Three-Dimensional Sulfite Oxidase Bioanodes Based on Graphene Functionalized Carbon Paper for Sulfite/O2 Biofuel CellsClick to copy article linkArticle link copied!
- Jing TangJing TangDepartment of Chemistry, Technical University of Denmark, 2800 Kongens Lyngby, DenmarkMore by Jing Tang
- Rebecka Maria Larsen WerchmeisterRebecka Maria Larsen WerchmeisterDepartment of Chemistry, Technical University of Denmark, 2800 Kongens Lyngby, Denmark
- Loredana PredaLoredana PredaDepartment of Molecular Enzymology, University of Potsdam, 14476 Potsdam−Golm, GermanyInstitute of Physical Chemistry of the Romanian Academy, 202 Spl. Independentei, 060021 Bucharest, RomaniaMore by Loredana Preda
- Wei HuangWei HuangDepartment of Chemistry, Technical University of Denmark, 2800 Kongens Lyngby, DenmarkMore by Wei Huang
- Zhiyong ZhengZhiyong ZhengDepartment of Chemistry, Technical University of Denmark, 2800 Kongens Lyngby, DenmarkMore by Zhiyong Zheng
- Silke LeimkühlerSilke LeimkühlerDepartment of Molecular Enzymology, University of Potsdam, 14476 Potsdam−Golm, GermanyMore by Silke Leimkühler
- Ulla WollenbergerUlla WollenbergerDepartment of Molecular Enzymology, University of Potsdam, 14476 Potsdam−Golm, GermanyMore by Ulla Wollenberger
- Xinxin XiaoXinxin XiaoDepartment of Chemistry, Technical University of Denmark, 2800 Kongens Lyngby, DenmarkMore by Xinxin Xiao
- Christian EngelbrektChristian EngelbrektDepartment of Chemistry, Technical University of Denmark, 2800 Kongens Lyngby, DenmarkMore by Christian Engelbrekt
- Jens UlstrupJens UlstrupDepartment of Chemistry, Technical University of Denmark, 2800 Kongens Lyngby, DenmarkMore by Jens Ulstrup
- Jingdong Zhang*Jingdong Zhang*E-mail: [email protected]Department of Chemistry, Technical University of Denmark, 2800 Kongens Lyngby, DenmarkMore by Jingdong Zhang
Abstract

We have developed a three-dimensional (3D) graphene electrode suitable for the immobilization of human sulfite oxidase (hSO), which catalyzes the electrochemical oxidation of sulfite via direct electron transfer (DET). The electrode is fabricated by drop-casting graphene-polyethylenimine (G-P) composites on carbon papers (CPs) precoated with graphene oxide (GO). The negatively charged hSO can be adsorbed electrostatically on the positively charged matrix (G-P) on CP electrodes coated with GO (CPG), with a proper orientation for accelerated DET. Notably, further electrochemical reduction of G-P on CPG electrodes leads to a 9-fold increase of the saturation catalytic current density (jm) for sulfite oxidation reaching 24.4 ± 0.3 μA cm–2, the highest value among reported DET-based hSO bioelectrodes. The increased electron transfer rate plays a dominating role in the enhancement of direct enzymatic current because of the improved electric contact of hSO with the electrode. The optimized hSO bioelectrode shows a significant catalytic rate (kcat: 25.6 ± 0.3 s–1) and efficiency (kcat/Km: 0.231 ± 0.003 s–1 μM–1) compared to the reported hSO bioelectrodes. The assembly of the hSO bioanode and a commercial platinum biocathode allows the construction of sulfite/O2 enzymatic biofuel cells (EBFCs) with flowing fuels. The optimized EBFC displays an open-circuit voltage (OCV) of 0.64 ± 0.01 V and a maximum power density of 61 ± 6 μW cm–2 (122 ± 12 mW m–3) at 30 °C, which exceeds the best reported value by more than 6 times.
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