CO2 utilization by formate dehydrogenase biocatalyst in a PhotoElectrochemical Cell (CO2BioPEC) (completed)

• Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios; Backe, Paul Hoff; Ruan, Qiushi; Tang, Junwang & Rise, Frode [Show all 8 contributors for this article] (2021). In situ cofactor regeneration enables selective CO2 reduction in a stable and efficient enzymatic photoelectrochemical cell. Applied Catalysis B: Environmental. ISSN 0926-3373. 296. doi: 10.1016/j.apcatb.2021.120349. Full text in Research Archive Show summary

  Mimicking natural photosynthesis by direct photoelectrochemical (PEC) reduction of CO2 to chemicals and fuels requires complex cell assemblies with limitations in selectivity, efficiency, cost, and stability. Here, we present a breakthrough cathode utilizing an oxygen tolerant formate dehydrogenase enzyme derived from clostridium carboxidivorans and coupled to a novel and efficient in situ nicotinamide adenine dinucleotide (NAD+/NADH) regeneration mechanism through interfacial electrochemistry on g-C3N4 films. We demonstrate stable (20 h) aerobic PEC CO2-to-formate reduction at close to 100 % faradaic efficiency and unit selectivity in a bio-hybrid PEC cell of minimal engineering with optimized Ta3N5 nanotube photoanode powered by simulated sunlight with a solar to fuel efficiency of 0.063 %, approaching that of natural photosynthesis.

• Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios; Risbakk, Sanne; Yang, Mingyi; Backe, Paul Hoff & Grandcolas, Mathieu [Show all 8 contributors for this article] (2020). High performance and toxicity assessment of Ta3N5 nanotubes for photoelectrochemical water splitting. Catalysis Today. ISSN 0920-5861. doi: 10.1016/j.cattod.2019.12.031. Full text in Research Archive Show summary

  In this work, Co-based cocatalysts are electrodeposited on mesoporous Ta3N5 nanotubes. The electrodeposition time is varied and the optimized photoelectrode reaches a photocurrent density of 6.3 mA/cm2 at 1.23 V vs. SHE, under simulated solar illumination of 1 Sun, in 1 M NaOH. The best performing electrode, apart from the high photocurrent density, shows improved stability under intense photoelectrochemical water splitting conditions. The dual function of the cocatalyst to improve not only the photoelectrochemical performance, but also the stability, is highlighted. Moreover, we adopted a simple protocol to assess the toxicity of Co and Ta contained nanostructured materials (representing used photoelectrodes) employing the human cell line HeLa S3 as target cells.

• Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios; Vøllestad, Einar; Ruan, Qiushi; Tang, Junwang & Norby, Truls Eivind (2019). Hydrogen from wet air and sunlight in a tandem photoelectrochemical cell. International Journal of Hydrogen Energy. ISSN 0360-3199. 44(2), p. 587–593. doi: 10.1016/j.ijhydene.2018.11.030. Full text in Research Archive
• Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios; Jensen, Ingvild Julie Thue; Grandcolas, Mathieu & Norby, Truls Eivind (2019). Ta3N5/Co(OH)x composites as photocatalysts for photoelectrochemical water splitting. Photochemical and Photobiological Sciences. ISSN 1474-905X. 18(4), p. 837–844. doi: 10.1039/c8pp00312b. Full text in Research Archive
• Grandcolas, Mathieu; Wabende, Brian; Yang, Juan; Mei, Sen; Xu, Kaiqi & Norby, Truls Eivind [Show all 7 contributors for this article] (2019). Preparation of TiO2 rutile nanorods decorated with cobalt oxide nanoparticles for solar photoelectrochemical activity. Materials Letters. ISSN 0167-577X. 247, p. 1–3. doi: 10.1016/j.matlet.2019.03.087. Full text in Research Archive Show summary

  The present paper investigates the preparation of titanium dioxide (TiO2) nanorods decorated with cobalt oxide (Co3O4) nanoparticles and its application as solar photoelectrocatalyst. TiO2 rutile nanorods have been prepared on conductive glass via a hydrothermal reaction in acidic media, shaped as squared rods with an average length of 1.7 µm and thicknesses between 50 and 120 nm. Co3O4 nanoparticles with an average diameter of 30 nm were synthesized using a simple precipitation method. Spin coating the nanoparticles on the TiO2 nanorods shows enhanced photocurrents under simulated solar light up to 1.3 mA/cm2 at 1.6 V vs. SHE.

• Sun, Xinwei; Xu, Kaiqi; Fleischer, Christian; Liu, Xin; Grandcolas, Mathieu & Strandbakke, Ragnar [Show all 9 contributors for this article] (2018). Earth-abundant electrocatalysts in proton exchange membrane electrolyzers. Catalysts. ISSN 2073-4344. 8:657(12), p. 1–41. doi: 10.3390/catal8120657. Full text in Research Archive Show summary

  In order to adopt water electrolyzers as a main hydrogen production system, it is critical to develop inexpensive and earth-abundant catalysts. Currently, both half-reactions in water splitting depend heavily on noble metal catalysts. This review discusses the proton exchange membrane (PEM) water electrolysis (WE) and the progress in replacing the noble-metal catalysts with earth-abundant ones. The efforts within this field for the discovery of efficient and stable earth-abundant catalysts (EACs) have increased exponentially the last few years. The development of EACs for the oxygen evolution reaction (OER) in acidic media is particularly important, as the only stable and efficient catalysts until now are noble-metal oxides, such as IrOx and RuOx. On the hydrogen evolution reaction (HER) side, there is significant progress on EACs under acidic conditions, but there are very few reports of these EACs employed in full PEM WE cells. These two main issues are reviewed, and we conclude with prospects for innovation in EACs for the OER in acidic environments, as well as with a critical assessment of the few full PEM WE cells assembled with EACs.

