Syngas, a CO and H2 mixture mostly generated from non-renewable fossil fuels, is an essential feedstock for production of liquid fuels. Electrochemical reduction of CO2 and H+/H2O is an alternative renewable route to produce syngas. Here we introduce the concept of coupling a hydrogen evolution reaction (HER) catalyst with a CDots/C3N4 composite (a CO2 reduction catalyst) to achieve a cheap, stable, selective and efficient route for tunable syngas production. Co3O4, MoS2, Au and Pt serve as the HER component. The Co3O4-CDots-C3N4 electrocatalyst is found to be the most efficient among the combinations studied. The H2/CO ratio of the produced syngas is tunable from 0.07:1 to 4:1 by controlling the potential. This catalyst is highly stable for syngas generation (over 100 h) with no other products besides CO and H2. Insight into the mechanisms balancing between CO2 reduction and H2 evolution when applying the HER-CDots-C3N4 catalyst concept is provided.
23 August 2017 in Journal of Materials Chemistry A
Photocatalytic overall water splitting using particulate semiconductors is a potential means of storing solar energy in using the intermittency of sunlight as a primary source of power and zero emission of carbon dioxide. Herein, we constructed a composite material with carbon dots (CDs) anchored on the surface of octahedral CoO as a highly efficient and long-term stable photocatalyst for overall water splitting under visible light irradiation (λ > 400 nm). The structure and morphology of the CDs/CoO composite were investigated by a series of characterization methods. The obtained CDs/CoO composites exhibit more-efficient visible light absorption than pure CoO, leading to higher photocatalytic activity for overall water splitting. The optimized photocatalytic H2 and O2 production was achieved for the CDs/CoO composite with a content of 5 wt% CDs (5% CDs/CoO), showing a H2 (O2) evolution rate of 1.67 μmol h−1 (0.91 μmol h−1) with an expected 2 : 1 stoichiometry, which is up to 6 times as high as that of pristine CoO. Additionally, the 5% CDs/CoO composite also shows outstanding photocatalytic stability for over 15 cycling experiments. This enhanced photocatalytic activity and outstanding stability in CDs/CoO composites could be ascribed to several merits of CDs that not only improved charge separation efficiency and visible-light absorption but also effectively conducted heat generated by the photo-thermal effect of CoO.