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Creators/Authors contains: "Jordan, Aldo"

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  1. ; ; ; ; ; ; ; (, Dalton Transactions)
    When irradiated with blue light in the presence of a Lewis base (L), [CpW(CO) 3 ] 2 undergoes metal–metal bond cleavage followed by a disproportionation reaction to form [CpW(CO) 3 L] + and [CpW(CO) 3 ] − . Here, we show that in the presence of pyridinium tetrafluoroborate, [CpW(CO) 3 ] − reacts further to form a metal hydride complex CpW(CO) 3 H. The rection was monitored through in situ photo 1 H NMR spectroscopy experiments and the mechanism of light-driven hydride formation was investigated by determining quantum yields of formation. Quantum yields of formation of CpW(CO) 3 H correlate with I −1/2 (I = photon flux on our sample tube), indicating that the net disproportionation of [CpW(CO) 3 ] 2 to form the hydride precursor [CpW(CO) 3 ] − occurs primarily through a radical chain mechanism. 
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  2. ; ; ; ; ; ; (, Chemical Communications)
    The masked Ti( ii ) synthon ( Ket guan)(η 6 -Im Dipp N)Ti ( 1 ) oxidatively adds across thiophene to give ring-opened ( Ket guan)(Im Dipp N)Ti[κ 2 - S (CH) 3 C H] ( 2 ). Complex 2 is photosensitive, and upon exposure to light, reductively eliminates thiophene to regenerate 1 – a rare example of early-metal mediated oxidative-addition/reductive-elimination chemistry. DFT calculations indicate strong titanium π-backdonation to the thiophene π*-orbitals leads to the observed thiophene ring opening across titanium, while a proposed photoinduced LMCT promotes the reverse thiophene elimination from 2 . Finally, pressurizing solutions of 2 with H 2 (150 psi) at 80 °C leads to the hydrodesulphurization of thiophene to give the Ti( iv ) sulphide ( Ket guan)(Im Dipp N)Ti(S) ( 3 ) and butane. 
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  3. ; ; ; ; ; ; ; (, Organometallics)
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  4. ; ; ; (, Dalton Transactions)
    A new diarylmido-based pincer proto ligand ( iPrPNHSbPh ) with one –PPr i 2 and one –SbPh 2 side donor has been synthesized. Three complexes of its amido form were prepared using standard metalation techniques: ( iPrPNSbPh ) PdCl , ( iPrPNSbPh ) RhCO , and ( iPrPNSbPh ) Ir(COE) , where COE = cis -cyclooctene. These complexes were compared with their previously reported analogs incorporating a –PPh 2 side donor in place of –SbPh 2 . The –SbPh 2 donor arm is less donating towards the metal and is less strongly trans -influencing, based on the structural and IR spectroscopic analysis of the Rh complexes. The redox potential of the Pd complexes is only marginally affected by the change from –PPh 2 to –SbPh 2 . (iPrPNSbPh)Ir(COE) proved to be a slower and less selective catalyst in the dehydrogenative borylation of terminal alkynes (DHBTA) than its –PPh 2 analog. 
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