Light-Driven Catalytic Upgrading of Butanol in a Biohybrid Photoelectrochemical SystemClick to copy article linkArticle link copied!
Abstract

This paper reports the design and preparation of a biohybrid photoelectrochemical cell (PEC) that can drive the tandem enzymatic oxidation and aldol condensation of n-butanol (BuOH) to C8 2-ethylhexenal (2-EH). In this work, BuOH was first oxidized to n-butyraldehyde (BA) by the alcohol oxidase enzyme (AOx), concurrently generating hydrogen peroxide (H2O2). To preserve enzyme activity and increase kinetics nearly 2-fold, the H2O2 was removed by oxidation at a bismuth vanadate (BiVO4) photoanode. Organocatalyzed aldol condensation of C4 BA to C8 2-EH improved the overall BuOH conversion to 6.2 ± 0.1% in a biased PEC after 16 h. A purely light-driven, unbiased PEC showed 3.1 ± 0.1% BuOH conversion, or ∼50% of that obtained from the biased system. Replacing AOx with the enzyme alcohol dehydrogenase (ADH), which requires the diffusional nicotinamide adenine dinucleotide cofactor (NAD+/NADH), resulted in only 0.2% BuOH conversion due to NAD+ dimerization at the photoanode. Lastly, the application of more positive biases with the biohybrid AOx PEC led to measurable production of H2 at the cathode, but at the cost of lower BA and 2-EH yields due to both product overoxidation and decreased enzyme activity.
Cited By
Smart citations by scite.ai include citation statements extracted from the full text of the citing article. The number of the statements may be higher than the number of citations provided by ACS Publications if one paper cites another multiple times or lower if scite has not yet processed some of the citing articles.
This article is cited by 18 publications.
- Alexander W. Harris, Albert Harguindey, Ryan E. Patalano, Shambojit Roy, Omer Yehezkeli, Andrew P. Goodwin, Jennifer N. Cha. Investigating Protein–Nanocrystal Interactions for Photodriven Activity. ACS Applied Bio Materials 2020, 3
(2)
, 1026-1035. https://doi.org/10.1021/acsabm.9b01025
- Caidi Jin, Mingxia Han, Yuheng Wu, Shurong Wang. Solar-driven photoelectrochemical conversion of biomass: recent progress, mechanistic insights and potential scalability. Energy & Environmental Science 2024, 17
(20)
, 7459-7511. https://doi.org/10.1039/D4EE02332C
- Sıdıka Çetinkaya, Levent Özcan, Leonardo Palmisano, Sedat Yurdakal. Partial Photoelectrocatalytic Oxidation of 3‐Methylpiridine in Green Conditions by Nanotube/Nanowire Ti/TiO
2
Plates Prepared in Aqueous, Glycerol, or Ethylene Glycol Medium. ChemCatChem 2024, 16
(18)
https://doi.org/10.1002/cctc.202400755
- Marianna Bellardita, Vittorio Loddo, Vincenzo Augugliaro, Leonardo Palmisano, Sedat Yurdakal. Selective photocatalytic and photoelectrocatalytic synthesis of valuable compounds in aqueous medium. Catalysis Today 2024, 432 , 114587. https://doi.org/10.1016/j.cattod.2024.114587
- Mor Shemesh, Yifat Cohen, Roy Cohen, Matan M. Meirovich, Nidaa S. Herzallh, Oleg Chmelnik, Yuval Shoham, Omer Yehezkeli. Light-driven and bias-free direct conversion of cellulose to electrical power. Cell Reports Physical Science 2023, 4
(9)
, 101546. https://doi.org/10.1016/j.xcrp.2023.101546
- Sıdıka Çetinkaya, Levent Özcan, Oğuzhan Alagöz, Leonardo Palmisano, Sedat Yurdakal. Selective photoelectrocatalytic oxidation of 3-methylpyridine to vitamin B
3
by WO
3
decorated nanotube-structured TiO
2. Chemical Communications 2023, 59
(38)
, 5741-5744. https://doi.org/10.1039/D3CC01394D
- Si-Yang Li, Ke-Fu Huang, Zhi-Yong Tang, Jing-Hao Wang. Photoelectrocatalytic organic synthesis: a versatile method for the green production of building-block chemicals. Journal of Materials Chemistry A 2023, 11
