@article{Sachs:2018:10.1038/s41467-018-07420-6,
author = {Sachs, M and Sprick, RS and Pearce, D and Hillman, SAJ and Monti, A and Guilbert, AAY and Brownbill, NJ and Dimitrov, S and Shi, X and Blanc, F and Zwijnenburg, MA and Nelson, J and Durrant, JR and Cooper, AI},
doi = {10.1038/s41467-018-07420-6},
journal = {Nature Communications},
title = {Understanding structure-activity relationships in linear polymer photocatalysts for hydrogen evolution},
url = {http://dx.doi.org/10.1038/s41467-018-07420-6},
volume = {9},
year = {2018}
}

Download

TY  - JOUR
AB  - Conjugated polymers have sparked much interest as photocatalysts for hydrogen production. However, beyond basic considerations such as spectral absorption, the factors that dictate their photocatalytic activity are poorly understood. Here we investigate a series of linear conjugated polymers with external quantum efficiencies for hydrogen production between 0.4 and 11.6%. We monitor the generation of the photoactive species from femtoseconds to seconds after light absorption using transient spectroscopy and correlate their yield with the measured photocatalytic activity. Experiments coupled with modeling suggest that the localization of water around the polymer chain due to the incorporation of sulfone groups into an otherwise hydrophobic backbone is crucial for charge generation. Calculations of solution redox potentials and charge transfer free energies demonstrate that electron transfer from the sacrificial donor becomes thermodynamically favored as a result of the more polar local environment, leading to the production of long-lived electrons in these amphiphilic polymers.
AU  - Sachs,M
AU  - Sprick,RS
AU  - Pearce,D
AU  - Hillman,SAJ
AU  - Monti,A
AU  - Guilbert,AAY
AU  - Brownbill,NJ
AU  - Dimitrov,S
AU  - Shi,X
AU  - Blanc,F
AU  - Zwijnenburg,MA
AU  - Nelson,J
AU  - Durrant,JR
AU  - Cooper,AI
DO  - 10.1038/s41467-018-07420-6
PY  - 2018///
SN  - 2041-1723
TI  - Understanding structure-activity relationships in linear polymer photocatalysts for hydrogen evolution
T2  - Nature Communications
UR  - http://dx.doi.org/10.1038/s41467-018-07420-6
UR  - http://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000451047900003&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
UR  - http://hdl.handle.net/10044/1/66649
VL  - 9
ER  - 

Download