Intermolecular cascaded π-conjugation channels for electron delivery powering CO2 photoreduction

Abstract

Photoreduction of CO 2 to fuels offers a promising strategy for managing the global carbon balance using renewable solar energy. But the decisive process of oriented photogenerated electron delivery presents a considerable challenge. Here, we report the construction of intermolecular cascaded π-conjugation channels for powering CO 2 photoreduction by modifying both intramolecular and intermolecular conjugation of conjugated polymers (CPs). This coordination of dual conjugation is firstly proved by theoretical calculations and transient spectroscopies, showcasing alkynyl-removed CPs blocking the delocalization of electrons and in turn delivering the localized electrons through the intermolecular cascaded channels to active sites. Therefore, the optimized CPs (N-CP-D) exhibiting CO evolution activity of 2247 μmol g −1 h −1 and revealing a remarkable enhancement of 138-times compared to unmodified CPs (N-CP-A).

Unique S-scheme heterojunctions in self-assembled TiO2/CsPbBr3 hybrids for CO2 photoreduction

“…4d , the total ion chromatographic peak ~3.44 min corresponded to CO, which produced three signals in the mass spectra. The main MS signal at m/z = 29 belonged to 13 CO and the others ( 13 C at m/z = 13 and O at m/z = 16) corresponded to the fragments of 13 CO, confirming that the CO product exactly originated from the CO 2 photoreduction over TiO 2 /CsPbBr 3 38 , 39 . In addition, the total ion chromatographic peaks ~2.36 and 2.48 min can be assigned to the O 2 and N 2 , respectively (Supplementary Fig.…”

Unraveling fundamental active units in carbon nitride for photocatalytic oxidation reactions

“…Semiconductor photocatalysts have emerged with increasing attention for artificial photosynthesis reactions 1 . Despite enormous advances, developing photocatalysts that have high activity and stability, meanwhile without complex synthetic processes and expensive/toxic elements, is still challenging.…”

Zr‐Based Metal‐Organic Framework Films Grown on Bio‐Template for Photoelectrocatalysis

“…UiO-67/B exhibits the highest photoelectrocatalytic HER activity probably because UiO-67/B exhibits the lowest energy bad gap, and the ligand of UiO-67/B with strong conjugate effect is advantageous to the transfer of photo-generated carriers. [69] UiO-66/B and NH 2 -UiO-66/B show similar performance. Due to the presence of the amino group the auxochromic and bathochromic shift introduces an absorption in the wavelength longer than 300 nm.…”

“…Both transient spectra for UiO-66 and NH 2 -UiO-66 are similar with continuous absorption from 300 to beyond 700 nm and relative maxima at 620 and 580 nm for UiO-66 and NH 2 -UiO-66, respectively, and it suggests that they have similar photogenerated transients and particularly similar states of charge separation. [69] It is worth mentioning that the MOF particle size affects the performance. Better HER performance was observed when the UiO-67 nanoparticles were smaller, which were prepared using a gelation method.…”