Precise tuning of photoinduced charge separation and transport has been an enduringly central issue in photocatalysis but meets with limited success. In particular, controllable, accurate and simultaneous modulation on the...
Crafting spatially controllable charge transfer channels at the nanoscale level remains an enduring challenge in solar-to-chemical conversion technology. Despite the advancements, it still suffers from sluggish interfacial charge transport kinetics and scarcity of strategies to finely modulate charge transport pathways. Herein, this article demonstrates the unexpected charge modulation property of non-conjugated insulating polymer assisted by a universal layer-by-layer self-assembly tactic. Oppositely charged poly(dimethyl diallyl ammonium chloride) (PDDA) and Ti 3 C 2 MXene quantum dots (MQDs) are periodically attached to the wide bandgap metal oxides (WMOs) to design multilayered heterostructured photoanodes. The intermediate PDDA layer acts as an efficacious charge relay medium to access directional electron flow from WMOs to Ti 3 C 2 MQDs, while Ti 3 C 2 MQDs serve as the electron extractor. Charge transfer cascade is thus stimulated on account of the simultaneous electron-trapping capabilities of interim PDDA layer and Ti 3 C 2 MQDs, which synergistically favors the conspicuously boosted charge separation over WMOs, affording the WMOs/(PDDA/MQDs) n photoanodes with considerably enhanced photoelectrochemical (PEC) water oxidation performances. Moreover, PEC performances of such photoanodes can be tuned by interface configuration via assembly number and sequence. This work will provide an insightful perspective to craft a directional charge transfer pathway through insulating polymer for solar energy conversion.
CO2 reduction to carbon feedstocks using heterogeneous photocatalysis technique has been deemed as an attractive means of addressing both deteriorating greenhouse effect and depletion of fossil fuels. Nevertheless, deficiency of accessible active sites on the catalyst surface, low CO2 adsorption rate, and short carrier lifetime retard the photocatalytic CO2 conversion into hydrocarbon fuels. In this study, the controllable construction of spatially separated directional charge transport pathways over multilayered heterostructured transition metal chalcogenides (TMCs) based photosystems for high‐performance photocatalytic CO2‐to‐syngas conversion are shown. In this scenario, ultrathin non‐conjugated insulating poly(diallyl‐dimethyl‐ammonium chloride) (PDDA) layer are intercalated in‐between TMCs and layered double hydroxide (LDH) and serve as an efficient electron transfer mediator, whilst LDH functions as a hole‐withdrawing regulator, both of which synergistically foster the spatial vectorial charge migration/separation over TMCs, thus endowing the TMCs/PDDA/LDH heterostructures with significantly boosted visible‐light‐driven photoactivity toward CO2 conversion into syngas. This study can inspire sparkling new ideas to realize fine tuning of charge motion for stimulating solar‐to‐fuel conversion.
Atomically precise metal nanoclusters (NCs) have recently emerged as a pivotal sector of metal nanomaterials due to unique atomic stacking mode, quantum confinement effect and abundant catalytically active sites. In...
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.