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• Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios; Norby, Truls Eivind & Bjørheim, Tor Svendsen (2019). Ta3N5 nanotubes loaded with Co(OH)x/Co-Pi-high photocurrent densities and improved photocorrosion resistance .
• Mei, Sen; mingyi, yang; yang, juan; P.H., Backe; Wabende, Brian & Grandcolas, Mathieu [Show all 8 contributors for this article] (2019). Formate dehydrogenase immobilised on PEC cathode for CO2 Utilization . Show summary

  Recently, the direct conversion of the waste CO2 emission as feedstock into valuable chemicals has attracted increasing research interest world widely. A number of approaches such as chemical, electrochemical, photochemical or biological routes have used CO2 as a sustainable carbon resource for the production of chemicals. In our work, a novel hybrid photoelectrochemical cell by using formate dehydrogenase (FDH) as biocatalyst was applied, to convert CO2 into energy-rich compounds. Therefore, it becomes imperative to immobilise FDH onto the surface of cathode with high electron transfer efficiency. In this work, several metallic substrates and carbon-based materials, such as carbon nanotube and graphene coating, were selected as electrodes to immobilise FDH enzyme onto their surfaces. In order to achieve an efficient immobilization, both chemical and physical functionalization were applied to the selected surfaces. A fast antibody-based dot blot method was established to detect the efficiency of the immobilization of the proteins. The activity of the purified enzymes was investigated by measuring the conversion ratio of NADH to NAD+. Preliminary results showed that the attachment of enzymes strongly depends on surface treatment of the electrodes. The immobilization of the enzymes was significantly improved by forming chemical bonding between the enzyme and the carbon-based materials. The electron transport and activity of the enzyme on the electrode surface will be investigated.

• Sun, Xinwei; Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios & Norby, Truls Eivind (2018). Can hydroxyl radicals travel far? Gas phase transport and detection after photocatalytic generation at TiO2 nanorods.
• Grandcolas, Mathieu; Wabende, Brian; Yang, Juan; Mei, Sen; Xu, Kaiqi & Chatzitakis, Athanasios Eleftherios [Show all 7 contributors for this article] (2018). TiO2 Nanorods Decorated With Cobalt oxide as Photoanodes for a Bio-Hybrid PEC Cell.
• Norby, Truls Eivind (2018). Dekarbonisering - henger Norge med?
• Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios; Vøllestad, Einar; Ruan, Qiushi; Tang, Junwang & Norby, Truls Eivind (2018). Solid-state photoelectrochemical cell for wet air electrolysis and hydrogen production.
• Yang, Juan; Mei, Sen; Grandcolas, Mathieu; Simon, Christian; Xu, Kaiqi & Chatzitakis, Athanasios Eleftherios [Show all 10 contributors for this article] (2017). Synthesis of Nanosized Cobalt Oxides and Application in a Bio-hybrid Photoelectrochemical Cell for CO2 Utilization. Show summary

  CO2 capture and utilization (CCU) can alleviate the disastrous effects of greenhouse gas (GHG) emissions form the use of fossil fuels. The use of CO2 emission as feedstock for direct conversion into valuable chemicals has attracted increasing research interest worldwide. A number of approaches, such as chemical, electrochemical, photochemical and biological routes have used CO2 as a sustainable carbon resource for the production of chemicals. In the present CO2BioPEC project, a novel hybrid photoelectrochemical concept, based on solar energy and formate dehydrogenase biocatalyst is applied, as illustrated in Figure 1 (left). This multidisciplinary project aims at demonstrating a bio-hybrid photoelectrochemical cell, in which solar energy is efficiently captured and utilized to convert CO2 into energy-rich compounds, using formate dehydrogenase enzymes as biocatalysts. Cobalt oxide is a low-cost material with a band gap that can absorb visible light. It is also a promising co-catalyst that has been widely used for oxygen evolution route. In the present work, nanosized cobalt oxide was synthesized and used as a co-catalyst on the photoanode. The results showed that the formation of cobalt oxides (Co3O4, CoOOH and Co(OH)2) is strongly dependent on the temperature and reaction time. The photochemical efficiency will be further investigated by impregnating nanosized cobalt oxides onto Ta3N4 /TaON nanotubes.

• Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios; Norby, Truls Eivind; Mei, Sen; Juan, Yang & Grandcolas, Mathieu [Show all 7 contributors for this article] (2017). Solid-state photoelectrochemical Cell with Tantalum Nitride Nanotubes as Photoanode.
• Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios; Bjørheim, Tor Svendsen & Norby, Truls Eivind (2017). Fuels from the sun, sea and air-by solid-state photoelectrochemical cell.
• Xu, Kaiqi; Chatzitakis, Athanasios Eleftherios; Bjørheim, Tor Svendsen & Norby, Truls Eivind (2017). Tantalum oxynitride for photoelectrochemical water splitting.
• Norby, Truls Eivind (2017). Novel approaches for conversion of H2O, CO2, and N2 with renewables.

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