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Kawde, A., Annamalai, A., Sellstedt, A., Glatzel, P., Wågberg, T. & Messinger, J. (2019). A microstructured p-Si photocathode outcompetes Pt as a counter electrode to hematite in photoelectrochemical water-splitting. Dalton Transactions, 48(4), 1166-1170
Open this publication in new window or tab >>A microstructured p-Si photocathode outcompetes Pt as a counter electrode to hematite in photoelectrochemical water-splitting
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2019 (English)In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 48, no 4, p. 1166-1170Article in journal (Refereed) Published
Abstract [en]

Herein, we communicate about an Earth-abundant semiconductor photocathode (p-Si/TiO2/NiOx) as an alternative for the rare and expensive Pt as a counter electrode for overall photoelectrochemical water splitting. The proposed photoelectrochemical (PEC) water-splitting device mimics the "Z"-scheme observed in natural photosynthesis by combining two photoelectrodes in a parallelillumination mode. A nearly 60% increase in the photocurrent density (Jph) for pristine α-Fe2Oand a 77% increase in the applied bias photocurrent efficiency (ABPE) were achieved by replacing the conventionally used Pt cathode with an efficient, cost effective p-Si/TiO2/NiOx photocathode under parallel illumination. The resulting photocurrent density of 1.26 mA cm−2 at 1.23VRHE represents a new record performance for hydrothermally grown pristine α-Fe2O3 nanorod photoanodes in combination with a photocathode, which opens the prospect for further improvement by doping α-Fe2O3 or by its decoration with co-catalysts. Electrochemical impedance spectroscopy measurements suggest that this significant performance increase is due to the enhancement of the space-charge field in α-Fe2O3. 

Place, publisher, year, edition, pages
Royal Society of Chemistry, 2019
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-153415 (URN)10.1039/c8dt03653e (DOI)000459625900002 ()30534760 (PubMedID)
Available from: 2018-11-20 Created: 2018-11-20 Last updated: 2019-03-27Bibliographically approved
Shevela, D., Ananyev, G., Vatland, A. K., Arnold, J., Mamedov, F., Eichacker, L. A., . . . Messinger, J. (2019). 'Birth defects' of photosystem II make it highly susceptible to photodamage during chloroplast biogenesis. Physiologia Plantarum: An International Journal for Plant Biology, 166(1), 165-180
Open this publication in new window or tab >>'Birth defects' of photosystem II make it highly susceptible to photodamage during chloroplast biogenesis
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2019 (English)In: Physiologia Plantarum: An International Journal for Plant Biology, ISSN 0031-9317, E-ISSN 1399-3054, Vol. 166, no 1, p. 165-180Article in journal (Refereed) Published
Abstract [en]

High solar flux is known to diminish photosynthetic growth rates, reducing biomass productivity and lowering disease tolerance. Photosystem II (PSII) of plants is susceptible to photodamage (also known as photoinactivation) in strong light, resulting in severe loss of water oxidation capacity and destruction of the water‐oxidizing complex (WOC). The repair of damaged PSIIs comes at a high energy cost and requires de novo biosynthesis of damaged PSII subunits, reassembly of the WOC inorganic cofactors and membrane remodeling. Employing membrane‐inlet mass spectrometry and O2‐polarography under flashing light conditions, we demonstrate that newly synthesized PSII complexes are far more susceptible to photodamage than are mature PSII complexes. We examined these ‘PSII birth defects’ in barley seedlings and plastids (etiochloroplasts and chloroplasts) isolated at various times during de‐etiolation as chloroplast development begins and matures in synchronization with thylakoid membrane biogenesis and grana membrane formation. We show that the degree of PSII photodamage decreases simultaneously with biogenesis of the PSII turnover efficiency measured by O2‐polarography, and with grana membrane stacking, as determined by electron microscopy. Our data from fluorescence, QB‐inhibitor binding, and thermoluminescence studies indicate that the decline of the high‐light susceptibility of PSII to photodamage is coincident with appearance of electron transfer capability QA− → QB during de‐etiolation. This rate depends in turn on the downstream clearing of electrons upon buildup of the complete linear electron transfer chain and the formation of stacked grana membranes capable of longer‐range energy transfer.

