Ordered Macroporous Carbonous Frameworks Implanted with CdS Quantum Dots for Efficient Photocatalytic CO₂ Reduction

Abstract

Solar‐driven photocatalytic CO2 reduction is regarded as a promising way to simultaneously mitigate the energy crisis and CO2 pollution. However, achieving high efficiency of photocatalytic CO2 reduction, especially without the assistance of sacrifice reagents or extra alkaline additives, remains a critical issue. Herein, a photocatalyst of 3D ordered macroporous N‐doped carbon (NC) supported CdS quantum dots (3DOM CdSQD/NC) is successfully fabricated toward photocatalytic CO2 reduction via an in situ transformation strategy. Additionally, an amines oxidation reaction is introduced to replace the H2O oxidation process to further boost the photocatalytic CO2 reduction efficiency. Impressively, 3DOM CdSQD/NC exhibits superior activity and selectivity in photocatalytic CO2 reduction coupled with amines oxidation, affording a CO production rate as high as 5210 µmol g−1 h−1 in the absence of any sacrificial agents and alkaline additives. Moreover, 3DOM CdSQD/NC achieves an apparent quantum efficiency of 2.9% at 450 nm. Mechanism studies indicate that the 3D ordered macropores in the NC matrix are beneficial to the transfer of photogenerated carriers. Furthermore, the highly dispersed CdS QDs on the NC skeleton are able to significantly promote the adsorption of both CO2 and amine molecules and depress the CO2 activation energy barriers by stabilizing the *COOH intermediate, directly contributing to the high activity.

Replacing Ru complex with carbon dots over MOF-derived Co3O4/In2O3 catalyst for efficient solar-driven CO2 reduction

“…The pure M-In 2 O 3 presents a strong emission peak at 455 nm, exhibiting severe electron–hole recombination. 51 The emission peak of M-Co 3 O 4 /In 2 O 3 is much lower than that of M-In 2 O 3 , indicating suppressed radiative recombination in the heterostructure. After coupling with CDs, the obviously decreased PL intensity of CDs-M-CIO can be observed, due to the remarkably improved charge transfer efficiency.…”

Confining single Pt atoms from Pt clusters on multi-armed CdS for enhanced photocatalytic hydrogen evolution

“…Among these bottlenecks, the narrow spectral response range, low separation efficiency of photogenerated carriers and insufficient redox active sites are still the main factors that hinder the improvement of photocatalytic efficiency. 3 To solve these problems, many strategies have been proposed, including the construction of heterojunctions, doping effects, plasma effects, and the utilization of co-catalysts. 4…”

Ordered carbonaceous frameworks: a new class of carbon materials with molecular-level design

“…At an early stage, silica gel was used as a hard template to obtain amorphous porous carbon materials in 1982, 8 and since then, a wide variety of threedimensional (3D) ordered porous carbons have been synthesized using oxide templates such as zeolites, [9][10][11][12][13][14][15] mesoporous silicas, 16,17 and silica opals. 18,19 The resulting materials with structural ordering are known as ordered porous carbons and include ''ordered microporous carbons'', ''ordered mesoporous carbons'', and ''ordered macroporous carbons''. More recently, the hard-template method has been expanded to the synthesis of graphene-based 3D nanoporous materials using Ni-foam, 20 Al 2 O 3 and MgO nanoparticles.…”