The goal of Subtask 2 "Artificial Water Oxidation Complex" is to develop a bio-inspired catalyst for water oxidation.

Researchers working on this subtask are trying to design a catalyst that will incorporate features of the natural  oxygen evolving complex (OEC)  via a framework of synthesized materials. Given the difficulties researchers have encountered in developing a robust water oxidation catalyst based on abundant materials and having both low overpotential and high turnover, the Center is investigating several approaches to this part of the project. Researchers at ASU and elsewhere have uncovered the structure of the peptide framework of the natural PSII water oxidation complex, although the details of the metal complex itself and its mechanism of operation still await discovery. Our knowledge and expertise are now sufficient to allow construction of an artificial oxygen evolving complex whose catalytic site is based on the natural one. We are investigating a novel design wherein DNA is used as a self-assembling framework upon which a peptide-based catalyst is constructed. Another approach is based upon design of water soluble analogs of the natural water oxidation complex. In a collaborative project, a totally artificial porphyrin-based system whose design is drawn from the natural complex is being studied. A final approach involves investigating the structure, properties and function of a natural oxygen-consuming enzyme whose active site will be used as the basis for a new type of bio-inspired water oxidation catalyst.

People working on Subtask 2

Zhao Zhao
Graduate Student
Yan Liu
Principal Investigator
Xixi Wei
Graduate student
Thomas Moore
Principal Investigator
Subtask 1 Leader
Shibom Basu
Graduate student
Raimund Fromme
Faculty Research Associate
Petra Fromme
Principal Investigator
Palash Dutta
Graduate student
Minghui Liu
Graduate student
Kim Rendek
Graduate student
Kevin Redding
Associate Director of the Center
Principal Investigator
Justin Flory
Graduate student
James Allen
Principal Investigator
Subtask 2 Leader
Hao Yan
Principal Investigator
Giovanna Ghirlanda
Principal Investigator
Subtask 3 Leader
Dong Wang
Graduate student
Chad Simmons
Academic Professional
Anindya Roy
Graduate student

Major projects of Subtask 2

  1. Peptide-based artificial OEC housed in a DNA nanocage
  2. Complete water splitting system based on IrO2 colloids
  3. A soluble OEC analog
  4. Water oxidation catalysts based on nanometric Co2O3 particles
  5. Water oxidation catalyst based on a re-engineered enzyme
  6. Water oxidation catalyst based on a bio-inspired Mn porphyrin complex

Research news on Subtask 2

9 Jul 2014

BISfuel, July 9, 2014 –  Deciphering the puzzles of the natural photosynthetic water oxidation mechanism empowers designers of artificial photosynthesis with knowledge to construct better water oxidation catalysts for solar fuel production. A group of Bisfuel researchers working with collaborators at the DOE free electron laser has achieved an important milestone in understanding the photosynthetic water oxidation catalytic process.

18 Feb 2014

by Jenny Green:      In a recent early online edition of Nature Chemistry, ASU scientists, along with colleagues at Argonne National Laboratory, have reported advances toward perfecting a functional artificial leaf. Designing an artificial leaf that uses solar energy to convert water cheaply and efficiently into hydrogen and oxygen is one of the goals of BISfuel, the Energy Frontier Research Center, funded by the Department of Energy, in the Department of Chemistry and Biochemistry at Arizona State University.

1 Feb 2013

BISfuel© :    A team of Bisfuel researchers led by Devens Gust, Ana Moore and Tom Moore has designed and characterized an artificial photosynthetic reaction center inspired by natural Photosystem II and comprising a highly oxidizing porphyrin linked to a biomimetic electron transfer relay and a porphyrin electron acceptor. Two articles with the results of the study have appeared in September special issue of PNAS “Chemical Approaches to Artificial Photosynthesis: Solar Fuels Special Feature” 

22 Jun 2011

A group of Center for Bio-inspired Solar Fuel Production researchers collaborating on Subtask 2 (Water oxidation catalyst) and Subtask 5 (Functional nanostructured transparent electrode materials) have found that transparent and conducting antimony tin oxide with controlled pore size incorporates DNA nanocages with high affinity and without damage. Results of the study have been published in  the June 2011 issue of ACS Nano. The study has brought the Center scientists a bit closer to a design of a transparent nanostructured electrode with entrapped functional water oxidation catalysts.