Place, publisher, year, edition, pages
Wiley-Blackwell, 2019
Keywords
Practice variation, Bronchopulmonary dysplasia, Preterm infants, Ventilation
National Category
Biophysics
Identifiers
urn:nbn:se:umu:diva-158931 (URN)10.1111/ppl.12932 (DOI)000466108300014 ()30693529 (PubMedID)
Funder
Swedish Research CouncilSwedish Research Council
Note

Special Issue: SI

Available from: 2019-05-15 Created: 2019-05-15 Last updated: 2019-06-10Bibliographically approved
Kwong, W. L., Lee, C. C., Shchukarev, A. & Messinger, J. (2019). Cobalt- doped hematite thin films for electrocatalytic water oxidation in highly acidic media. Chemical Communications, 55(34), 5017-5020
Open this publication in new window or tab >>Cobalt- doped hematite thin films for electrocatalytic water oxidation in highly acidic media
2019 (English)In: Chemical Communications, ISSN 1359-7345, E-ISSN 1364-548X, Vol. 55, no 34, p. 5017-5020Article in journal (Refereed) Published
Abstract [en]

Earth-abundant cobalt-doped hematite thin-film electrocatalysts were explored for acidic water oxidation. The strategically doped hematite produced a stable geometric current density of 10 mA cm(-2) for up to 50 h at pH 0.3, as a result of Co-enhanced intrinsic catalytic activity and charge transport properties across the film matrix.

Place, publisher, year, edition, pages
The Royal Society of Chemistry, 2019
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-159862 (URN)10.1039/c9cc01369e (DOI)000468618000025 ()30968887 (PubMedID)
Available from: 2019-06-10 Created: 2019-06-10 Last updated: 2019-09-05Bibliographically approved
Krieger-Liszkay, A., Spetea, C. & Messinger, J. (2019). Photosynthesis - European Congress on Photosynthesis Research. Physiologia Plantarum: An International Journal for Plant Biology, 166(1), 4-6
Open this publication in new window or tab >>Photosynthesis - European Congress on Photosynthesis Research
2019 (English)In: Physiologia Plantarum: An International Journal for Plant Biology, ISSN 0031-9317, E-ISSN 1399-3054, Vol. 166, no 1, p. 4-6Article in journal, Editorial material (Other academic) Published
Place, publisher, year, edition, pages
Wiley-Blackwell, 2019
National Category
Biological Sciences
Identifiers
urn:nbn:se:umu:diva-159868 (URN)10.1111/ppl.12968 (DOI)000466108300001 ()31012147 (PubMedID)
Available from: 2019-06-10 Created: 2019-06-10 Last updated: 2019-06-10Bibliographically approved
Chatterjee, R., Lassalle, L., Gul, S., Fuller, F. D., Young, I. D., Ibrahim, M., . . . Yano, J. (2019). Structural isomers of the S-2 state in photosystem II: do they exist at room temperature and are they important for function?. Paper presented at 1st European Congress on Photosynthesis Research (EPS), JUN 25-28, 2018, Uppsala, SWEDEN. Physiologia Plantarum: An International Journal for Plant Biology, 166(1), 60-72
Open this publication in new window or tab >>Structural isomers of the S-2 state in photosystem II: do they exist at room temperature and are they important for function?
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2019 (English)In: Physiologia Plantarum: An International Journal for Plant Biology, ISSN 0031-9317, E-ISSN 1399-3054, Vol. 166, no 1, p. 60-72Article in journal (Refereed) Published
Abstract [en]

In nature, an oxo‐bridged Mn4CaO5 cluster embedded in photosystem II (PSII), a membrane‐bound multi‐subunit pigment protein complex, catalyzes the water oxidation reaction that is driven by light‐induced charge separations in the reaction center of PSII. The Mn4CaO5 cluster accumulates four oxidizing equivalents to enable the four‐electron four‐proton catalysis of two water molecules to one dioxygen molecule and cycles through five intermediate S‐states, S0 – S4 in the Kok cycle. One important question related to the catalytic mechanism of the oxygen‐evolving complex (OEC) that remains is, whether structural isomers are present in some of the intermediate S‐states and if such equilibria are essential for the mechanism of the O‐O bond formation. Here we compare results from electron paramagnetic resonance (EPR) and X‐ray absorption spectroscopy (XAS) obtained at cryogenic temperatures for the S2state of PSII with structural data collected of the S1, S2 and S3 states by serial crystallography at neutral pH (∼6.5) using an X‐ray free electron laser at room temperature. While the cryogenic data show the presence of at least two structural forms of the S2 state, the room temperature crystallography data can be well‐described by just one S2 structure. We discuss the deviating results and outline experimental strategies for clarifying this mechanistically important question.

