2020
DOI: 10.1021/acscatal.0c02315
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Demonstrating the Direct Relationship between Hydrogen Evolution Reaction and Catalyst Deactivation in Synthetic Fe Nitrogenases

Abstract: Synthetic Fe nitrogenases are promising catalysts for atmospheric pressure ammonia synthesis. However, their catalytic efficiency is severely limited by the accompanying hydrogen evolution reaction (HER) and fast catalyst deactivation. In order to reveal the origin of these undesired transformations, we study potential reaction routes of HER, catalyst deactivation, and nitrogen reduction reaction (N2RR) by density functional theory in combination with microkinetic modeling, using a triphosphino-silyl ligated i… Show more

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Cited by 18 publications
(30 citation statements)
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“…Similar to our previous DFT studies on nitrogenases, ,, we performed the geometry optimization at the BP86/def2-SVP level of theory. The RI density fitting approximation was applied with the def2/J auxiliary basis set . To take relativistic effects and dispersion interactions into account, the zeroth-order relativistic approximation (ZORA) , and Grimme’s Becke–Johnson damped dispersion correction (D3­(BJ)) , were used in all calculations.…”
Section: Computational Detailsmentioning
confidence: 99%
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“…Similar to our previous DFT studies on nitrogenases, ,, we performed the geometry optimization at the BP86/def2-SVP level of theory. The RI density fitting approximation was applied with the def2/J auxiliary basis set . To take relativistic effects and dispersion interactions into account, the zeroth-order relativistic approximation (ZORA) , and Grimme’s Becke–Johnson damped dispersion correction (D3­(BJ)) , were used in all calculations.…”
Section: Computational Detailsmentioning
confidence: 99%
“…The selection of conformation and spin state of EP 3 Fe–N 2 , EP 3 Fe–H 2 , and EP 3 Fe complexes was based on recent experimental and computational studies. ,, …”
Section: Computational Detailsmentioning
confidence: 99%
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“…Such an analysis is difficult to achieve experimentally, as only macroscopic quantities (such as the time course of adduct formation) can be determined in this way; moreover, precise measurements can only be performed on simplified model systems [9,19,25] where the reaction conditions (e.g., pH, distribution of protonated/deprotonated species, reactant concentrations) might significantly deviate from those peculiar to an actual breast cell nucleus. Computational chemistry, on the contrary, enables the detailed examination of any reaction sequence at the level of elementary steps, which has been proven to be especially useful in studying complex reaction mechanisms [26][27][28][29], including biochemical transformations [30,31].…”
Section: Introductionmentioning
confidence: 99%