Mamoru Nango / Profile and research work
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PhD 1974 from University of Osaka Prefecture. Post-Doctoral Fellow at Northwestern University for 1974-1976 and returned to Department of Applied Chemistry, University of Osaka Prefecture as Assistant Professor in 1976 . Visiting research associate at Northwestern University in 1981. Associate Professor, Professor at Nagoya Institute of Technology in 1990-2010. Retirement of Nagoya Institite of Technology in 2010, a Professor Emeritus and at the present; Specially-Appointed Professor Nagoya Institute of Technology and Osaka-city University, Institute of Integrated Advanced Research(OCARINA).
Biofunctional chemistry, Bioinspired Chemisry, Artificial Photosynthesis
The purpose of this proposal is to use photosynthetic pigment complexes of purple photosynthetic bacteria or green plant in order to construct an artificial photosynthesis assembling these complexes on electrodes with a fine direction and orientation for developing solar PV and fuel cells. The advantage of the pigment complex is its high efficiency of light-energy conversion throughout the near UV to near IR region and much higher durability using these methods than ordinary light-harvesting (LH) complex isolated from photosynthetic bacteria or green plant. Expanding existing PV technologies by incorporation of modified photosynthetic protein/pigments complexes or their protein-mimic materials to perform tasks of light-harvesting and charge separation, is currently explored as a novel concept, which makes use of natural protein environments to create a directional flow of light energy and electronic charge separation, meanwhile reducing the cost aspect by the use of bio-materials and their synthetic protein-mimic materials. The majority of the aim is construction of the array of artificial photosynthetic system with patterning substrate and building solar batteries and solar fuel using modified photosynthetic protein materials prepared from modern biosynthetic manufacturing methods and photosynthetic pigments for energy harvesting materials.
1.Artificial Photosynthetic Antenna and Development of Nanobiodevices.
i)Artificial domain assembly of LH pigment complexes from photosynthetic bacterial membranes on nanopatterning and lipid modified substrates to construct efficient energy harvesting and electron transfer systems.
The LH pigment-protein complexes of photosynthetic bacterial membrane complexes (LH2 and LH1-RC) were laid down onto functionalized electrodes, such as ITO, Au and SiO2 electrodes modified with or without lipid bilayers. Upon illumination photocurrents were successfully measured. Excitation spectra confirmed that these photocurrents was produced by light absorbed by the pigment-protein complexes. It proved critical in these studies to capitalize on our knowledge of the behavior of these complexes to select those that are the most stable and well organized. The best results was only obtained with the subset of the most stable complexes, the combination of LH2-SH and C-His-tag LH1-RC assembly onto SiO2 and Au, respectively which the orientation and direction of these complexes are controlled. These studies were examined to correlate the supramolecular organization of the complexes on the electrodes with an efficient capture of photons. AFM and EM studies resolved the organization of antenna complexes both in reconstituted lipid bilayers and in native photosynthetic membranes. These techniques are now being applied to investigate the organization of the antenna complexes and their synthetic model complexes on the electrodes. This work required very careful attention to detail and the current pictures are very exciting. A clear fluorescence of LH2 with SH-tag was observed at the Mal sites on the substrate with lined patterning when illuminated at near IR region. Following this study, LH1-RC with His-tag was further assembled on the NTA site to produce an efficient energy transfer from LH2 to LH1-RC on the same substrate for development of new type of nano-sensors and nano-semiconductors (nanobiophotonics). We could see an enhanced photocurrent of LH1-RC due to the co-assembly of LH2 on the same electrode with this patterning. This method of approach will be useful for constructing a new type of solar cell. Following this research, clear fluorescence lines can be observed on gold electrode with more fined pattern due to the presence of lipid bilayers. In contrast, no fluorescence was observed without lipid bilayers. This result fist showed that a method for yielding the fluorescence of LH2 complex was demonstrated by using a lipid-modified surface on the gold substrate, which is more easy for patterning in comparison to other substrates. This method of approach, applying to gold surface is very useful for constructing a new type of solar cell with more fined pattern.
ii) Artificial domain assembly of LH1-RC on lipid modified substrates to construct an efficient energy transfer system.
