The ability to efficiently reduce CO2 to dense hydrocarbon fuels would revolutionize the global economy and climate. Photosynthetic CO2 reduction, in particular, has been a grand challenge of the Department of Energy and global scientific community due to its potential positive impact on humanity.
To date, two strategies for large-scale synthetic CO2 reduction have been pursued, namely (a) metal-based inorganic catalysts,82 or (b) bioengineering of photosynthetic organisms.83 Photosynthetic CO2 reduction is a challenging catalytic problem that has remained inefficient in laboratory settings. Light-driven reactions taking CO2 to reduced hydrocarbons involve the localization of multiple electrons of specific energies generated from photo-excitation – a process that is inherently difficult to control. Our work developing high-performance methods for accurate atomic simulation will enable a computationally-guided iterative design process to address this challenge for both inorganic and biological photocatalyst design, which can be directly employed for CO2 reduction.