DESIGNING RATIONAL SCHEMES FOR SOLAR FUEL AND METHANE OXIDIZING CATALYSTS
PRODUCTION OF CARBON-NEUTRAL ENERGY SOURCES IS THE MOST URGENT SCIENTIFIC CHALLENGE DUE TO THE RAPID DEPLETION OF FOSSIL FUELS, CLEAN ENERGY CAN BE PRODUCTED THROUGH FUEL-FORMING REACTIONS BY NATURAL PHOTOSYNTHESIS SUCH AS THE LIG...
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Descripción del proyecto
PRODUCTION OF CARBON-NEUTRAL ENERGY SOURCES IS THE MOST URGENT SCIENTIFIC CHALLENGE DUE TO THE RAPID DEPLETION OF FOSSIL FUELS, CLEAN ENERGY CAN BE PRODUCTED THROUGH FUEL-FORMING REACTIONS BY NATURAL PHOTOSYNTHESIS SUCH AS THE LIGHT-INDUCED SPLITTING OF WATER INTO HYDROGEN AND OXYGEN, OR METHANE MONOOXYGENASE ENZYMES (MMO) THROUGH THE AMBIENT OXIDATION OF METHANE TO METHANOL, IN SPITE OF ACTIVE EFFORTS IN CHARACTERIZING ARTIFICIAL PHOTOSYNTHETIC ASSEMBLIES AND MMO ENZYMES, THERE IS A PRESSING NEED TO CORRELATE THE STRUCTURE AND ACTIVITY OF A CATALYST TO ITS STABILITY AND PERFORMANCE, FURTHER, THE NATURE OF THE HIGH VALENT FEIV SPECIES RESPONSIBLE FOR BREAKING THE C-H BOND IN MMO ENZYMES IS STILL UNKNOWN,THE PROPOSED CATDESIGN ERC GRANT FOCUSES ON THE DEVELOPMENT AND APPLICATION OF ADVANCED SPECTROSCOPIC TOOLS NAMELY X-RAY ABSORPTION (XAS), EMISSION (XES), AND VALENCE TO CORE XES TO DELIVER IN-SITU INFORMATION ON THE SITE SYMMETRY, NUCLEAR CHARGE, AND METAL-TO-LIGAND BOND STRENGTH OF EARTH-ABUNDANT CATALYTIC MOLECULES, CORRELATIONS DRAWN BETWEEN THE GEOMETRIC CONFIGURATION OF A CATALYSTS LIGAND TO ITS ELECTRON DENSITY, AND REDOX POTENTIALS WILL OUTLINE A WELL-DEFINED RECIPE FOR THE DESIGNS OF ROBUST CATALYSTS WITH LOW REACTION BARRIERS, AND ABILITY TO PERFORM UNDER A WIDE RANGE OF CONDITIONS ON ELECTRODE SURFACES, XAS AND XES WILL FURTHER BE EXTENDED TO THE TIME REGIME THROUGH STOPPED-FLOW APPROACHES TO ELUCIDATE THE STRUCTURE OF THE FE(IV) SPECIES IN MMO ENZYMES, LASTLY, TIME-RESOLVED PUMP LASER AND PROBE X-RAY APPROACHES IN HOMOGENEOUS AND SURFACE-ANCHORED MODULES OF ARTIFICIAL MMO ASSEMBLIES WILL IDENTIFY TRANSIENT REACTIVE INTERMEDIATES, AND RATE LIMITING STEPS LEADING TO METHANOL FORMATION WITH FEMTO-PICO TIME RESOLUTION, PROPOSED X-RAY APPROACHES WILL BE COMPLEMENTED WITH ELECTRON PARAMAGNETIC RESONANCE AND RAMAN SPECTROSCOPY TO VALIDATE THE SPIN DENSITY, AND VIBRATIONAL CHANGES, EXPECTED RESULTS WILL LEAD TO OPTIMIZED FUNCTIONAL CATALYSTS FOR PRACTICAL HYBRID DEVICES, ARTIFICIAL PHOTOSYNTHESIS\METHANE TO METHANOL OXIDATION\SYNCHROTRON-BASED X-RAY ABSORPTION AND E\ULTRAFAST TIME-RESOLVED SPECTROSCOPY\ELECTROCHEMISTRY\UV-VISIBLE SPECTROSCOPY\ELECTRON PARAMAGNETIC RESONANCE\RAMAN
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