Place, publisher, year, edition, pages
Wiley-Blackwell, 2019
National Category
Physical Chemistry Biological Sciences
Identifiers
urn:nbn:se:umu:diva-159873 (URN)10.1111/ppl.12947 (DOI)000466108300007 ()30793319 (PubMedID)
Conference
1st European Congress on Photosynthesis Research (EPS), JUN 25-28, 2018, Uppsala, SWEDEN
Funder
NIH (National Institute of Health), GM110501NIH (National Institute of Health), GM126289NIH (National Institute of Health), GM055302Swedish Research Council, 2016-05183
Note

Special Issue: SI

Available from: 2019-06-10 Created: 2019-06-10 Last updated: 2019-06-10Bibliographically approved
Conlan, B. l., Govindjee, . & Messinger, J. (2019). Thomas John Wydrzynski (8 July 1947-16 March 2018). Photosynthesis Research, 140(3), 253-261
Open this publication in new window or tab >>Thomas John Wydrzynski (8 July 1947-16 March 2018)
2019 (English)In: Photosynthesis Research, ISSN 0166-8595, E-ISSN 1573-5079, Vol. 140, no 3, p. 253-261Article in journal (Refereed) Published
Abstract [en]

With this Tribute, we remember and honor Thomas John (Tom) Wydrzynski. Tom was a highly innovative, independent and committed researcher, who had, early in his career, defined his life-long research goal. He was committed to understand how Photosystem II produces molecular oxygen from water, using the energy of sunlight, and to apply this knowledge towards making artificial systems. In this tribute, we summarize his research journey, which involved working on soft money' in several laboratories around the world for many years, as well as his research achievements. We also reflect upon his approach to life, science and student supervision, as we perceive it. Tom was not only a thoughtful scientist that inspired many to enter this field of research, but also a wonderful supervisor and friend, who is deeply missed (see footnote*).

Place, publisher, year, edition, pages
Springer Netherlands, 2019
Keywords
Water oxidation, Photosystem II, Manganese, Chloride, Artificial photosynthesis
National Category
Botany
Identifiers
urn:nbn:se:umu:diva-159594 (URN)10.1007/s11120-018-0606-9 (DOI)000467577100001 ()30478710 (PubMedID)
Available from: 2019-06-17 Created: 2019-06-17 Last updated: 2019-06-17Bibliographically approved
Pham, L. V., Olmos, J. D., Chernev, P., Kargul, J. & Messinger, J. (2019). Unequal misses during the flash-induced advancement of photosystem II: effects of the S state and acceptor side cycles. Paper presented at 8th International Conference on Photosynthesis and Hydrogen Energy Research for Sustainability in honor of Agepati S Raghavendra, William A Cramer, and Govindjee, 2017, Hyderabad, India. Photosynthesis Research, 139(1-3), 93-106
Open this publication in new window or tab >>Unequal misses during the flash-induced advancement of photosystem II: effects of the S state and acceptor side cycles
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2019 (English)In: Photosynthesis Research, ISSN 0166-8595, E-ISSN 1573-5079, Vol. 139, no 1-3, p. 93-106Article in journal (Refereed) Published
Abstract [en]

Photosynthetic water oxidation is catalyzed by the oxygen-evolving complex (OEC) in photosystem II (PSII). This process is energetically driven by light-induced charge separation in the reaction center of PSII, which leads to a stepwise accumulation of oxidizing equivalents in the OEC (S-i states, i=0-4) resulting in O-2 evolution after each fourth flash, and to the reduction of plastoquinone to plastoquinol on the acceptor side of PSII. However, the S-i-state advancement is not perfect, which according to the Kok model is described by miss-hits (misses). These may be caused by redox equilibria or kinetic limitations on the donor (OEC) or the acceptor side. In this study, we investigate the effects of individual S state transitions and of the quinone acceptor side on the miss parameter by analyzing the flash-induced oxygen evolution patterns and the S-2, S-3 and S-0 state lifetimes in thylakoid samples of the extremophilic red alga Cyanidioschyzon merolae. The data are analyzed employing a global fit analysis and the results are compared to the data obtained previously for spinach thylakoids. These two organisms were selected, because the redox potential of Q(A)/Q(A)(-) in PSII is significantly less negative in C. merolae (E-m=-104mV) than in spinach (E-m=-163mV). This significant difference in redox potential was expected to allow the disentanglement of acceptor and donor side effects on the miss parameter. Our data indicate that, at slightly acidic and neutral pH values, the E-m of Q(A)(-)/Q(A) plays only a minor role for the miss parameter. By contrast, the increased energy gap for the backward electron transfer from Q(A)(-) to Pheo slows down the charge recombination reaction with the S-3 and S-2 states considerably. In addition, our data support the concept that the S-2 S-3 transition is the least efficient step during the oxidation of water to molecular oxygen in the Kok cycle of PSII.