From measurements of the conductive AFM, clear rectification was observed, indicating that LH1-RC is well organized on AU electrode with a defined orientation due to the presence of lipid bilayers and thus electron is efficiently transfer from gold electrode to Pt via LH1-RC complex. Further, from results of the photocurrent measurements, photocurrent response of LH1-RC on APS-ITO modified with lipid bilayers was clearly observed in the presence of UQ-10 as well as UQ-1. UQ-10 which can be easily embedded into lipid bilayers showed an enhanced photocurrent in comparison to UQ-1. This method of approach using lipid bilayers will be very useful for the assembly of the LH complexes on electrodes with pattern and a defined orientation for construction of solar cell with the functions of photo-response and photo-electric currents.
2.Artificial domain assembly of LH pigment complexes and their model complexes to construct energy transfer systems.
This MBP modified-rubrum LH- with His-tag /Zn-Chlorins complex was successfully immobilized onto modified Au electrodes and cathodic photocurrent was observed, irradiated at the Soret and Qy bands of Zn-Chlorins. These findings imply a versatile capability of the LH polypeptide to assemble various kinds of pigments analogs that can facilitate efficient energy and electron transfer, leading to the construction of photosensitive energy transfer materials, "artificial leaf" as well as solar cell. Taken together, the results of this study suggest that the genetically engineered MBP modified-rubrum LH- with His-tag is useful for construction of artificial photosynthetic antenna systems based on the promising methodology using functional hydrophilic domains, His-tag and MBP for immobilization onto electrodes with a defined orientation and as a molecular landmark for AFM observation at the molecular level, respectively.
Nature provides a number of examples, in which processes of energy conversion, storage and transport are combined and optimized through 'smart matrices' at various levels, going from molecular to cellular or higher organisms in photosynthetic bacterias and plants. Based on biological design principles, future biology-based photonics or their synthetic organic materials could form clean and inexpensive future alternatives for productions of nano-semiconductors and constructing fuelization's system of hydrogen and carbon dioxide (the artificial leaf). The light-harvesting mechanisms in these light-harvesting complexes cellular or higher organisms in photosynthetic bacteria and plants have been studied both spectroscopically and theoretically. These advances put us in a unique position of being able to exploit this information to design artificial photosynthetic antenna systems based on 'biological blueprint'. Our aim is to see if we could produce an antenna module, which acts as a 'sensitizer', and a light-induced redox component for nano-biophotonics and nanobiomaterial (the artificial leaf ) from solar to fuel.
We proposed a scenario where the construction of electron transfer system analogous to artificial photosynthetic system from photosynthetic bacterias and plants with patterning substrate is expected to start from molecular and supra-molecular entities in a variety of smart matrices that collect light energy and separate charge for developing new types of nanobiodevices and for the artificial leaf to construct the fuelization system from solar to fuel.
- "Solar to Chemical Energy Conversion", M. Sugiyama, K.Fujii & S. Nakamura eds., Springer, Lecture Notes Energy 32, Part IV. pp.437-4554,(2016) M.Kondo, T.Dewa, M.Nango, “Electronic Device Approach Using Photosynthesis Assembly of Photosynthetic Protein Complexes for the Development of Nanodevice”.
- M. Nango, M. Sugiura ed., "Photosynthesis and artificial photosynthesis research", Res Chem Intermed, 40, 9, Springer (2014).
- "Supramolecules, Self-Assemblies, and Organized Films", K. Ariga, H. S. Nalwa eds., (ASP),Vol. 2, Chap. 6, pp.177-198, (2009); M. Nango, M. Nagata, K. Iida, T. Dewa, "Assembly of Bacteriochlorophyll a Complexes Using Light-harvesting Polypeptide from Photosynthetic Bacteria and Its Model Synthetic Polypeptides".
