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      The hangman effect boosts hydrogen production by a manganese terpyridine complex

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          Abstract

          By virtue of a hangman effect, a manganese terpyridine complex catalyzes electrochemical hydrogen evolution from phenol in acetonitrile solution and achieves a turnover frequency of 525 s −1 with an overpotential of ca. 230 mV.

          Abstract

          The manganese terpyridine complex 1 with a coordinated carboxylate in the axial position was obtained in situ. By virtue of a hangman effect, complex 1 catalyzes electrochemical hydrogen evolution from phenol in acetonitrile solution with a turnover frequency of 525 s −1 at a low overpotential of ca. 230 mV.

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          [Mn(bipyridyl)(CO)3Br]: An Abundant Metal Carbonyl Complex as Efficient Electrocatalyst for CO2 Reduction

          Marc Bourrez, Florian Molton, Sylvie Chardon-Noblat … (2011)
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            Proton-Coupled Electron Transfer Guidelines, Fair and Square

            Robin Tyburski, Tianfei Liu, Starla D Glover … (2021)
            Proton-coupled electron transfer (PCET) reactions are fundamental to energy transformation reactions in natural and artificial systems and are increasingly recognized in areas such as catalysis and synthetic chemistry. The interdependence of proton and electron transfer brings a mechanistic richness of reactivity, including various sequential and concerted mechanisms. Delineating between different PCET mechanisms and understanding why a particular mechanism dominates are crucial for the design and optimization of reactions that use PCET. This Perspective provides practical guidelines for how to discern between sequential and concerted mechanisms based on interpretations of thermodynamic data with temperature-, pressure-, and isotope-dependent kinetics. We present new PCET-zone diagrams that show how a mechanism can switch or even be eliminated by varying the thermodynamic (ΔG PT ° and ΔG ET °) and coupling strengths for a PCET system. We discuss the appropriateness of asynchronous concerted PCET to rationalize observations in organic reactions, and the distinction between hydrogen atom transfer and other concerted PCET reactions. Contemporary issues and future prospects in PCET research are discussed.
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              The hydrophilic phosphatriazaadamantane ligand in the development of H2 production electrocatalysts: iron hydrogenase model complexes.

              Rosario Mejia-Rodriguez, Daesung Chong, Joseph H. Reibenspies … (2004)
              As functional biomimics of the hydrogen-producing capability of the dinuclear active site in [Fe]H(2)ase, the Fe(I)Fe(I) organometallic complexes, (mu-pdt)[Fe(CO)(2)PTA](2), 1-PTA(2), (pdt = SCH(2)CH(2)CH(2)S; PTA = 1,3,5-triaza-7-phosphaadamantane), and (mu-pdt)[Fe(CO)(3)][Fe(CO)(2)PTA], 1-PTA, were synthesized and fully characterized. For comparison to the hydrophobic (mu-pdt)[Fe(CO)(2)(PMe(3))](2) and [(mu-H)(mu-pdt)[Fe(CO)(2)(PMe(3))](2)](+) analogues, electrochemical responses of 1-PTA(2) and 1-(PTA.H(+))(2) were recorded in acetonitrile and in acetonitrile/water mixtures in the absence and presence of acetic acid. The production of H(2) and the dependence of current on acid concentration indicated that the complexes were solution electrocatalysts that decreased over-voltage for H(+) reduction from HOAc in CH(3)CN by up to 600 mV. The most effective electrocatalyst is the asymmetric 1-PTA species, which promotes H(2) formation from HOAc (pK(a) in CH(3)CN = 22.6) at -1.4 V in CH(3)CN/H(2)O mixtures at the Fe(0)Fe(I) redox level. Functionalization of the PTA ligand via N-protonation or N-methylation, generating (mu-pdt)[Fe(CO)(2)(PTA-H(+))](2), 1-(PTA.H(+))(2), and (mu-pdt)[Fe(CO)(2)(PTA-CH(3)(+))](2), 1-(PTA-Me(+))(2), provided no obvious advantages for the electrocatalysis because in both cases the parent complex is reclaimed during one cycle under the electrochemical conditions and H(2) production catalysis develops from the neutral species. The order of proton/electron addition to the catalyst, i.e., the electrochemical mechanism, is dependent on the extent of P-donor ligand substitution and on the acid strength. Cyclic voltammetric curve-crossing phenomena was observed and analyzed in terms of the possible presence of an eta(2)-H(2)-Fe(II)Fe(I) species, derived from reduction of the Fe(I)Fe(I) parent complex to Fe(0)Fe(I) followed by uptake of two protons in an ECCE mechanism.
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                Author and article information

                Contributors
                Journal
                Journal ID (publisher-id): CHCOFS
                Title: Chemical Communications
                Abbreviated Title: Chem. Commun.
                Publisher: Royal Society of Chemistry (RSC)
                ISSN (Print): 1359-7345
                ISSN (Electronic): 1364-548X
                Publication date Created: April 21 2022
                Publication date (Electronic): 2022
                Volume: 58
                Issue: 33
                Pages: 5128-5131
                Affiliations
                [1 ]State Key Laboratory of Environment-Friendly Energy Materials, School of Materials Science and Engineering, Southwest University of Science and Technology, Mianyang 621010, P. R. China
                [2 ]College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan 250014, P. R. China
                [3 ]State Key Laboratory of Fine Chemicals, Dalian University of Technology, Dalian 116024, P. R. China
                Article
                DOI: 10.1039/D2CC00757F
                SO-VID: c5a83274-e15f-4200-aa34-d53bbc79e5a9
                Copyright © © 2022
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