(7)
, 3281-3296. https://doi.org/10.1039/D2TA09430D
- Zhu Chen, Yuguang Wang, Haina Cheng, Hongbo Zhou. Integrated chemo‐ and biocatalytic processes: a new fashion toward renewable chemicals production from lignocellulosic biomass. Journal of Chemical Technology & Biotechnology 2023, 98
(2)
, 331-345. https://doi.org/10.1002/jctb.7241
- Sedat Yurdakal, Oğuzhan Alagöz, Levent Özcan, Leonardo Palmisano. Selective photoelectrocatalytic transformations of organic compounds. 2023, 361-420. https://doi.org/10.1016/B978-0-12-823989-6.00001-1
- Andoni Rodriguez‐Abetxuko, Antonio Reifs, Daniel Sánchez‐deAlcázar, Ana Beloqui. A Versatile Chemoenzymatic Nanoreactor that Mimics NAD(P)H Oxidase for the In Situ Regeneration of Cofactors. Angewandte Chemie 2022, 134
(39)
https://doi.org/10.1002/ange.202206926
- Andoni Rodriguez‐Abetxuko, Antonio Reifs, Daniel Sánchez‐deAlcázar, Ana Beloqui. A Versatile Chemoenzymatic Nanoreactor that Mimics NAD(P)H Oxidase for the In Situ Regeneration of Cofactors. Angewandte Chemie International Edition 2022, 61
(39)
https://doi.org/10.1002/anie.202206926
- Zhenfu Wang, Yang Hu, Songping Zhang, Yan Sun. Artificial photosynthesis systems for solar energy conversion and storage: platforms and their realities. Chemical Society Reviews 2022, 51
(15)
, 6704-6737. https://doi.org/10.1039/D1CS01008E
- Daniel Antón-García, Esther Edwardes Moore, Mark A. Bajada, Annika Eisenschmidt, Ana R. Oliveira, Inês A. C. Pereira, Julien Warnan, Erwin Reisner. Photoelectrochemical hybrid cell for unbiased CO2 reduction coupled to alcohol oxidation. Nature Synthesis 2022, 1
(1)
, 77-86. https://doi.org/10.1038/s44160-021-00003-2
- Nidaa S. Herzallh, Yifat Cohen, Roy Cohen, Oleg Chmelnik, Yuval Shoham, Omer Yehezkeli. Cellulose to electricity conversion by an enzymatic biofuel cell. Sustainable Energy & Fuels 2021, 5
(18)
, 4580-4586. https://doi.org/10.1039/D1SE00896J
- Shuobo Wang, Xu Han, Yihe Zhang, Na Tian, Tianyi Ma, Hongwei Huang. Inside‐and‐Out Semiconductor Engineering for CO
2
Photoreduction: From Recent Advances to New Trends. Small Structures 2021, 2
(1)
https://doi.org/10.1002/sstr.202000061
- Nidaa Shrara Herzallh, Yifat Cohen, Dina Mukha, Ehud Neumann, Dorit Michaeli, Rachel Nechushtai, Omer Yehezkeli. Photosynthesis Z-Scheme biomimicry: Photosystem I/BiVO4 photo-bioelectrochemical cell for donor-free bias-free electrical power generation. Biosensors and Bioelectronics 2020, 168 , 112517. https://doi.org/10.1016/j.bios.2020.112517
- Yan-Chen Wu, Ren-Jie Song, Jin-Heng Li. Recent advances in photoelectrochemical cells (PECs) for organic synthesis. Organic Chemistry Frontiers 2020, 7
(14)
, 1895-1902. https://doi.org/10.1039/D0QO00486C
- Alexander W. Harris, Jennifer N. Cha. Bridging bio-nano interactions with photoactive biohybrid energy systems. Molecular Systems Design & Engineering 2020, 5
(6)
, 1088-1097. https://doi.org/10.1039/D0ME00031K
Article Views are the COUNTER-compliant sum of full text article downloads since November 2008 (both PDF and HTML) across all institutions and individuals. These metrics are regularly updated to reflect usage leading up to the last few days.
Citations are the number of other articles citing this article, calculated by Crossref and updated daily. Find more information about Crossref citation counts.
The Altmetric Attention Score is a quantitative measure of the attention that a research article has received online. Clicking on the donut icon will load a page at altmetric.com with additional details about the score and the social media presence for the given article. Find more information on the Altmetric Attention Score and how the score is calculated.