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  • 1.
    Hsu, Yu-Cheng
    et al.
    Acad Sinica, Inst Chem, Taipei 11529, Taiwan;Natl Taiwan Univ, Dept Chem, Taipei 10161, Taiwan.
    Wang, Vincent Cho-Chien
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry. Acad Sinica, Inst Chem, Taipei 11529, Taiwan.
    Au-Yeung, Ka-Chun
    Acad Sinica, Inst Chem, Taipei 11529, Taiwan.
    Tsai, Chung-Yu
    Acad Sinica, Inst Chem, Taipei 11529, Taiwan.
    Chang, Chun-Chi
    Acad Sinica, Inst Chem, Taipei 11529, Taiwan.
    Lin, Bo-Chao
    Acad Sinica, Inst Chem, Taipei 11529, Taiwan.
    Chan, Yi-Tsu
    Natl Taiwan Univ, Dept Chem, Taipei 10161, Taiwan.
    Hsu, Chao-Ping
    Acad Sinica, Inst Chem, Taipei 11529, Taiwan.
    Yap, Glenn P. A.
    Univ Delaware, Dept Chem & Biochem, Newark, DE 19716 USA.
    Jurca, Titel
    Univ Cent Florida, Dept Chem, Orlando, FL 32816 USA;Univ Cent Florida, Cluster Rational Design Catalysts Energy Applicat, Orlando, FL 32816 USA.
    Ong, Tiow-Gan
    Acad Sinica, Inst Chem, Taipei 11529, Taiwan;Natl Chiao Tung Univ, Dept Appl Chem, Hsinchu 300, Taiwan.
    One-Pot Tandem Photoredox and Cross-Coupling Catalysis with a Single Palladium Carbodicarbene Complex2018In: Angewandte Chemie International Edition, ISSN 1433-7851, E-ISSN 1521-3773, Vol. 57, no 17, p. 4622-4626Article in journal (Refereed)
    Abstract [en]

    The combination of conventional transition-metal-catalyzed coupling (2e(-) process) and photoredox catalysis (1e(-) process) has emerged as a powerful approach to catalyze difficult cross-coupling reactions under mild reaction conditions. Reported is a palladium carbodicarbene (CDC) complex that mediates both a Suzuki-Miyaura coupling and photoredox catalysis for C-N bond formation upon visible-light irradiation. These two catalytic pathways can be combined to promote both conventional transition-metal-catalyzed coupling and photoredox catalysis to mediate C-H arylation under ambient conditions with a single catalyst in an efficient one-pot process.

  • 2.
    Wang, Vincent Cho-Chien
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Esmieu, Charlène
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Redman, Holly J.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Berggren, Gustav
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics.
    Hammarström, Leif
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    The reactivity of molecular oxygen and reactive oxygen species with [FeFe] hydrogenase biomimetics: reversibility and the role of the second coordination sphere2020In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 49, no 3, p. 858-865Article in journal (Refereed)
    Abstract [en]

    The development of oxygen-tolerant H-2-evolving catalysts plays a vital role for a future H-2 economy. For example, the [FeFe] hydrogenase enzymes are excellent catalyst for H-2 evolution but rapidly become inactivated in the presence of O-2. The mechanistic details of the enzyme's inactivation by molecular oxygen still remain unclear. Here, two H-2-evolving diiron complexes [Fe-2(mu-SCH2NHCH2S)(CO)(6)] (1(adt)) and [Fe-2(mu-SCH2CH2CH2S)(CO)(6)] (2(pdt)), inspired by the active site of [FeFe] hydrogenase, were investigated for their reactivity with molecular oxygen and reactive oxygen species. A one-electron reduced and oxygenated 1(adt) species was identified and characterized spectroscopically, which can be directly generated by reacting with molecular oxygen and chemical reductants at room temperature but it is unstable and gradually decomposes. Interestingly, the whole process is reversible and the addition of protons can facilitate the deoxygenation process and prevent further degradation at room temperature. This new identification of intermediate species serves as a model for studying the reversible inactivation and degradation of oxygen-sensitive [FeFe] hydrogenases by O-2, and provides chemical precedence for such processes. In comparison, the complex lacking the nitrogen bridgehead, 2(pdt), exhibits reduced reactivity towards O-2 in the presence of reductants, highlighting that the importance of the second coordination sphere on modulating the oxygenation processes. These results provide new directions to design molecular electrocatalysts for proton reduction operated at ambient conditions and the re-engineering of [FeFe] hydrogenases for improving oxygen tolerance.

  • 3.
    Wang, Vincent Cho-Chien
    et al.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Physical Chemistry.
    Johnson, Ben A.
    Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Synthetic Molecular Chemistry.
    Interpreting the Electrocatalytic Voltammetry of Homogeneous Catalysts by the Foot of the Wave Analysis and Its Wider Implications2019In: ACS Catalysis, ISSN 2155-5435, E-ISSN 2155-5435, Vol. 9, no 8, p. 7109-7123Article in journal (Refereed)
    Abstract [en]

    Mechanistic studies of electrocatalytic reactions play a crucial role in developing efficient electrocatalysts and solar-fuel devices. The foot of the wave analysis (FOWA) for cyclic voltammetry, recently developed by Saveant and Costentin, provides a powerful means to evaluate the performance of molecular electrocatalysts. However, there is a considerable amount of confusion in the community on how to interpret FOWA in multielectron electrochemical reactions. Herein, we further expand their earlier models from the Nernstian region to all scenarios (i.e., including non-Nernstian behavior) and systematically examine individual parameters, such as formal potentials and reaction rate constants, to explore deeper insights and limitations. Detailed analysis from in silico voltammograms based on different mechanistic models reveals characteristic features of FOWA traces for different kinetic phenomena, which is useful to diagnose kinetic profiles and elucidate the limits of FOWA. The lessons learned from these analyses are further used to reconcile the discrepancy of rate constants determined by FOWA versus other methods, such as time-resolved spectroscopy, for molecular electrocatalysts that catalyze proton reduction or the reduction of CO2 to CO. Such reconciliation demonstrates that electrochemical methods along with FOWA can serve as an alternative tool to determine kinetic information and probe mechanistic insights, which otherwise may be challenging and complicated to achieve by conventional methods. In addition, general guidelines and warnings are also presented to avoid potential errors or mishandling when using FOWA.

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