Jing Tang, Rebecka Maria Larsen Werchmeister, Loredana Preda, Wei Huang, Zhiyong Zheng, Silke Leimkühler, Ulla Wollenberger, Xinxin Xiao, Christian Engelbrekt, Jens Ulstrup, Jingdong Zhang
- 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 (j(m)) for sulfite oxidation reaching 24.4 +/- 0.3 mu A to 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 significantWe 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 (j(m)) for sulfite oxidation reaching 24.4 +/- 0.3 mu A to 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 (k(cat): 25.6 +/- 0.3 s(-1)) and efficiency (k(cat)/K-m: 0.231 +/- 0.003 s(-1) mu M-1) compared to the reported hSO bioelectrodes. The assembly of the hSO bioanode and a commercial platinum biocathode allows the construction of sulfite/O-2 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 mu W cm(-2) (122 +/- 12 mW m(-3)) at 30 degrees C, which exceeds the best reported value by more than 6 times.…
MetadatenAuthor details: | Jing TangORCiD, Rebecka Maria Larsen Werchmeister, Loredana Preda, Wei HuangORCiD, Zhiyong ZhengORCiD, Silke LeimkühlerORCiDGND, Ulla WollenbergerORCiDGND, Xinxin XiaoORCiD, Christian EngelbrektORCiD, Jens UlstrupORCiD, Jingdong ZhangORCiD |
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DOI: | https://doi.org/10.1021/acscatal.9b01715 |
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ISSN: | 2155-5435 |
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Title of parent work (English): | ACS catalysis |
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Publisher: | American Chemical Society |
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Place of publishing: | Washington |
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Publication type: | Article |
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Language: | English |
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Date of first publication: | 2019/07/05 |
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Publication year: | 2019 |
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Release date: | 2021/01/14 |
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Tag: | carbon paper; direct electron transfer; enzymatic biofuel cell; reduced graphene oxide; sulfite oxidase |
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Volume: | 9 |
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Issue: | 7 |
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Number of pages: | 23 |
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First page: | 6543 |
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Last Page: | 6554 |
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Funding institution: | Danish Council for Independent ResearchDet Frie Forskningsrad (DFF) [DFF 4093-00297]; China Scholarship Council (CSC)China Scholarship Council [201706220080, 201606130019]; Independent Research Fund Denmark [DFF-5054-00107]; Deutsche Forschungsgemeinschaft (DFG, German Research Foundation (DFG) [EXC 314/2, EXC 2008/1, 390540038]; Russian Science FoundationRussian Science Foundation (RSF) [17-13-01274] |
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Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Biochemie und Biologie |
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DDC classification: | 5 Naturwissenschaften und Mathematik / 57 Biowissenschaften; Biologie / 570 Biowissenschaften; Biologie |
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Peer review: | Referiert |
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