- "The Purple Photosynthetic Bacteria", C.N. Hunter, F. Daldal, M. C. Thurnauer, J. T. Beatty eds., (Springer, Dordrecht), Vol. 28, Chap. 43, pp. 861-875 (2008); K. Iida, T. Dewa, *M. Nango, "Assembly of Bacterial Light Harvesting Complexes on Solid Substrates".
- In "Chlorophylls and Bacteriochlirophylls", ed by B.Grimm, R.J.Porra, W.Rüdiger, H.Scheer, Springer, 25 (2006) 365-373; M.Nango, "Molecular Assembly of Bacteriochlorophyll Complexes Using Synthetic Light-harvesting (LH) Model Polypeptides".
- Y. Yoneda, T. Noji, T. Katayama, N. Mizutani, D. Komori, M. Nango, H. Miyasaka, S. Itoh, Y. Nagasawa, T. Dewa, "Extension of Light-Harvesting Ability of Photosynthetic Light-Harvesting Complex 2 (LH2) through Ultrafast Energy Transfer from Covalently Attached Artificial Chromophores", J. Am. Chem. Soc. 137, 13121 (2015).
- M. Kondo, S. Ishigure, Y. Maki, T.Dewa, M. Nango, Y.Amao, "Photoinduced hydrogen Production with photosensitsization of Zn Chrorophyll analog dimer as a phtososynsthetic special pair model", J. Hydrogen Energy, 40,5313-5318 (2015).
- M. Kondo, M.Amano, T.Joke, S. Ishigure, T.Noji, T.Dewa, Y.Amao , M. Nango, "Immobilization of Photosystem I or II Complexes on Electrodes for Photoenergy-ConversionDevices", Res Chem Intermed, 40, 3287-3293 (2014).
- T. Noji, M. Kondo, T.Jin, T.Yazawa, H. Osuka, Y. Higuchi, M. Nango, S. Itoh, T. Dewa, "Light-Driven Hydrogen Production by Hydrogenases and a Ru- Complex inside a Nanoporous Glass Plate under Aerobic External Conditions", J. Phys.Chem. Lett., 5, 2403-2407(2014).
- M.Kondo, M. Amano, F. Kaoru , A.Okuda, S. Isigure, T. Dewa, Y.Amao, H. Hashimoto, M. Nango, "Self-assembly of the light-harvesting complex of photosystem II (LHCII) on alkanethiol-modified gold electrodes", Res Chem Intermed, 40, 3277-3285 (2014).
- T. Noji, M. Kondo, K. Kawakami, Jian-ren Shen, M. Nango, T. Dewa, "Durability of oxygen evolution of photosystem II incorporated into lipid bilayers", Res Chem Intermed, 40, 3231-3241 (2014).
- T.Dewa, A.Sumino, N. Watanabe, T. Noji, M. Nango, "Structure-function relationships of the supramolecular assembly of the bacterial photosynthetic antenna complexes in lipid membranes", Res Chem Intermed, 40, 3243-3256 (2014).
- A. Sumino, T. Dewa, T. Noji, Y.Nakano, N.Watanabe, R. Hildner, N. Bösch, J. Köhler, M. Nango, "Phospholipids Modulate Self-Assembled Nanostructure and Energy Transfer of the Light-Harvesting Complex 2 in Lipid Bilayers", J. Phys. Chem. B,117, 10395-10404 (2013).
- T. Dewa, A. Sumino, N. Watanabe, T. Noji, M. Nango, "Energy Transfer and Clustering of Photosynthetic Light-Harvesting Complexes in Reconstituted Lipid Membranes", Chem. Phys., 419, 200-204 (2013).
- E. Kenjo, T. Asai, T. Dewa, M. Nango, N. Oku, "Systemic delivery of small interfering RNA by use of targeted polycation liposomes for cancer therapy", Biol. Pharm. Bull., 36, 287-291 (2013).
