Carbon catalysts with metal and nitrogen
dopants hold significant
promises for an electrochemical CO2 reduction reaction
(CO2RR). However, the fabrication of these carbon catalysts
normally requires an energy-intensive synthesis process. Traditionally,
2D graphene and 1D carbon nanotubes (CNTs) are the most widely used
carbon supports, but graphene tends to aggregate and CNTs suffer from
low density of active sites on the surface. In this work, we developed
a 3D hybrid carbon nanosheet/nanotube catalyst with nickel (Ni) and
nitrogen (N) co-doped active sites for the CO2RR by a one-step
chemical vapor deposition (CVD) method. Both single atomic sites and
nanoparticles of Ni were observed on the hybrids, but the Ni nanoparticles
were encapsulated by graphitic carbon layers during the CVD process,
and as a result, the competing hydrogen evolution reaction was suppressed
and high CO selectivity was achieved. The as-prepared catalyst with
20 min CVD delivered a stable CO Faradaic efficiency of 91% with a
partial current density of 28.9 mA/cm2 at −0.74
V in an H-cell setup. The same catalyst achieved a commercially viable
current density of 600 mA/cm2 in a flow cell with CO selectivity
above 85%, at an applied voltage of −2.0 V vs reversible hydrogen
electrode without iR compensation. To the best of our knowledge, these
results are among the best performances in the literature in terms
of both current density and CO selectivity for the CO2RR
by carbon-based catalysts. Furthermore, catalysts developed in this
work are synthesized at a moderate temperature without any acid/oxidant
pretreatment or post-washing. The energy-efficient and environmentally
benign synthesis and the significantly high performance of catalysts
are essential to future large-scale CO2RR applications.