B-DNA
15 Apr 2011

Center researchers have developed a new DNA origami design strategy for engineering complex, arbitrarily shaped 3D DNA nanostructures that have substantial intrinsic curvatures. This strategy has been presented in a paper by Professors Hao Yan, Yan Liu and coworkers that was featured on the cover of Science for April 15, 2011.

4 Feb 2011

Professor Petra Fromme, a Principal Investigator of Subtask 2 at the Center, and members of her lab, Ingo Grotjohan and Raimund Fromme, have recently been involved in international collaboration study on time-resolved structure determination of membrane proteins. A recent breakthrough publication in Nature based on results of this study is entitled “Femtosecond X-ray protein nanocrystallography”.

DNA origami using 'tiles' not 'staples'
2 Mar 2010

The group of Yan Liu and Hao Yan has discovered a way to scale up DNA origami using tiles not staples to pin the DNA into place. Their method has great potential for providing cheap access to complicated nanostructures.

Recent papers on Subtask 2

  1. Kupitz, Christopher; Basu, Shibom; Grotjohann, Ingo; Fromme, Raimund; Zatsepin, Nadia A.; Rendek, Kimberly N.; Hunter, Mark; Shoeman, Robert L.; White, Thomas A.; Wang, Dingjie; James, Daniel; Yang, Jay-How; Cobb, Danielle E.; Brenda, Reeder; Raymond, G. Sierra; Liu, Haiguang; Barty, Anton; Aquila, Andrew L.; Deponte, Daniel; Kirian, Richard A.; Bari, Sadia; Bergkamp, Jesse J.; Beyerlein, Kenneth R.; Bogan, Michael J.; Caleman, Carl; Chao, Tzu-Chiao; Conrad, Chelsie E.; Davis, Katherine M.; Fleckenstein, Holger; Galli, Lorenzo; Hau-Riege, Stefan P.; Kassemeyer, Stephan; Laksmono, Hartawan; Liang, Mengning; Lomb, Lukas; Marchesini, Stefano; Martin, Andrew V.; Messerschmidt, Marc; Milathianaki, Despina; Nass, Karol; Ros, Alexandra; Roy-Chowdhury, Shatabdi; Schmidt, Kevin; Seibert, Marvin; Steinbrener, Jan; Stellato, Francesco; Yan, Lifen; Yoon, Chunhong; Moore, Thomas A.; Moore, Ana L.; Pushkar, Yulia; Williams, Garth J.; Boutet, Sébastien; Doak, R. Bruce; Weierstall, Uwe; Frank, Matthias; Chapman, Henry N.; Spence, John C.H., and Fromme, Petra (2014) Serial time-resolved crystallography of photosystem II using a femtosecond X-ray laser, Nature, Published online 09 July 2014 , (Read online)"
  2. Kupitz, C., Grotjohann, I., Conrad, C.E., Roy-Chowdhury, S., Fromme, R., and Fromme, P. (2014) Microcrystallization techniques for serial femtosecond crystallography using Photosystem II from Thermosynechococcus elongatus as a model system, Phil. Trans. R. Soc. B, Published online June 9, 2014, (Read online)"
  3. Flory, J. D., Simmons, C. R., Lin, S., Johnson, T., Andreoni, A., Zook, J., Ghirlanda, G., Liu, Y., Yan, H., and Fromme, P. (2014) Low Temperature Assembly of Functional 3D DNA-PNA-Protein Complexes, J. Am. Chem. Soc., 136 (23), 8283–8295 (Read online)"
  4. Mukhopadhyay, T.K., Flores, M., Groy, T.L., and Trovitch, R.J. (2014) A highly active manganese precatalyst for the hydrosilylation of ketones and esters, Journal of the American Chemical Society , 136 (3), 882–885 (Read online)"
  5. Porter, T.M., Hall, G.B., Groy, T.L., and Trovitch, R.J. (2013) Importance of co-donor field strength in the preparation of tetradentate α-diimine nickel hydrosilylation catalysts, Dalton Trans., 42, 14689 - 14692 (Read online)"
