction of graphene oxide (GO) and simultaneous electrodeposition of positively charged polyethylenimine (PEI), resulting in a well dispersed MtCDH surface. The resulting MtCDH bio-interface was characterized structurally in detail, optimized, and found to exhibit a DET maximum current density of 7.7 ± 0.9 μA cm−2 and a half-lifetime of 48 h for glucose oxidation, attributed to favorable MtCDH surface orientation. A dual, entirely DET-based enzymatic biofuel cell (EBFC) was constructed with a MtCDH bioanode and a Myrothecium verrucaria bilirubin oxidase (MvBOD) biocathode. The EBFC delivers a maximum power density (Pmax) of 7.6 ± 1.3 μW cm−2, an open-circuit voltage (OCV) of 0.60 V, and an operational lifetime over seven days, which exceeds most reported CDH based DET-type EBFCs. A biosupercapacitor/EBFC hybrid was also constructed and found to register maximum power densities 62 and 43 times higher than single glucose/air and lactose/air EBFCs, respectively. This hybrid also shows excellent operational stability with self-charging/discharging over at least 500 cycles.
KW - Biosupercapacitor
KW - Cellobiose dehydrogenase
KW - Direct electron transfer
KW - Enzymatic biofuel cell
KW - Graphene
KW - Polyethylenimine
UR - http://www.scopus.com/inward/record.url?scp=85129695004&partnerID=8YFLogxK
U2 - 10.1016/j.bios.2022.114337
DO - 10.1016/j.bios.2022.114337
M3 - Journal article
C2 - 35537312
AN - SCOPUS:85129695004
SN - 0956-5663
VL - 210
JO - Biosensors and Bioelectronics
JF - Biosensors and Bioelectronics
M1 - 114337
ER -