Place, publisher, year, edition, pages
Springer, 2019
Keywords
Photosynthesis, Photosystem II, Mechanism of water oxidation, Flash-induced oxygen oscillation pattern (FIOP), Unequal miss parameter, Cyanidioschyzon merolae
National Category
Physical Chemistry
Identifiers
urn:nbn:se:umu:diva-156869 (URN)10.1007/s11120-018-0574-0 (DOI)000458553100008 ()30191436 (PubMedID)
Conference
8th International Conference on Photosynthesis and Hydrogen Energy Research for Sustainability in honor of Agepati S Raghavendra, William A Cramer, and Govindjee, 2017, Hyderabad, India
Available from: 2019-03-12 Created: 2019-03-12 Last updated: 2019-06-17Bibliographically approved
Kwong, W. L., Lee, C. C., Shchukarev, A., Björn, E. & Messinger, J. (2018). High-performance iron (III) oxide electrocatalyst for water oxidation in strongly acidic media. Journal of Catalysis, 365, 29-35
Open this publication in new window or tab >>High-performance iron (III) oxide electrocatalyst for water oxidation in strongly acidic media
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2018 (English)In: Journal of Catalysis, ISSN 0021-9517, E-ISSN 1090-2694, Vol. 365, p. 29-35Article in journal (Refereed) Published
Abstract [en]

Stable and efficient oxygen evolution reaction (OER) catalysts for the oxidation of water to dioxygen in highly acidic media are currently limited to expensive noble metal (Ir and Ru) oxides since presently known OER catalysts made of inexpensive earth-abundant materials generally suffer anodic corrosion at low pH. In this study, we report that a mixed-polymorph film comprising maghemite and hematite, prepared using spray pyrolysis deposition followed by low-temperature annealing, showed a sustained OER rate (>24 h) corresponding to a current density of 10 mA cm−2 at an initial overpotential of 650 mV, with a Tafel slope of only 56 mV dec−1 and near-100% Faradaic efficiency in 0.5 M H2SO4 (pH 0.3). This performance is remarkable, since iron (III) oxide films comprising only maghemite were found to exhibit a comparable intrinsic activity, but considerably lower stability for OER, while films of pure hematite were OER-inactive. These results are explained by the differences in the polymorph crystal structures, which cause different electrical conductivity and surface interactions with water molecules and protons. Our findings not only reveal the potential of iron (III) oxide as acid-stable OER catalyst, but also highlight the important yet hitherto largely unexplored effect of crystal polymorphism on electrocatalytic OER performance.

Place, publisher, year, edition, pages
Academic Press, 2018
Keywords
Artificial photosynthesis, Water oxidation, Oxygen evolution reaction, Acidic electrolyte, Iron oxide
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:umu:diva-150224 (URN)10.1016/j.jcat.2018.06.018 (DOI)000442976400005 ()
Funder
Knut and Alice Wallenberg Foundation
Available from: 2018-07-19 Created: 2018-07-19 Last updated: 2018-09-21Bibliographically approved
Kawde, A., Annamalai, A., Amidani, L., Boniolo, M., Kwong, W. L., Sellstedt, A., . . . Messinger, J. (2018). Photo-electrochemical hydrogen production from neutral phosphate buffer and seawater using micro-structured p-Si photo-electrodes functionalized by solution-based methods. Sustainable Energy and Fuels, 2(10), 2215-2223
Open this publication in new window or tab >>Photo-electrochemical hydrogen production from neutral phosphate buffer and seawater using micro-structured p-Si photo-electrodes functionalized by solution-based methods
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2018 (English)In: Sustainable Energy and Fuels, ISSN 2398-4902, Vol. 2, no 10, p. 2215-2223Article in journal (Refereed) [Artistic work] Published
Abstract [en]