  6. Han, D., Jiang, S., Samanta, A., Liu, Y., and Yan, H. (2013) Unidirectional Scaffold-Strand Arrangement in DNA Origami, Angewandte Chemie International Edition, 52, 9031–9034 (Read online)"
  7. Ben-Daat, H., Hall, G.B., Groy, T.L., and Trovitch, R.J (2013) Rational Design of Rhodium Complexes Featuring κ4-N,N,N,N- and κ5-N,N,N,P,P-Bis(imino)pyridine Ligands, European Journal of Inorganic Chemistry, 25, 4430–4442 (Read online)"
  8. Liu, M., Fu, J., Hejesen, C., Yang, Y., Woodbury, N.W., Gothelf, K., Liu, Y., and Yan, H. (2013) A DNA tweezer-actuated enzyme nanoreactor, Nature Communications, 4, article 2127 (Read online)"
  9. Flory, J.D., Shinde, S., Lin, S., Liu, Y., Yan, H., Ghirlanda, G., and Fromme, P. (2013) PNA-peptide Assembly in a 3D DNA Nanocage at Room Temperature, J. Am. Chem. Soc., 135 (18), 6985-6993 (Read online)"
  10. Han, D., Pal, S., Yang, Y., Jiang, S., Nangreave, J., Liu, Y., and Yan, H. (2013) DNA Gridiron Nanostructures Based on Four-Arm Junctions, Science, 339, 1412-1415 (Read online)"
  11. Rendek, K.N., Fromme, R., Grotjohann, I., Fromme, P. (2013) Crystallization of a self-assembled three-dimensional DNA nanostructure, Acta Crystallogr. Sect. F , F69, 141-146 (Read online)"
  12. Lu, N., Pei, H., Ge, Z., Simmons, C.R., Yan, H., and Fan, C. (2012) Charge Transport within a Three-Dimensional DNA Nanostructure Framework, Journal of the American Chemical Society, 134, 13148−13151 (Read online)"
  13. Brunger, A.T., Adams, P.D., Fromme, P., Fromme, R., Levitt, M., and Schröder, G.F. (2012) Improving the accuracy of macromolecular structure refinement , Structure, 20, 20, 957–966 (Read online)"
  14. Johansson LC, Arnlund D, White TA, Katona G, Deponte DP, Weierstall U, Doak RB, Shoeman RL, Lomb L, Malmerberg E, Davidsson J, Nass K, Liang M, Andreasson J, Aquila A, Bajt S, Barthelmess M, Barty A, Bogan MJ, Bostedt C, Bozek JD, Caleman C, Coffee R, Coppola N, Ekeberg T, Epp SW, Erk B, Fleckenstein H, Foucar L, Graafsma H, Gumprecht L, Hajdu J, Hampton CY, Hartmann R, Hartmann A, Hauser G, Hirsemann H, Holl P, Hunter MS, Kassemeyer S, Kimmel N, Kirian RA, Maia FR, Marchesini S, Martin AV, Reich C, Rolles D, Rudek B, Rudenko A, Schlichting I, Schulz J, Seibert MM, Sierra RG, Soltau H, Starodub D, Stellato F, Stern S, Strüder L, Timneanu N, Ullrich J, Wahlgren WY, Wang X, Weidenspointner G, Wunderer C, Fromme P, Chapman HN, Spence JC, Neutze R. (2012) Lipidic phase membrane protein serial femtosecond crystallography, Nature Methods, 9, 263-265 (Read online)"
  15. Aquila, A., Hunter, M. S., Doak, R. B., Kirian, R. A., Fromme, P., White, T. A., Andreasson, J., Arnlund, D., Bajt, S. a., Barends, T. R. M., Barthelmess, M., Bogan, M. J., Bostedt, C., Bottin, H., Bozek, J. D., Caleman, C., Coppola, N., Davidsson, J., DePonte, D. P., Elser, V., Epp, S. W., Erk, B., Fleckenstein, H., Foucar, L., Frank, M., Fromme, R., Graafsma, H., Grotjohann, I., Gumprecht, L., Hajdu, J., Hampton, C. Y., Hartmann, A., Hartmann, R., Hau-Riege, S., Hauser, G., Hirsemann, H., Holl, P., Holton, J. M., Hömke, A., Johansson, L., Kimmel, N., Kassemeyer, S., Krasniqi, F., Kühnel, K.-U., Liang, M., Lomb, L., Malmerberg, E., Marchesini, S., Martin, A. V., Maia, F. R. N. C., Messerschmidt, M., Nass, K., Reich, C., Neutze, R., Rolles, D., Rudek, B., Rudenko, A., Schlichting, I., Schmidt, C., Schmidt, K. E., Schulz, J., Seibert, M. M., Shoeman, R. L., Sierra, R., Soltau, H., Starodub, D., Stellato, F., Stern, S., Strüder, L., Timneanu, N., Ullrich, J., Wang, X., Williams, G. J., Weidenspointner, G., Weierstall, U., Wunderer, C., Barty, A., Spence, J. C. H., and Chapman, H. N. (2012) Time-resolved protein nanocrystallography using an X-ray free-electron laser, OPTICS EXPRESS, 20, 2706-2716 (Read online)"
