Contemporary carbon
and hydrogen production processes release significant
CO2 emissions with negative consequences for the Earth’s
climate. Here we report a process in which concentrated irradiation
from a simulated solar source converts methane to high-value graphitic
carbon and hydrogen gas. Methane flows within a photothermal reactor
through pores of a thin substrate, with the process reaching steady-state
conditions from room temperature within the first minute of irradiation
by several thousand suns. Methane decomposes primarily into hydrogen
while depositing highly graphitic carbon that grows conformally over
ligaments in the substrate. The localized solar heating serves to
capture solid carbon into a readily extractable form while maintaining
active deposition site density with persistent catalytic activity
until the ligaments coalesce to block the flow. Even with a large
flow area through regions of lower irradiation and temperature, methane
conversions and hydrogen yields of approximately 70% are achieved,
and 58% of the inlet carbon is fully captured in graphitic form.