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Fuel Production from Seawater and Fuel Cells Using Seawater
Fukuzumi, Shunichi,Lee, Yong-Min,Nam, Wonwoo Wiley (John WileySons) 2017 ChemSusChem Vol.10 No.22
<P>Seawater is the most abundant resource on our planet and fuel production from seawater has the notable advantage that it would not compete with growing demands for pure water. This Review focuses on the production of fuels from seawater and their direct use in fuel cells. Electrolysis of seawater under appropriate conditions affords hydrogen and dioxygen with 100% faradaic efficiency without oxidation of chloride. Photo-electrocatalytic production of hydrogen from seawater provides a promising way to produce hydrogen with low cost and high efficiency. Microbial solar cells (MSCs) that use biofilms produced in seawater can generate electricity from sunlight without additional fuel because the products of photosynthesis can be utilized as electrode reactants, whereas the electrode products can be utilized as photosynthetic reactants. Another important source for hydrogen is hydrogen sulfide, which is abundantly found in Black Sea deep water. Hydrogen produced by electrolysis of Black Sea deep water can also be used in hydrogen fuel cells. Production of a fuel and its direct use in a fuel cell has been made possible for the first time by a combination of photocatalytic production of hydrogen peroxide from seawater and dioxygen in the air and its direct use in one-compartment hydrogen peroxide fuel cells to obtain electric power.</P>
Fukuzumi, Shunichi,Saito, Kenji,Ohkubo, Kei,Khoury, Tony,Kashiwagi, Yukiyasu,Absalom, Mark A.,Gadde, Suresh,D'Souza, Francis,Araki, Yasuyuki,Ito, Osamu,Crossley, Maxwell J. Royal Society of Chemistry 2011 Chemical communications Vol.47 No.28
<P>Multiple photosynthetic reaction centres have successfully been constructed using supramolecular complexes of zinc porphyrin dendrimers [D(ZnP)<SUB><I>n</I></SUB>: <I>n</I> = 4, 8, 16] with fulleropyrrolidine bearing a pyridine ligand (C<SUB>60</SUB>py). Efficient energy migration occurs completely between the ZnP units of dendrimers prior to the electron transfer with increasing the generation of dendrimers to attain an extremely long charge–separation lifetime.</P> <P>Graphic Abstract</P><P>Efficient energy migration occurs more efficiently between the ZnP units of dendrimers prior to the electron transfer with increasing the generation of dendrimers to attain an extremely long charge–separation lifetime. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c1cc11725d'> </P>
Fukuzumi, Shunichi,Mandal, Sukanta,Mase, Kentaro,Ohkubo, Kei,Park, Hyejin,Benet-Buchholz, Jordi,Nam, Wonwoo,Llobet, Antoni American Chemical Society 2012 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.134 No.24
<P>Four-electron reduction of O<SUB>2</SUB> by octamethylferrocene (Me<SUB>8</SUB>Fc) occurs efficiently with a dinuclear cobalt-μ-1,2-peroxo complex, <B>1</B>, in the presence of trifluoroacetic acid in acetonitrile. Kinetic investigations of the overall catalytic reaction and each step in the catalytic cycle showed that proton-coupled electron transfer from Me<SUB>8</SUB>Fc to <B>1</B> is the rate-determining step in the catalytic cycle.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2012/jacsat.2012.134.issue-24/ja303674n/production/images/medium/ja-2012-03674n_0011.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja303674n'>ACS Electronic Supporting Info</A></P>
Mimicry and functions of photosynthetic reaction centers
Fukuzumi, Shunichi,Lee, Yong-Min,Nam, Wonwoo Biochemical Society 2018 Biochemical Society transactions Vol.46 No.5
<P>The structure and function of photosynthetic reaction centers (PRCs) have been modeled by designing and synthesizing electron donor-acceptor ensembles including electron mediators, which can mimic multi-step photoinduced charge separation occurring in PRCs to obtain long-lived charge-separated states. PRCs in photosystem I (PSI) or/and photosystem II (PSII) have been utilized as components of solar cells to convert solar energy to electric energy. Biohybrid photoelectrochemical cells composed of PSII have also been developed for solar-driven water splitting into H-2 and O-2. Such a strategy to bridge natural photosynthesis with artificial photosynthesis is discussed in this minireview.</P>
Fukuzumi, Shunichi,Ohkubo, Kei,Kawashima, Yuki,Kim, Dong Sub,Park, Jung Su,Jana, Atanu,Lynch, Vincent M.,Kim, Dongho,Sessler, Jonathan L. American Chemical Society 2011 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.133 No.40