  16. Barty, A., Caleman, C., Aquila, A., Timneanu, N., Lomb, L., White, T. A., Andreasson, J., Arnlund, D., Bajt, S., Barends, T. R. M., Barthelmess, M., Bogan, M. J., Bostedt, C., Bozek, J. D., Coffee, R., Coppola, N., Davidsson, J., DePonte, D. P., Doak, R. B., Ekeberg, T., Elser, V., Epp, S. W., Erk, B., Fleckenstein, H., Foucar, L., Fromme, P., Graafsma, H., Gumprecht, L., Hajdu, J., Hampton, C. Y., Hartmann, R., Hartmann, A., Hauser, G., Hirsemann, H., Holl, P., Hunter, M. S., Johansson, L., Kassemeyer, S., Kimmel, N., Kirian, R. A., Liang, M., Maia, F. R. N. C., Malmerberg, E., Marchesini, S., Martin, A. V., Nass, K., Neutze, R., Reich, C., Rolles, D., Rudek, B., Rudenko, A., Scott, H., Schlichting, I., Schulz, J., Seibert, M. M., Shoeman, R. L., Sierra, R. G., Soltau, H., Spence, J. C. H., Stellato, F., Stern, S., Struder, L., Ullrich, J., WangX, Weidenspointner, G., Weierstall, U., Wunderer, C. B., and Chapman, H. N. (2011) Self-terminating diffraction gates femtosecond X-ray nanocrystallography measurements, Nature Photonics, 6, 35-40 (Read online)"
  17. Pinheiro, A. V., Han, D., Shih, W. M., and Yan, H. (2011) Challenges and opportunities for structural DNA nanotechnology, Nature nanotechnology, 6, 763-772 (Read online)"
  18. Fromme, P., and Spence, J. C. H. (2011) Femtosecond nanocrystallography using X-ray lasers for membrane protein structure determination, Current Opinion in Structural Biology, 21, 509-516 (Read online)"
  19. Dutta, P. K., Varghese, R., Nangreave, J., Lin, S., Yan, H., and Liu, Y. (2011) DNA-Directed Artificial Light-Harvesting Antenna, Journal of the American Chemical Society, 133, 11985-11993 (Read online)"
  20. Simmons, C. R., Schmitt, D., Wei, X., Han, D., Volosin, A. M., Ladd, D. M., Seo, D.-K., Liu, Y., and Yan, H. (2011) Size-Selective Incorporation of DNA Nanocages into Nanoporous Antimony-Doped Tin Oxide Materials, ACS Nano, 5, 6060-6068 (Read online)"
  21. Tørring, T., Voigt, N.V., Nangreave, J., Yan, H., and Gothelf, K.V. (2011) DNA origami: A quantum leap for self assembly of complex structures, Chem. Soc. Rev., 40, 5636 – 5646 (Read online)"
  22. Han, D., Pal, S., Nangreave, J., Deng, Z., Liu, Y., and Yan, H. (2011) DNA Origami with Complex Curvatures in Three-Dimensional Space, Science, 332, 342-346 (Read online)"
  23. Pal, S., Varghese, R., Deng, Z., Zhao, Z., Kumar, A., Yan, H., and Liu, Y. (2011) Site-Specific Synthesis and In Situ Immobilization of Fluorescent Silver Nanoclusters on DNA Nanoscaffolds by Use of the Tollens Reaction, Angewandte Chemie International Edition, 50, 4176–4179 (Read online)"
  24. Deng, Z., Tong, L., Flores, M., Lin, S., Cheng, J.-X., Yan, H., and Liu, Y. (2011) High-Quality Manganese-Doped Zinc Sulfide Quantum Rods with Tunable Dual-Color and Multiphoton Emissions, Journal of the American Chemical Society, 133, 5389-5396 (Read online)"
  25. Nangreave, J., Yan, H., and Liu, Y. (2011) DNA Nanostructures as Models for Evaluating the Role of Enthalpy and Entropy in Polyvalent Binding, Journal of the American Chemical Society, 133, 4490-4497 (Read online)"
