Isotype Heterojunction-Boosted CO2 Photoreduction to CO

Abstract

Photocatalytic conversion of CO2 to high-value products plays a crucial role in the global pursuit of carbon–neutral economy. Junction photocatalysts, such as the isotype heterojunctions, offer an ideal paradigm to navigate the photocatalytic CO2 reduction reaction (CRR). Herein, we elucidate the behaviors of isotype heterojunctions toward photocatalytic CRR over a representative photocatalyst, g-C3N4. Impressively, the isotype heterojunctions possess a significantly higher efficiency for the spatial separation and transfer of photogenerated carriers than the single components. Along with the intrinsically outstanding stability, the isotype heterojunctions exhibit an exceptional and stable activity toward the CO2 photoreduction to CO. More importantly, by combining quantitative in situ technique with the first-principles modeling, we elucidate that the enhanced photoinduced charge dynamics promotes the production of key intermediates and thus the whole reaction kinetics.

A Comprehensive Review on Graphitic Carbon Nitride for Carbon Dioxide Photoreduction

“…In a similar study Ban et al. [ 645 ] fabricated isotype g‐C 3 N 4 homojunction (ICN) from g‐C 3 N 4 synthesized from melamine (MCN) and thiourea (TCN). The produced material exhibit a remarkable CO yield of 12.09 µmol g −1 h −1 than 3.97 µmol g −1 h −1 for MCN and 3.05 µmol g −1 h −1 for TCN.…”

“…As a result, the photocatalytic CO 2 reduction activity reached 7.75 µmol g −1 h −1 under normal pressure and temperature, which is 16.1 and 13.8 times higher than the TCN and MCN (Figure 48d). In a similar study Ban et al [645] fabricated isotype g-C 3 N 4 homojunction (ICN) from g-C 3 N 4 synthesized from melamine (MCN) and thiourea (TCN). The produced material exhibit a remarkable CO yield of 12.09 µmol g −1 h −1 than 3.97 µmol g −1 h −1 for MCN and 3.05 µmol g −1 h −1 for TCN.…”

Selective CO2 Photoreduction to Acetate at Asymmetric Ternary Bridging Sites

“…The interfacial energy barriers with the high defect state at the interface would adjust the absorbed state of intermediates. Moreover, the interface engineering also increases the number of active sites through the introduction of more interfacial areas. − In CO 2 reduction, the adsorption of adjacent C 1 intermediates across the asymmetric interface provides a feasible way to moderate dipole–dipole repulsion for producing C 2 products.…”

Frustrated Lewis Pairs on In(OH)3–x Facilitate Photocatalytic CO2 Reduction

“…Semiconductor-based photocatalytic reduction of CO 2 into fuels or chemicals is a promising route and has attracted extensive attention. − The challenge lies in the efficient activation of stable CO bonds. − Engineering the photocatalyst via the introduction of surface defects, organic amines, or inorganic bases , has been reported to enhance the adsorption and activation of CO 2 . ,− Recently, frustrated Lewis pairs (FLPs), composed of sterically hindered Lewis acid (LA) and Lewis base (LB), have offered an opportunity for effectively activating CO 2 . − Specifically, the unoccupied orbitals of LA and the nonbonding orbitals of LB interact with the bonding and antibonding orbitals of the trapped molecules, respectively, resulting in an efficient activation. , …”