<P>Binding of chloride anion to a tetrathiafulvalene calix[4]pyrrole (TTF-C4P) donor results in ET to Li<SUP>+</SUP>@C<SUB>60</SUB> to produce the radical pair (TTF-C4P<SUP>•+</SUP>/Li<SUP>+</SUP>@C<SUB>60</SUB><SUP>•–</SUP>), the structure of which was characterized by X-ray crystallographic analysis. The addition of tetraethylammonium cation, which binds more effectively than Li<SUP>+</SUP>@C<SUB>60</SUB><SUP>•–</SUP> as a guest within the TTF-C4P cavity, leads to electron back-transfer, restoring the initial oxidation states of the donor and acceptor pair.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2011/jacsat.2011.133.issue-40/ja207588c/production/images/medium/ja-2011-07588c_0012.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja207588c'>ACS Electronic Supporting Info</A></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja207588c'>ACS Electronic Supporting Info</A></P>
Hydrogen storage and evolution catalysed by metal hydride complexes
Fukuzumi, Shunichi,Suenobu, Tomoyoshi The Royal Society of Chemistry 2013 Dalton transactions Vol.42 No.1
<P>The storage and evolution of hydrogen are catalysed by appropriate metal hydride complexes. Hydrogenation of carbon dioxide by hydrogen is catalysed by a [C,N] cyclometalated organoiridium complex, [Ir<SUP>III</SUP>(Cp*)(4-(1<I>H</I>-pyrazol-1-yl-κ<I>N</I><SUP>2</SUP>)benzoic acid-κ<I>C</I><SUP>3</SUP>)(OH<SUB>2</SUB>)]<SUB>2</SUB>SO<SUB>4</SUB> [<B>Ir</B>–OH<SUB>2</SUB>]<SUB>2</SUB>SO<SUB>4</SUB>, under atmospheric pressure of H<SUB>2</SUB> and CO<SUB>2</SUB> in weakly basic water (pH 7.5) at room temperature. The reverse reaction, <I>i.e.</I>, hydrogen evolution from formate, is also catalysed by [<B>Ir</B>–OH<SUB>2</SUB>]<SUP>+</SUP> in acidic water (pH 2.8) at room temperature. Thus, interconversion between hydrogen and formic acid in water at ambient temperature and pressure has been achieved by using [<B>Ir</B>–OH<SUB>2</SUB>]<SUP>+</SUP> as an efficient catalyst in both directions depending on pH. The Ir complex [<B>Ir</B>–OH<SUB>2</SUB>]<SUP>+</SUP> also catalyses regioselective hydrogenation of the oxidised form of β-nicotinamide adenine dinucleotide (NAD<SUP>+</SUP>) to produce the 1,4-reduced form (NADH) under atmospheric pressure of H<SUB>2</SUB> at room temperature in weakly basic water. In weakly acidic water, the complex [<B>Ir</B>–OH<SUB>2</SUB>]<SUP>+</SUP> also catalyses the reverse reaction, <I>i.e.</I>, hydrogen evolution from NADH to produce NAD<SUP>+</SUP> at room temperature. Thus, interconversion between NADH (and H<SUP>+</SUP>) and NAD<SUP>+</SUP> (and H<SUB>2</SUB>) has also been achieved by using [<B>Ir</B>–OH<SUB>2</SUB>]<SUP>+</SUP> as an efficient catalyst and by changing pH. The iridium hydride complex formed by the reduction of [<B>Ir</B>–OH<SUB>2</SUB>]<SUP>+</SUP> by H<SUB>2</SUB> and NADH is responsible for the hydrogen evolution. Photoirradiation (<I>λ</I> > 330 nm) of an aqueous solution of the Ir–hydride complex produced by the reduction of [<B>Ir</B>–OH<SUB>2</SUB>]<SUP>+</SUP> with alcohols resulted in the quantitative conversion to a unique [C,C] cyclometalated Ir–hydride complex, which can catalyse hydrogen evolution from alcohols in a basic aqueous solution (pH 11.9). The catalytic mechanisms of the hydrogen storage and evolution are discussed by focusing on the reactivity of Ir–hydride complexes.</P> <P>Graphic Abstract</P><P>Hydrogen storage and evolution were catalysed by [C,N] and [C,C] cyclometalated iridium hydride complexes in water at ambient temperature under atmospheric pressure. <IMG SRC='http://pubs.rsc.org/services/images/RSCpubs.ePlatform.Service.FreeContent.ImageService.svc/ImageService/image/GA?id=c2dt31823g'> </P>
Fukuzumi, Shunichi,Kobayashi, Takeshi,Suenobu, Tomoyoshi American Chemical Society 2010 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.132 No.34
<P>A heterodinuclear iridium−ruthenium complex [Ir<SUP>III</SUP>(Cp*)(H<SUB>2</SUB>O)(bpm)Ru<SUP>II</SUP>(bpy)<SUB>2</SUB>](SO<SUB>4</SUB>)<SUB>2</SUB> (Cp* = η<SUP>5</SUP>-pentamethyl-cyclopentadienyl, bpm = 2,2′-bipyrimidine, bpy = 2,2′-bipyridine) acts as an effective catalyst for removal of dissolved O<SUB>2</SUB> by the four-electron reduction of O<SUB>2</SUB> with formic acid in water at an ambient temperature.</P><P><B>Graphic Abstract</B> <IMG SRC='http://pubs.acs.org/appl/literatum/publisher/achs/journals/content/jacsat/2010/jacsat.2010.132.issue-34/ja104486h/production/images/medium/ja-2010-04486h_0007.gif'></P><P><A href='http://pubs.acs.org/doi/suppl/10.1021/ja104486h'>ACS Electronic Supporting Info</A></P>