  26. Chapman, H.N., Fromme, P., Barty, A., White, T.A., Kirian, R.A., Aquila, A., Hunter, M.S., Schulz, J., DePonte, D.P., Weierstall, U., Doak, R.B., Maia, F.R.N.C., Martin, A.V., Schlichting, I., Lomb, L., Coppola, N., Shoeman, R.L., Epp, S.W., Hartmann, R., Rolles, D., Rudenko, A., Foucar, L., Kimmel, N., Weidenspointner, G., Holl, P., Liang, M., Barthelmess, M., Caleman, C., Boutet, S., Bogan, M.J., Krzywinski, J., Bostedt, C., Bajt, S., Gumprecht, L., Rudek, B., Erk, B., Schmidt, C., Homke, A., Reich, C., Pietschner, D., Struder, L., Hauser, G., Gorke, H., Ullrich, J., Herrmann, S., Schaller, G., Schopper, F., Soltau, H., Kuhnel, K.-U., Messerschmidt, M., Bozek, J.D., Hau-Riege, S.P., Frank, M., Hampton, C.Y., Sierra, R. G., Starodub, D., Williams, G.J., Hajdu, J., Timneanu, N., Seibert, M.M., Andreasson, J., Rocker, A., Jonsson, O., Svenda, M., Stern, S., Nass, K., Andritschke, R., Schroter, C.-D., Krasniqi, F., Bott, M., Schmidt, K.E., Wang, X., Grotjohann, I., Holton, J.M., Barends, T.R.M., Neutze, R., Marchesini, S., Fromme, R., Schorb, S., Rupp, D., Adolph, M., Gorkhover, T., Andersson, I., Hirsemann, H., Potdevin, G., Graafsma, H., Nilsson, B., and Spence, J.C.H. (2011) Femtosecond X-ray protein nanocrystallography, Nature, 470, 73-77 (Read online)"
  27. Zhao, Z., Jacovetty, E. L., Liu, Y., and Yan, H. (2011) Encapsulation of Gold Nanoparticles in a DNA Origami Cage, Angewandte Chemie International Edition, 50, 2041-2044 (Read online)"
  28. Ding, B., Wu, H., Xu, W., Zhao, Z., Liu, Y., Yu, H., and Yan, H. (2010) Interconnecting gold islands with DNA origami, Nano Lett., 10, 5065–5069 (Read online)"
  29. Li, Z., Liu, M., Wang, L., Nangreave, J., Yan, H., and Liu, Y. (2010) Molecular behavior of DNA origami in higher order self-assembly, Journal of the American Chemical Society, 132, 13545-13552 (Read online)"
  30. Nangreave, J., Han, D., Liu, Y., and Yan, H. (2010) DNA Origami: A History and Current Perspective, Current Opinion in Chemical Biology, 14, 608-615 (Read online)"
  31. Stephanopoulos, N., Liu, M., Tong, G., Li, Z., Liu, Y., Yan, H., and Francis, M. (2010) Immobilization and One-Dimensional Arrangement of Virus Capsids with Nanoscale Precision Using DNA Origami, Nano Letters, 10, 2714-2720 (Read online)"
  32. Deng, Z., Schulz, O., Lin, S., Ding, B., Liu, X., Wei, X., Ros, R., Liu, Y., Yan, H., and Francis, M. (2010) Aqueous Synthesis of Zinc Blende CdTe/CdS Magic-Core/Thick-Shell Tetrahedral Shaped Nanocrystals with Emission Tunable to Near-Infrared, Journal of the American Chemical Society, 132, 5592-5593 (Read online)"
  33. Pal, S., Deng, Z., Ding, B., Yan, H., and Liu, Y. (2010) DNA Origami Directed Self-Assembly of Discrete Silver Nanoparticle Architectures, Angewandte Chemie International Edition, 49, 2700-2704 (Read online)"
  34. Ding, B., Deng, Z., Yan, H., Cabrini, S., Zukerman, R., and Boker, J. (2010) Gold Nanoparticles Self-Similar Chain Structure Organized by DNA Origami, Journal of the American Chemical Society, 132, 3248-3249 (Read online)"
  35. Zhao, Z., Yan, H., and Liu, Y. (2010) A Route to Scale up DNA Origami Using DNA Tiles as Folding Staples, Angewandte Chemie International Edition, 49, 1414-1417
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