- H. Ando, A. Okamoto, M. Yokota, K. Shimizu, T. Asai, T. Dewa, M. Nango, N. Oku, "Development of a miR-92a delivery system for antiangiogenesis-based cancer therapy", J. Gene Med., 15, 20-27 (2013).
- S.Tubasum, S.Sakai, T.Dewa, V.Sundstrom, S. Ivan, M. Nango, T. Pullerits, "Anchored LH2 Complexes in 2D Polarization Imaging", J. Phys. Chem.B, 117, 11391-11396(2013).
- S. Sakai, T. Noji, M. Kondo, T. Mizuno, T. Dewa, T. Ochiai, Y. Hisanori,S.Ito, H.Hashimoto, M. Nango, "Molecular Assembly of Zinc Chlorophyll Derivatives by Using Recombinant Light-Harvesting Polypeptides with His-tag and Immobilization on a Gold Electrode",Langmuir, 29, 5104-5109(2013).
- A.Sumino, T. Dewa, N. Sasaki, M. Kondo. M. Nango, "Electron Conduction and Photocurrent Generation of Light-Harvesting/ Reaction Center Core Complex in Lipid Membrane Environments", J. Phys. Chem. Lett., 4, 1087-1092(2013).
- N. Yonenaga, E. Kenjo, T. Asai, A. Tsuruta, K. Shimizu, T. Dewa, M. Nango, N. Oku, "RGD-based active targeting of novel polycation liposomes bearing siRNA for cancer treatment", J. Cont. Release, 160, 177-181 (2012).
- S. Yajima, R.A. Furukawa, M. Nagata, S. Sakai, M. Kondo, K.Iida, T. Dewa, and M. Nango, "Two-dimensional patterning of bacterial light-harvesting 2 complexes on lipid-modified gold surface", Appl. Phys. Lett., 100, 233701 (2012).
- M. Nagata, M. Amano, T.Joke, K. Fuji, A. Okuda, M. Kondo, S.Ishigure, T. Dewa, K. Iida, F. Secundo, Y. Amao, H.Hashimoto, M. Nango, "Immobilization and Photocurrent Activity of a Light-Harvesting Antenna Complex II, LHCII Isolated from a Plant on Electrodes", ACS Macro Lett., 1, 296-299(2012).
- T. Ochiai, M. Nagata, K. Shimoyama, T. Kato, T. Asaoka, M. Kondo, T. Dewa, K. Yamashita, A. Kashiwada, S. Futaki, H. Hashimoto, M. Nango, "Two-Dimensional Molecular Assembly of Bacteriochlorophyll a Derivatives Using Synthetic Poly(Ethylene Glycol)-Linked Light-Harvesting Model Polypeptides on a Gold Electrode Modified with Supported Lipid Bilayers", ACS Macro Lett., 1, 28-22(2012).
- M.Kondo, K. Iida, T. Dewa, H. Tanaka, T. Ogawa, S. Nagashima, K. V. P. Nagashima, K.Shimada, H. Hashimoto, A. T. Gardiner, R. J. Cogdell, M. Nango , "Photocurrent and Electronic Activities of Oriented-His-tagged Photosynthetic Light-Harvesting/Reaction Centre Core Complexes Assembled onto a Gold Electrode", Biomacromolecules, 13, 432-438(2012).
- H. Koide, T. Asai, K. Furuya, T. Tsuzuku, H. Kato, T. Dewa, M. Nango, N. Maeda, N. Oku, "Inhibition of Akt (ser473) phosphorylation and rapamycin-resistant cell growth by knockdown of mammalian target of rapamycin with siRNA in VEGFR-1-targeting vector", Biol. Pharm. Bull., 34, 602-608 (2011).
- S. Sakai, A. Hiro, A. Sumino, T. Mizuno, T. Tanaka, H. Hashimoto, T. Dewa, M. Nango, "Reconstitution and Organization of Photosynthetic Antenna Protein Complex Bearing Functional Hydrophilic Domains", Chem. Lett., 40, 1280-1282, (2011).
