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Manganese plays multiple role in many biological redox reactions in which it exists in different oxidation states from Mn(II) to Mn(IV). Among them the high-valent manganese-oxo intermediate plays important role in the activity of certain enzymes and lessons from the natural system provide inspiration for new developments of artificial systems for a sustainable energy supply and various organic conversions. This review describes recent advances and key lessons learned from the nature on high-valent Mn-oxo intermediates. Also we focus on the elemental science developed from the natural system, how the novel strategies are realised in nano particles and molecular sites at heterogeneous and homogeneous reaction conditions respectively. Finally, perspectives on the utilisation of the high-valent manganese-oxo species towards other organic reactions are proposed.
A model has been developed based on Colburn–Drew type formulation to analyze a vertical tube in tube stainless steel generator with forced convective boiling. Desorption of refrigerant vapor from refrigerant–absorbent solution takes place in the inner tube of the generator, when hot water through the annulus is used as heating medium. Simultaneous heat and mass transfer phenomena of desorption are described mathematically using the mass and energy balances, considering the heat and mass transfer resistances in liquid as well as vapor phases. Model equations are solved simultaneously by means of initial value problem solvers using explicit Runge–Kutta method with 4th order accuracy. A computer code has been developed in MATLAB to obtain the results. A parametric analysis has also been performed to study the effect of various parameters on the performance of the generator.
Jeong, Hui-Yun,Balamurugan, Mani,Choutipalli, Venkata Surya Kumar,Jeong, Eun-suk,Subramanian, Venkatesan,Sim, Uk,Nam, Ki Tae The Royal Society of Chemistry 2019 Journal of Materials Chemistry A Vol.7 No.17
<P>The electrochemical reduction of carbon dioxide (CO2) to value-added products is a promising approach to reduce excess CO2 in the atmosphere. However, the selective reduction of CO2 in aqueous electrolytes has been challenging owing to a competing hydrogen evolution reaction occurring in aqueous electrolytes. In this study, single atom nickel and nitrogen doped three-dimensional porous carbon catalysts are developed for the selective production of carbon monoxide (CO) from CO2. The catalysts exhibit high CO selectivity with over 99% faradaic efficiency at −0.8 V <I>vs.</I> the reversible hydrogen electrode (RHE), and achieve a high current density of over 50 mA cm<SUP>−2</SUP> at −1.0 V <I>vs.</I> RHE in a bicarbonate electrolyte. To further improve the CO2 reduction rate, the accessibility of CO2 to the catalysts was enhanced by directly supplying gaseous CO2 to the surface of the catalysts. The catalysts were deposited between a gas diffusion layer and an ion exchange membrane to form a membrane electrode assembly (MEA). Benefiting from the high concentration of CO2 over the catalyst surfaces and the three-dimensional structure of the catalysts, a high CO production rate exceeding 300 mA cm<SUP>−2</SUP> with 99% faradaic efficiency can be achieved.</P>
Jin, Kyoungsuk,Seo, Hongmin,Hayashi, Toru,Balamurugan, Mani,Jeong, Donghyuk,Go, Yoo Kyung,Hong, Jung Sug,Cho, Kang Hee,Kakizaki, Hirotaka,Bonnet-Mercier, Nadè,ge,Kim, Min Gyu,Kim, Sun Hee,Nakamu American Chemical Society 2017 JOURNAL OF THE AMERICAN CHEMICAL SOCIETY - Vol.139 No.6
<P>The development of active water oxidation catalysts is critical to achieve high efficiency in overall water splitting. Recently, sub 10 nm-sized monodispersed partially oxidized manganese oxide nanoparticles were shown to exhibit not only superior catalytic performance for oxygen evolution, but also unique electrokinetics, as compared to their bulk counterparts. In the present work, the water oxidizing mechanism of partially oxidized MnO nanoparticles was investigated using integrated in situ spectroscopic and electrokinetic analyses. We successfully demonstrated that, in contrast to previously reported manganese (Mn)-based catalysts, Mn(III) species are stably generated on the, surface of MnO nanoparticles via a proton-coupled electron transfer pathway. Furthermore, we confirmed as to MnO nanoparticles that the one-electron oxidation step from Mn(II) to Mn(III) is no longer the rate-determining step for water oxidation and that Mn(W)=O species are generated as reaction intermediates during catalysis.</P>