Solar fuels such as H2 generated from sunlight and seawater using earth-abundant materials are expected to be a crucial component of a next generation renewable energy mix. We herein report a systematic analysis of the photo-electrochemical performance of TiO2 coated, microstructured p-Si photoelectrodes (p-Si/TiO2) that were functionalized with CoOx and NiOx for H2 generation. These photocathodes were synthesized from commercial p-Si wafers employing wet chemical methods. In neutral phosphate buffer and standard 1 sun illumination, the p-Si/TiO2/NiOx photoelectrode showed a photocurrent density of 1.48 mA cm2 at zero bias (0 VRHE), which was three times and 15 times better than the photocurrent densities of p-Si/TiO2/CoOx and p-Si/TiO2, respectively. No decline in activity was observed over a five hour test period, yielding a Faradaic efficiency of 96% for H2 production. Based on the electrochemical characterizations and the high energy resolution fluorescence detected X-ray absorption near edge structure (HERFD-XANES) and emission spectroscopy measurements performed at the Ti Ka1 fluorescence line, the superior performance of the p-Si/TiO2/ NiOx photoelectrode was attributed to improved charge transfer properties induced by the NiOx coating on the protective TiO2 layer, in combination with a higher catalytic activity of NiOx for H2-evolution. Moreover, we report here an excellent photo-electrochemical performance of p-Si/TiO2/NiOx photoelectrode in corrosive artificial seawater (pH 8.4) with an unprecedented photocurrent density of 10 mA cm2 at an applied potential of 0.7 VRHE, and of 20 mA cm2 at 0.9 VRHE. The applied bias photon-to-current conversion efficiency (ABPE) at 0.7 VRHE and 10 mA cm2 was found to be 5.1%

Keywords
solar water splitting, artificial photosynthesis, X-ray Spectroscopy
National Category
Materials Chemistry
Identifiers
urn:nbn:se:umu:diva-153381 (URN)10.1039/c8se00291f (DOI)000447950800007 ()
Funder
Wallenberg Foundations, KAW 2011.0055
Available from: 2018-11-19 Created: 2018-11-19 Last updated: 2018-11-20Bibliographically approved
Tikhonov, K., Shevela, D., Klimov, V. V. & Messinger, J. (2018). Quantification of bound bicarbonate in photosystem II. Photosynthetica (Praha), 56(1), 210-216
Open this publication in new window or tab >>Quantification of bound bicarbonate in photosystem II
2018 (English)In: Photosynthetica (Praha), ISSN 0300-3604, E-ISSN 1573-9058, Vol. 56, no 1, p. 210-216Article in journal (Refereed) Published
Abstract [en]

In this study, we presented a new approach for quantification of bicarbonate (HCO3-) molecules bound to PSII. Our method, which is based on a combination of membrane-inlet mass spectrometry (MIMS) and O-18-labelling, excludes the possibility of "non-accounted" HCO3- by avoiding (1) the employment of formate for removal of HCO3- from PSII, and (2) the extremely low concentrations of HCO3-/CO2 during online MIMS measurements. By equilibration of PSII sample to ambient CO2 concentration of dissolved CO2/HCO3-, the method ensures that all physiological binding sites are saturated before analysis. With this approach, we determined that in spinach PSII membrane fragments 1.1 +/- 0.1 HCO3- are bound per PSII reaction center, while none was bound to isolated PsbO protein. Our present results confirmed that PSII binds one HCO3- molecule as ligand to the non-heme iron of PSII, while unbound HCO3- optimizes the water-splitting reactions by acting as a mobile proton shuttle.

Keywords
hydrogen carbonate, inorganic carbon, mass spectrometry, Mn-stabilizing protein, non-heme iron, ygen-evolving complex
National Category
Biophysics
Identifiers
urn:nbn:se:umu:diva-147475 (URN)10.1007/s11099-017-0758-4 (DOI)000430309200019 ()
Funder
Swedish Research Council, 2016-05183
Available from: 2018-05-04 Created: 2018-05-04 Last updated: 2018-06-09Bibliographically approved
Projects
Water-binding and water-splitting by photosystem II and artificial catalysts [2009-03722_VR]; Umeå UniversityTRANSFORMERS - Integrated biomass production using Swedish microorganisms, local wastewaters and flue gases [2015-92_Formas]; Umeå UniversityMechanism and assembly of the water oxidation catalyst in photosystem II [2016-05183_VR]; Umeå University
Organisations
Identifiers
ORCID iD: ORCID iD iconorcid.org/0000-0003-2790-7721

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