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Two [NiFeSe] variants were electrically wired by means of low\u2010potential viologen\u2010modified redox polymers and evaluated with respect to H<jats:sub>2<\/jats:sub>\u2010oxidation and stability against O<jats:sub>2<\/jats:sub> in the immobilized state. The two variants showed maximum current densities of (450\u00b184)\u2005\u03bcA\u2009cm<jats:sup>\u22122<\/jats:sup> for G491A and (476\u00b1172)\u2005\u03bcA\u2009cm<jats:sup>\u22122<\/jats:sup> for variant G941S on glassy carbon electrodes and a higher O<jats:sub>2<\/jats:sub> tolerance than the wild type. In addition, the polymer protected the enzyme from O<jats:sub>2<\/jats:sub> damage and high\u2010potential inactivation, establishing a triple protection for the bioanode. The use of gas\u2010diffusion bioanodes provided current densities for H<jats:sub>2<\/jats:sub>\u2010oxidation of up to 6.3\u2005mA\u2009cm<jats:sup>\u22122<\/jats:sup>. Combination of the gas\u2010diffusion bioanode with a bilirubin oxidase\u2010based gas\u2010diffusion O<jats:sub>2<\/jats:sub>\u2010reducing biocathode in a membrane\u2010free biofuel cell under anode\u2010limiting conditions showed unprecedented benchmark power densities of 4.4\u2005mW\u2009cm<jats:sup>\u22122<\/jats:sup> at 0.7\u2005V and an open\u2010circuit voltage of 1.14\u2005V even at moderate catalyst loadings, outperforming the previously reported system obtained with the [NiFeSe] wild type and the [NiFe] hydrogenase from <jats:italic>D.\u2005vulgaris<\/jats:italic> Miyazaki\u2005F.<\/jats:p>","DOI":"10.1002\/cssc.202000999","type":"journal-article","created":{"date-parts":[[2020,4,27]],"date-time":"2020-04-27T15:48:14Z","timestamp":1588002494000},"page":"3627-3635","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":13,"title":["Redox\u2010Polymer\u2010Wired [NiFeSe] Hydrogenase Variants with Enhanced O<sub>2<\/sub> Stability for Triple\u2010Protected High\u2010Current\u2010Density H<sub>2<\/sub>\u2010Oxidation Bioanodes"],"prefix":"10.1002","volume":"13","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5659-8556","authenticated-orcid":false,"given":"Adrian","family":"Ruff","sequence":"first","affiliation":[{"name":"Analytical Chemistry\u2014Center for Electrochemical Sciences (CES) Faculty of Chemistry and Biochemistry Ruhr-University Bochum  Universit\u00e4tsstr. 150 44780 Bochum Germany"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8842-8057","authenticated-orcid":false,"given":"Julian","family":"Szczesny","sequence":"additional","affiliation":[{"name":"Analytical Chemistry\u2014Center for Electrochemical Sciences (CES) Faculty of Chemistry and Biochemistry Ruhr-University Bochum  Universit\u00e4tsstr. 150 44780 Bochum Germany"}]},{"given":"Maria","family":"Vega","sequence":"additional","affiliation":[{"name":"Facultat de Bioci\u00e8ncies Universitat Aut\u00f2noma de Barcelona (UAB)  Carrer de la Vall Moronta 08193 Bellaterra Spain"}]},{"given":"Sonia","family":"Zacarias","sequence":"additional","affiliation":[{"name":"Instituto de Tecnologia Qu\u00edmica e Biol\u00f3gica Ant\u00f3nio Xavier (ITQB NOVA) Universidade NOVA de Lisboa  Av. da Rep\u00fablica 2780-157 Oeiras Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6170-451X","authenticated-orcid":false,"given":"Pedro M.","family":"Matias","sequence":"additional","affiliation":[{"name":"Instituto de Tecnologia Qu\u00edmica e Biol\u00f3gica Ant\u00f3nio Xavier (ITQB NOVA) Universidade NOVA de Lisboa  Av. da Rep\u00fablica 2780-157 Oeiras Portugal"},{"name":"Instituto de Biologia Experimental e Tecnol\u00f3gica (iBET)  Apartado 12 2780-901 Oeiras Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7602-9657","authenticated-orcid":false,"given":"S\u00e9bastien","family":"Gounel","sequence":"additional","affiliation":[{"name":"CNRS CRPP, UMR 5031 Univ. 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