Abstract
Photosynthesis is the model system for energy conversion. It uses CO2 as a starting reactant to convert solar energy into chemical energy, i.e., organic molecules or biomass. The first and rate-determining step of this cycle is the immobilization and activation of CO2, catalyzed by RuBisCO enzyme, the most abundant protein on earth. Here, we propose a strategy to develop novel biomimetic two-dimensional (2D) nanostructures for CO2 adsorption at room temperature by reductionist mimicking of the Mg–carboxylate RuBisCO active site. We present a method to synthesize a 2D surface-supported system based on Mg2+ centers stabilized by a carboxylate environment and track their structural dynamics and reactivity under either CO2 or O2 exposure at room temperature. The CO2 molecules adsorb temporarily on the Mg2+ centers, producing a charge imbalance that catalyzes a phase transition into a different configuration, whereas O2 adsorbs on the Mg2+ center, giving rise to a distortion in the metal–organic bonds that eventually leads to the collapse of the structure. The combination of bioinspired synthesis and surface reactivity studies demonstrated here for Mg-based 2D ionic networks holds promise for the development of new catalysts that can work at room temperature.
Highlights
For almost 3 billion years, nature has developed fantastic methods to convert solar energy to fuels in a way that humans are trying to replicate
The CO2 molecules adsorb temporarily on the Mg2+ centers, producing a charge imbalance that catalyzes a phase transition into a different configuration, whereas O2 adsorbs on the Mg2+ center, giving rise to a distortion in the metal−organic bonds that eventually leads to the collapse of the structure
Inspired by the structure of the active site of RuBisCO, we have presented a method to synthesize a system based on a Mg2+ center stabilized by a carboxylate environment
Summary
For almost 3 billion years, nature has developed fantastic methods to convert solar energy to fuels in a way that humans are trying to replicate This process is called photosynthesis,[1] which occurs in two steps: the light reactions (which require light) and carbon fixation ( known as the dark reaction or Calvin cycle). There exists only a single conversion technology with prospects for long-term large-scale use: photovoltaics.[2,3] In a photovoltaic cell, photons are absorbed and converted to electrical energy (light reaction). This leads to electric currents that have to be used immediately. Pursuing the long-term goal of direct fuel production from solar energy requires mimicking the other part of photosynthesis, conversion of CO2 (dark reaction)
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