Ultrathin origami accordion‐like structure of vacancy‐rich graphitized carbon nitride for enhancing CO₂ photoreduction

Abstract

Retaining the ultrathin structure of two‐dimensional materials is very important for stabilizing their catalytic performances. However, aggregation and restacking are unavoidable, to some extent, due to the van der Waals interlayer interaction of two‐dimensional materials. Here, we address this challenge by preparing an origami accordion structure of ultrathin two‐dimensional graphitized carbon nitride (oa‐C3N4) with rich vacancies. This novel structured oa‐C3N4 shows exceptional photocatalytic activity for the CO2 reduction reaction, which is 8.1 times that of the pristine C3N4. The unique structure not only prevents restacking but also increases light harvesting and the density of vacancy defects, which leads to modification of the electronic structure, regulation of the CO2 adsorption energy, and a decrease in the energy barrier of the carbon dioxide to carboxylic acid intermediate reaction. This study provides a new avenue for the development of stable high‐performance two‐dimensional catalytic materials.

N-heterocyclic carbene-ligated metal complexes and clusters for photocatalytic CO2reduction

“…The gasphase reactions between CO 2 and water vapor offer a new solution to reduce the competitiveness of the proton reduction process, as there is a higher potential barrier for proton reduction in the gas phase (5.39 eV, H 2 O to H 2 ) compared to the liquid phase (1.25 eV, H + to H 2 ). 53,54 Modulating the hydrophilic/hydrophobic nature of the catalyst may largely overcome the low solubility problem and slow diffusion kinetics of CO 2 in the aqueous phase. 55 Moreover, the confined MOF porosity is an ideal platform for the fast mass transport of gas-phase molecules, which is promising to achieve selective CO 2 photoreduction by M-NHC-functionalized MOFs.…”

Optimizing CO2 photoreduction on bismuth oxyhalides via intrinsic and extrinsic techniques

“…via photocatalytic CO 2 reduction (PCR) is one of the realistic solutions, 2,4–8 PCR suffers from thermodynamic challenges and has inadequate conversion efficiency. 1,5,9–12 To cope with this, numerous photocatalysts have been designed and developed in recent years, 13–24 and among those, bismuth oxyhalides (BiOX; X = Cl, Br, I) are a special family of layered semiconducting materials that have gained tremendous attention because of their unique physicochemical/optoelectronic properties and cost-effectiveness. 25–31 Particularly, the redox potential adjustability, distinct inherent internal electric field (IEF), defect tolerability, and tunable atomic-lattice-derived electronic structure make BiOX promising for PCR.…”

Cobalt-based Polymerized Porphyrinic Network for Visible-light-driven CO2 Reduction

“…Over the past few decades, significant research has been conducted on various porous organic structures, including metal–organic frameworks (MOFs), covalent organic frameworks (COFs), and porous organic polymers (POPs). − Porous organic polymers (POPs) are recognized as promising materials in catalysis owing to their interconnected organic bonds characterized by exceptional chemical stability and porous structures. The diverse array of organic bonds and organic groups present in POFs facilitates the facile regulation of their structures. − These inherent advantages render them versatile for the reduction of CO 2 .…”