研究领域
Photochemistry, Materials, Transition Metal Chemistry
Light Harvesting
Chemists can play a significant role in the search for new sources of renewable energy to help meet future world energy needs. Of all the prospective renewable energy sources, solar offers the greatest potential return (as much as ten times the world energy needs expected at the end of this century). One area of solar energy related research for chemists is the study of photochemical reactions of molecules that absorb visible light.
Our research includes considerable organic and inorganic synthesis. Our recent efforts have focused on preparing clusters of visible light absorbing chromophores that may be used to "harvest" light. Such light harvesting arrays can be used to channel energy into electrochemical cells designed to convert light to electrical energy (photoelectrochemical cells). The types of chromophores we have examined include porphyrins , phthalocyanines and a variety of transition metal complexes. Through a combination of synthetic and laser spectroscopic investigations, our group studies the factors that influence the reactivity and stability of these classes of visible chromophores.
Photocatalysts
Another area of research in our group, related to solar energy conversion to chemical energy, is the study of what is referred to as one photon-two electron reactions. Using transition metal complexes that undergo two electron redox processes (i.e. Pt(II) to Pt(IV)), we are attempting to develop photochemical systems that can undergo redox cycling to serve as photocatalysts for the production of useful reagents.
Materials
Many of the N-heterocyclic ligands we prepare for light harvesting systems are strongly luminescent and are related to materials used for the development of organic light emitting diodes (OLEDs). The ligands have emission that can be tuned to span the visible spectrum.
We are currently exploring the luminescence behavior of these complexes in solution and on surfaces. By gaining control of surface morphology via various surface deposition techniques, we hope to prepare highly luminescent surface bound chromophores that can be used in OLEDs or sensing applications. We study surface marpology using scanning electron microscopy (SEM) and (TEM).
近期论文
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Mengyuan Zhu, Gyan H Aryal, Nan Zhang, Hong Zhang, Xiaoye Su, Russell Schmehl, Xue Liu, Jin Hu, Jiang Wei, and Janarthanan Jayawickramarajah "Host-guest interactions derived multilayer perylene diimide thin film constructed on a scaffolding porphyrin monolayer" Langmuir, 2015, 31 (1), pp 578–586. DOI: 10.1021/la504297w.
Bing Shan and Russell H. Schmehl "Photochemical Generation of Strong One-Electron Reductants via Light-Induced Electron Transfer with Reversible Donors Followed by Cross Reaction with Sacrificial Donors" J. Phys. Chem. A, 2014,118, 10400-10406. http://pubs.acs.org/doi/abs/10.1021%2Fjp503901v
Tod A. Grusenmeyer; Albert W. King; Joel T. Mague; Jeffrey J. Rack and Russell H. Schmehl, “Sn(IV) Schiff Base Complexes: Triplet Photosensitizers for Photoredox Reactions” Dalton Transactions, 2014, 43 (47), 17754-17765. DOI: 10.1039/c4dt01427h
Jing Gu, Yong Yan, Brian J.Helbig, Zhuangqun Huang, Tianquan Lian and Russell H. Schmehl “The influence of ligand localized excited states on the photophysics of second and third row transition metal terpyridyl complexes: recent examples and a case study”, Coord. Chem. Rev., 2014, in. press. DOI: 10.1016/j.ccr.2014.06.028
Yuankai Yue, Tod Grusenmeyer, Zheng Ma, Peng Zhang, Russell H. Schmehl, David N. Beratan, Igor V. Rubtsov “Full-Electron Ligand-to-Ligand Charge Transfer in a Compact Re(I) Complex”, J. Phys. Chem., A., 2014, 118, 10407-10415. DOI 10.1021/jp5039877.
Hong Zhang, Boyu Zhang, Mengyuan Zhu, Scott M. Grayson, Russell Schmehl, Janarthanan Jayawickramarajah Water-soluble porphyrin nanospheres: enhanced photo-physical properties achieved via cyclodextrin driven double self-inclusion, Chem. Commun., 2014, 50 (37), 4853-55. DOI: 10.1039/c4cc01372g.
Tingting Feng, Max Lupin, Tod A. Grusenmeyer and Russell H. Schmehl, “Following Oxygen Consumption In Singlet Oxygen Reactions Via Changes In Sensitizer Phosphorescence” Photochemistry and Photobiology, 2014, on line (issue in memory of Michael Kasha). DOI: 10.1111/php.12381.
