Electrical Wiring of Glucose Oxidase by Reconstitution of FAD-Modified Monolayers Assembled onto Au-Electrodes

Willner, Itamar; Heleg-Shabtai, Vered; Blonder, Ron; Katz, Eugenii; Tao, Guoliang; Bückmann, Andreas F.; Heller, Adam

doi:10.1021/ja9608611

Cited by 393 publications

(292 citation statements)

References 25 publications

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“…However, functionalization of surfaces by redox-active compounds is a common electrochemical theme. For example, flavin-based linkers can wire glucose oxidase to gold nanoparticles (34), electrodes modified to contain phenazines increase electron transfer rates from bacteria to electrodes (35), and sorption of polyaniline-based compounds to stainless steel protects surfaces from corrosion (36). Flavins, and phenazines produced by Pseudomonas representatives (37) should be viewed as compounds that have been present not only in the soluble phase, but on surfaces in experiments where analytical methods indicated they were removed.…”

Section: Resultsmentioning

confidence: 99%

Shewanella secretes flavins that mediate extracellular electron transfer

Marsili¹,

Baron²,

Shikhare³

et al. 2008

Proc. Natl. Acad. Sci. U.S.A.

1,667

1,507

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Bacteria able to transfer electrons to metals are key agents in biogeochemical metal cycling, subsurface bioremediation, and corrosion processes. More recently, these bacteria have gained attention as the transfer of electrons from the cell surface to conductive materials can be used in multiple applications. In this work, we adapted electrochemical techniques to probe intact biofilms of Shewanella oneidensis MR-1 and Shewanella sp. MR-4 grown by using a poised electrode as an electron acceptor. This approach detected redox-active molecules within biofilms, which were involved in electron transfer to the electrode. A combination of methods identified a mixture of riboflavin and riboflavin-5 -phosphate in supernatants from biofilm reactors, with riboflavin representing the dominant component during sustained incubations (>72 h). Removal of riboflavin from biofilms reduced the rate of electron transfer to electrodes by >70%, consistent with a role as a soluble redox shuttle carrying electrons from the cell surface to external acceptors. Differential pulse voltammetry and cyclic voltammetry revealed a layer of flavins adsorbed to electrodes, even after soluble components were removed, especially in older biofilms. Riboflavin adsorbed quickly to other surfaces of geochemical interest, such as Fe(III) and Mn(IV) oxy(hydr)oxides. This in situ demonstration of flavin production, and sequestration at surfaces, requires the paradigm of soluble redox shuttles in geochemistry to be adjusted to include binding and modification of surfaces. Moreover, the known ability of isoalloxazine rings to act as metal chelators, along with their electron shuttling capacity, suggests that extracellular respiration of minerals by Shewanella is more complex than originally conceived.bioelectrochemistry ͉ biogeochemistry ͉ redox mediator ͉ riboflavin

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Section: Resultsmentioning

confidence: 99%

Shewanella secretes flavins that mediate extracellular electron transfer

Marsili¹,

Baron²,

Shikhare³

et al. 2008

Proc. Natl. Acad. Sci. U.S.A.

1,667

1,507

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“…Neste processo, o mediador é ligado diretamente ao centro redox da enzima, sendo a apoenzima (enzima sem o centro redox) posteriormente reconstituída sobre a superfície do eletrodo, de acordo com o esquema mostrado na Figura 8 118,120 . Empregando-se este método foi construído um sensor para glicose 121 , onde o mediador pirroloquinolina quinona (PQQ) foi covalentemente ligado a uma monocamada de cisteamina e, posteriormente, reagido com um derivado amina do FAD, o N(6)-(2-aminoethyl)-FAD. A apo-glicose oxidase foi então reconstituída sobre esta superfície, apresentando propriedades bioeletrocatalíticas.…”

Section: Eletrodos Modificados Com Sam -Análise De Compostos Orgânicosunclassified

Emprego de monocamadas auto-organizadas no desenvolvimento de sensores eletroquímicos

