TY - JOUR
T1 - Photo-recycling the Sacrificial Electron Donor
T2 - Towards Sustainable Hydrogen Evolution in a Biphasic System
AU - Ge, Peiyu
AU - Hojeij, Mohamad
AU - Scanlon, Micheál D.
AU - Girault, Hubert H.
N1 - Publisher Copyright:
© 2020 Wiley-VCH GmbH
PY - 2020/12/14
Y1 - 2020/12/14
N2 - H2 may be evolved biphasically using a polarised liquid|liquid interface, acting as a “proton pump”, in combination with organic soluble metallocenes as electron donors. Sustainable H2 production requires methodologies to recycle the oxidised donor. Herein, the photo-recycling of decamethylferrocenium cations (DcMFc+) using aqueous core-shell semiconductor CdSe@CdS nanoparticles is presented. Negative polarisation of the liquid|liquid interface is required to extract DcMFc+ to the aqueous phase. This facilitates the efficient capture of electrons by DcMFc+ on the surface of the photo-excited CdSe@CdS nanoparticles, with hydrophobic DcMFc subsequently partitioning back to the organic phase and resetting the system. TiO2 (P25) and CdSe semiconductor nanoparticles failed to recycle DcMFc+ due to their lower conduction band energy levels. During photo-recycling, CdS (on CdSe) may be self-oxidised and photo-corrode, instead of water acting as the hole scavenger.
AB - H2 may be evolved biphasically using a polarised liquid|liquid interface, acting as a “proton pump”, in combination with organic soluble metallocenes as electron donors. Sustainable H2 production requires methodologies to recycle the oxidised donor. Herein, the photo-recycling of decamethylferrocenium cations (DcMFc+) using aqueous core-shell semiconductor CdSe@CdS nanoparticles is presented. Negative polarisation of the liquid|liquid interface is required to extract DcMFc+ to the aqueous phase. This facilitates the efficient capture of electrons by DcMFc+ on the surface of the photo-excited CdSe@CdS nanoparticles, with hydrophobic DcMFc subsequently partitioning back to the organic phase and resetting the system. TiO2 (P25) and CdSe semiconductor nanoparticles failed to recycle DcMFc+ due to their lower conduction band energy levels. During photo-recycling, CdS (on CdSe) may be self-oxidised and photo-corrode, instead of water acting as the hole scavenger.
KW - CdSe@CdS nanoparticles
KW - hydrogen evolution reaction
KW - liquid-liquid interfaces
KW - metallocenes
KW - nanoparticles
KW - sacrificial electron donor
UR - http://www.scopus.com/inward/record.url?scp=85096656378&partnerID=8YFLogxK
U2 - 10.1002/cphc.202000844
DO - 10.1002/cphc.202000844
M3 - Article
C2 - 33166015
AN - SCOPUS:85096656378
SN - 1439-4235
VL - 21
SP - 2630
EP - 2633
JO - ChemPhysChem
JF - ChemPhysChem
IS - 24
ER -