Yue, Yuankai; Grusenmeyer, Tod; Ma, Zheng; Zhang, Peng; Mague, Joel T.; Donahue, James P.; Schmehl, Russell H.; Beratan, David N.; Rubtsov, Igor V. " Evaluating the extent of intramolecular charge transfer in the excited states of rhenium(I) donor-acceptor complexes with time-resolved vibrational spectroscopy " J. Phys. Chem., B., 2013, ASAP. http://dx.doi.org/10.1021/jp409628e
Shan, Bing; Baine, T.; Ma, X.A.N.; Zhao, Xuan; Schemehl, Russell, "Mechanisitic Details for Cobalt Catalyzed Photochemical Hydrogen Production in Aqueous Solution: Efficiencies of the Non-Photochemical Steps" Inorg. Chem., 2013, 52(9), oo 4853-4850. DOI: 10. 1021/ic302381w.
Grusenmeyer, Tod A.; Chen, Jin; Jin, Yuhuan; Nguyen, Jonathan; Rack, Jeffrey J.; Schmehl, Russell H. "ph Control of Intramolecular Energy Transfer and Oxygen Quenching in Ru(II) Complexes Having Coupled Electronic Excited States" J. Am. Chem. Soc., 2012, 134, 7497-7506/ DOI 10.1021/ja30086.
Choi, Nakwon; Verbridge, Scott S.; Williams, Rebecca M.; Chen, Jin; Kim, J-Y.; Schmehl, Russell; Farnum, Cornelia E.; Zipfel, Warren R.; Fischbach, Claudia; Stroock, Abraham D.; "Phosphorescent nanoparticles for quantitative measurements of oxygen profiles in vitro and in vivo" Biomaterials, 2012, 33, 2710-2722.
Vaidya, Srivathsa and Schmehl, Russell H. “Vapor phase pH induced fluorescence switching of a dimethylaminostyryl terpyridine derivative in thin films “ New J. Chem., (2012) 36, 52-55.
Kurtz, J. P.; Grusenmeyer, T.; Tong, L.; Kosgei, G.; Schmehl, R. H.; Mague, J. T.; Pascal, R. A., Jr. “Highly luminescent, polyaryl mesobenzanthrones.” Tetrahedron, (2011) 67, 7211-7216.
Fathalla, M.; Neuberger, A.; Li, S.; Schmehl, R.; Diebold, U.; Jayawickramarajah, J. “Straightforward Self-Assembly of Porphyrin Nanowires in Water: Harnessing Adamantane/beta-Cyclodextrin Interactions”. J. Am. Chem. Soc., 2010) 132, 9966-9967.
Jing Gu, Jin Chen, Russell H. Schmehl "Using Intramolecular Energy Transfer to Transform non-Photoactive, Visible-Light-Absorbing Chromophores into Sensitizers for Photoredox Reactions, J. Am. Chem. Soc. (2010) 132, 7338-46.
Jarosz, P; Lotito, K; Schneider, J; Kumaresan, D; Schmeh,l R; Eisenberg, R “Platinum(II) Terpyridyl-Acetylide Dyads and Triads with Nitrophenyl Acceptors via a Convenient Synthesis of a Boronated Phenylterpyridine”, Inorg. Chem., (2009) 48, 2420.
Duraisamy Kumaresan, Kristi Lebkowsky and Russell H. Schmehl "Photophysical Charge Separation and Recombination in Solution and in Gels of a Pt(II) Terpyridyl-Naphthalene Diimide Copmlex", J. Photochem. Photobiol. A: Chemistry (in honor of Haruo Inoue), (2009, 207, 86-93.
Paul Jarosz, Jason thall, Jacob Schneider, Duraisamy Kumaresan, Russell Schmehl, and Richard Eisenberg "Synthesis Characterization, and Photophysical Properties of Platinum(II) Terpyridyl-based Multi-component Systems", Energy and Environmental Science (2008), 1, 573.
Akatsuka, Kosho; Ebina, Yasuo; Muramatsu, Masaru; Sato, Toshiyuki; Hester, Heidi; Kumaresan, Duraisamy; Schmehl, Russell H.; Sasaki, Takayoshi; Haga, Masa-Aki. Photoelectrochemical Properties of Alternating Multilayer Films Composed of Titania Nanosheets and Zn Porphyrin. Langmuir (2007), 23(12), 6730-6736
Vaidya, Srivathsa; Johnson, Claire; Wang, Xian-Yong; Schmehl, Russell H.. Fluorescence solvato and vapochromism of a dimethylaminostyryl terpyridine derivative. Journal of Photochemistry and Photobiology, A: Chemistry (2007), 187(2-3), 258-262