Freire¹,

Pessôa²,

Kubota³

2003

Quím. Nova

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Recebido em 18/7/02; aceito 9/10/02 SELF-ASSEMBLED MONOLAYERS APPLICATIONS FOR THE DEVELOPMENT OF ELECTROCHEMICAL SENSORS. Selfassembled monolayers (SAMs) modified electrodes exhibit unique behavior that can greatly benefit electrochemical sensing. This brief review highlights the applications of SAM modified electrodes in electroanalytical chemistry. After a general introduction, which includes the approaches for SAM development, different electrochemical systems for detecting inorganic and organic species are described and discussed. Special attention to the coupling of biological sensing element to the SAM is given, which can selectively recognize the analyte. Future prospects are also evaluated.Keywords: chemically modified electrodes; self-assembled monolayers; electrochemical sensors. INTRODUÇÃOO desenvolvimento de sensores eletroquímicos é uma das áreas de maior e mais rápido crescimento dentro da Química Analítica, principalmente devido aos novos desafios impostos por amostras de interesse industrial, clínico e ambiental, que têm levado a uma crescente busca por sensores com melhores características, tais como alta sensibilidade, seletividade e estabilidade [1][2][3][4][5][6][7][8] . Apesar da grande versatilidade e perspectivas apresentadas pelos sensores eletroquímicos, a utilidade de um eletrodo é muitas vezes limitada devido a uma passivação gradual de sua superfície, que é conseqüência principalmente da adsorção dos produtos da própria reação de óxido-redução utilizada na detecção, ou ainda, dos sub-produtos destas reações que podem se polimerizar e se depositar sobre a superfície dos eletrodos 6 . Além disso, a sensibilidade de muitos analitos importantes pode ser prejudicada em função da cinética de transferência de elétrons entre estes compostos e os materiais dos eletrodos ser excessivamente lenta 9 . Uma outra limitação é a dificuldade de discriminar entre compostos alvos que possuam características redox similares 9 . Uma área que oferece grande potencial para minimizar os problemas acima descritos, e conseqüentemente para aumentar a aplicabilidade e eficiência dos sensores eletroquímicos, é a que compreende os chamados eletrodos quimicamente modificados (EQM) 9,10 . A habilidade para controlar e manipular deliberadamente as propriedades das superfícies dos eletrodos pode proporcionar uma variedade de efeitos atrativos, levando a superfícies com características que podem contornar efetivamente muitos dos problemas apresentados pelos sensores eletroquímicos tradicionais.Estudos experimentais, suportados pela teoria, têm mostrado que a velocidade de transferência de elétrons pode ser sensivelmente afetada em função da modificação da superfície dos eletrodos 11. A classificação das reações do eletrodo pode ser feita com base no grau de interação entre os reagentes e a superfície do eletrodo, ocorrida durante o estado de transição da transferência de elétrons 12 . Os processos de transferência de elétrons onde as interações entre as espécies reagentes e a superfície do eletrodo são fracas e não es...

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“…The electrical contacting of redox proteins with electrodes attracted substantial research efforts directed to the development of amperometric biosensors [26][27][28][29] or biofuel cell elements [30][31][32][33][34][35] . Different methods to integrate redox proteins with electrodes in electrically contacted configurations were developed, including the modification of the proteins with relay units 36,37 , the reconstitution of the proteins on relay-cofactor units [38][39][40] and the immobilization of the proteins in redox-active polymer matrices 41 . Related principles were implemented to electrically wire PSII with electrode surfaces.…”

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confidence: 99%

Integrated photosystem II-based photo-bioelectrochemical cells

et al. 2012

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Photosynthesis is a sustainable process that converts light energy into chemical energy. substantial research efforts are directed towards the application of the photosynthetic reaction centres, photosystems I and II, as active components for the light-induced generation of electrical power or fuel products. nonetheless, no integrated photo-bioelectrochemical device that produces electrical power, upon irradiation of an aqueous solution that includes two inter-connected electrodes is known. Here we report the assembly of photobiofuel cells that generate electricity upon irradiation of biomaterial-functionalized electrodes in aqueous solutions. The cells are composed of electrically contacted photosystem II-functionalized photoanodes and an electrically wired bilirubin oxidase/carbon nanotubes-modified cathode. Illumination of the photoanodes yields the oxidation of water to o 2 and the transfer of electrons through the external circuit to the cathode, where o 2 is re-reduced to water.

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Electrical Wiring of Glucose Oxidase by Reconstitution of FAD-Modified Monolayers Assembled onto Au-Electrodes

Cited by 393 publications

References 25 publications

Shewanella secretes flavins that mediate extracellular electron transfer

Shewanella secretes flavins that mediate extracellular electron transfer

Emprego de monocamadas auto-organizadas no desenvolvimento de sensores eletroquímicos

Integrated photosystem II-based photo-bioelectrochemical cells

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