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In Situ Determination of Photobioproduction of H2 by In2S3-[NiFeSe] Hydrogenase from Desulfovibrio vulgaris Hildenborough Using Only Visible Light

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† Instituto de Catálisis y Petroleoquímica, CSIC, c/Marie Curie 2, 28049 Madrid, Spain
‡ Instituto de Tecnologia Quimica e Biologica, Universidade Nova de Lisboa, Apartado 127, 2781-901 Oeiras, Portugal
*E-mail for M.P.: [email protected]
*E-mail for A.L.D.L.: [email protected]
Cite this: ACS Catal. 2016, 6, 9, 5691–5698
Publication Date (Web):July 22, 2016
https://doi.org/10.1021/acscatal.6b01512
Copyright © 2016 American Chemical Society
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Abstract

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An interesting strategy for photocatalytic production of hydrogen from water and sunlight is the formation of a hybrid photocatalyst that combines an inorganic semiconductor able to absorb in the visible light spectral range with an enzymatic catalyst for reducing protons. In this work we study how to optimize the interfacing of In2S3 particles with the soluble form of [NiFeSe] hydrogenase from Desulfovibrio vulgaris Hildenborough by means of its initial H2 photoproduction rate. The kinetics of the photocatalytic process was studied by membrane-inlet mass spectrometry, in order to optimize the interaction between both components of the hybrid photocatalyst. Membrane-inlet mass spectrometry allows measuring in the same experiment, for comparison, the rate of H2 production by the photocatalyst hybrid directly in the aqueous solution in real time and the result of a standard assay of the hydrogenase activity. An incubation period of 6 h with mild stirring of hydrogenase with In2S3 particles was necessary for optimal interaction of the enzyme molecules with the porous surface of the semiconductor. A turnover frequency of the NiFeSe hydrogenase (TOFHase) for H2 photobioproduction of 986 s–1 was measured under the optimized conditions. This means that the immobilized hydrogenase has a photocatalytic efficiency for H2 generation which is 94% of that obtained in the standard specific activity test of H2 production using reduced methyl viologen as an electron donor.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acscatal.6b01512.

  • Visual details of the In2S3 synthesis, pore area analysis, and electrochemical characterization (PDF)

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Cited By

This article is cited by 20 publications.

  1. Gabriel García-Molina Marcos PitaAntonio L. De Lacey . Novel Bioelectrocatalytic Strategies Based on Immobilized Redox Metalloenzymes on Tailored Electrodes. 2020,,, 207-229. https://doi.org/10.1021/bk-2020-1342.ch010
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  3. Cristina Tapia, Sergey Shleev, José Carlos Conesa, Antonio L. De Lacey, and Marcos Pita . Laccase-Catalyzed Bioelectrochemical Oxidation of Water Assisted with Visible Light. ACS Catalysis 2017, 7 (7) , 4881-4889. https://doi.org/10.1021/acscatal.7b01556
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  11. Yunhong Pi, Shuo Jin, Xiyi Li, Shi Tu, Zhong Li, Jing Xiao. Encapsulated [email protected] In2S3 tubular heterostructures for boosted visible-light-driven degradation of tetracycline. Applied Catalysis B: Environmental 2019, 256 , 117882. https://doi.org/10.1016/j.apcatb.2019.117882
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  15. Liyun Zhang, Stephen E. Beaton, Stephen B. Carr, Fraser A. Armstrong. Direct visible light activation of a surface cysteine-engineered [NiFe]-hydrogenase by silver nanoclusters. Energy & Environmental Science 2018, 11 (12) , 3342-3348. https://doi.org/10.1039/C8EE02361A
  16. Dong Heon Nam, Jenny Z. Zhang, Virgil Andrei, Nikolay Kornienko, Nina Heidary, Andreas Wagner, Kenichi Nakanishi, Katarzyna P. Sokol, Barnaby Slater, Ingo Zebger, Stephan Hofmann, Juan C. Fontecilla‐Camps, Chan Beum Park, Erwin Reisner. Solar Water Splitting with a Hydrogenase Integrated in Photoelectrochemical Tandem Cells. Angewandte Chemie 2018, 130 (33) , 10755-10759. https://doi.org/10.1002/ange.201805027
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  18. Sónia Zacarias, Marisela Vélez, Marcos Pita, Antonio L. De Lacey, Pedro M. Matias, Inês A.C. Pereira. Characterization of the [NiFeSe] hydrogenase from Desulfovibrio vulgaris Hildenborough. 2018,,, 169-201. https://doi.org/10.1016/bs.mie.2018.10.003
  19. Jie Xu, Bifu Luo, Wei Gu, Yaping Jian, Feilong Wu, Yubin Tang, Hao Shen. Fabrication of In 2 S 3 /NaTaO 3 composites for enhancing the photocatalytic activity toward the degradation of tetracycline. New Journal of Chemistry 2018, 42 (7) , 5052-5058. https://doi.org/10.1039/C7NJ05123A
  20. Sheng-qi Guo, Ling-chang Wang, Chen-guang Zhang, Gao-can Qi, Bing-chuan Gu, Lu Liu, Zhi-hao Yuan. A unique semiconductor–carbon–metal hybrid structure design as a counter electrode in dye-sensitized solar cells. Nanoscale 2017, 9 (20) , 6837-6845. https://doi.org/10.1039/C7NR00718C

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