Abstract
Photoabsorption, charge separation efficiency and surface reactive catalytic sites are three critical factors in semiconductor photocatalytic process, which determine the photocatalytic activity. For bulk g-C3N4 derived from direct pyrolysis of C/N rich precursors, reactive sites distributed on the lateral edges are very scarce. In this work, we report the template-free preparation of three novel structured g-C3N4, namely, porous tubular (PT) g-C3N4, porous tubular yolk-shell (PTYS) g-C3N4, and porous split yolk-shell (PSYS) g-C3N4, by an unprecedented precursor microstructure regulation of melamine crystals in a gas-pressure mediated re-crystallization process. Enhanced photoabsorption, increased surface area, largely improved separation and migration efficiencies of photoinduced charge carriers are simultaneously realized in these g-C3N4 structures. Noticeably, selective photo-deposition test uncovers that the porous outer-walls and inner-rods of PTYS g-C3N4 are enriched by abundant reductive reactive sites, which consumedly boost the photo-reduction activity. Collectively promoted by these advantages, PTYS g-C3N4 shows not only an efficient H2 production activity with a high apparent quantum efficiency (AQE) of 11.8% at λ = 420 ± 15 nm, but also a superior CO2 reduction for CO production than bulk g-C3N4 by a factor 5.6, which is verified by the 13C isotopic labeling. This work develops precursor microstructure engineering as a promising strategy for rational design of unordinary g-C3N4 structure for renewable energy production.
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