- T. Asai, S. Matsushita, E. Kenjo, T. Tsuzuku, N. Yonenaga, H. Koide, K. Hatanaka, T. Dewa, M. Nango, N. Maeda, H. Kikuchi, N. Oku, "Dicetyl phosphate-tetraethylenepentamine-based Liposomes for Systemic siRNA Delivery", Bioconjugate Chem., 22 429-435 (2011).
- S. Sakai, A. Hiro, M. Kondo, T. Mizuno, T. Tanaka, T. Dewa, M. Nango, "Overexpression of Rhodobacter sphaeroides PufX-bearing maltose-binding protein and its effect on the stability of reconstituted light-harvesting core antenna complex", Photosynthesis Res., 111, 63-69(2011).
- A. Sumino, T. Dewa, T. Takeuchi, R. Sugiura, N. Sasaki, N. Misawa, R. Tero, T. Urisu, A.T. Gardiner, R.J. Cogdell, H. Hashimoto, M. Nango "Construction and Structural Analysis of Tethered Lipid Bilayer Containing Photosynthetic Antenna Proteins for Functional Analysis", Biomacromolecules, 12, 2850-2858(2011).
- Ayumi Sumino, Takehisa Dewa, Masaharu Kondo, Takashi Morii, Hideki Hashimoto, Alastair Gardiner, Richard Cogdell, and M. Nango, "Selective Assembly of Photosynthetic Antenna Proteins into a Domain-Structured Lipid Bilayer for the Construction of Artificial Photosynthetic Antenna Systems: Structural Analysis of the Assembly using Surface Plasmon Resonance and Atomic Force Microscopy",Lamgmuir, 27, 1092-1099(2011).
- Shuichi Ishigure, Takashi Joke, Yoshito Takeuchi, Kotaro Kuzuya, Tatsuro Mitsui, Shingo Ito, Yuji Kondo, Shigeki Kawabe, Masaharu Kondo, Takehisa Dewa, Keiji Yamashita, Hiroyuki Mino, Shigeru Itoh , and M. Nango, "Peroxide Decoloration of CI Acid Orange 7 Catalyzed by Manganese Chlorophyll Derivatives at the Surfaces of Micelles and Lipid Bilayers", Langmuir, 26, 7774-7782(2010).
- Takehisa Dewa, Tomohiro Asai, Yuka Tsunoda, Kiyoshi Kato, Daisuke Baba, Misa Uchida, Ayumi Sumino, Kayoko Niwata, Takuya Umemoto, Kouji Iida, Naoto Oku and M. Nango, "Liposomal Polyamine-Dialkyl Phosphate Conjugates as Effective Gene Carriers: Chemical Structure, Morphology, and Gene Transfer activity", Bioconjugate Chem. 21, 844-852 (2010).
- Tsuyoshi Ochiai, Morio Nagata, Kosuke Shimoyama, Mizuki Amano,Masaharu Kondo, Takehisa Dewa, Hideki Hashimoto, and M. Nango, "Immobilization of Porphyrin Derivatives with a Defined Distance andOrientation onto a Gold Electrode Using Synthetic Light-Harvestingα-Helix Hydrophobic Polypeptides", Langmuir, 26(18), 14419-14422 (2010).
- H. Oikawa, S. Fujiyoshi, T. Dewa, M. Nango and M. Matsushita "How Deep Is the Potential Well Confining a Protein in a Specific Conformation? A Single-Molecule Study on Temperature Dependence of Conformational Change between 5 and 18 K", J. Am. Chem. Soc., 130, 4580(2008).
- K. Nakagawa, S. Suzuki, R. Fujii, A. T. Gardiner, R. J. Cogdell, M. Nango, and H. Hashimoto "Probing the Effect of the Binding Site on the Electrostatic Behavior of a Series of Carotenoids Reconstituted into the Light-harvesting 1 Complex from Purple Photosynthetic Bacterium Rhodospirillum rubrum Detected by Stark Spectroscopy", J. Phys. Chem., 112, 9467-9475(2008).