Abstract
We discuss a low-cost computational workflow for the high-throughput screening of polymeric photocatalysts and demonstrate its utility by applying it to a number of challenging problems that would be difficult to tackle otherwise. Specifically we show how having access to a low-cost method allows one to screen a vast chemical space, as well as to probe the effects of conformational degrees of freedom and sequence isomerism. Finally, we discuss both the opportunities of computational screening in the search for polymer photocatalysts, as well as the biggest challenges.
Highlights
Starting with the original work from Fujishima and Honda on the photoelectrolysis of water[1] using a TiO2 photoanode, hydrogen evolution and water splitting photocatalysis generally involves the use of an inorganic semiconductor as a photoelectrode or photocatalyst
We recently developed an approach[33] based on semiempirical tight-binding calculations using the (GFN/IPEA/simpli ed Tamm–Dancoff approach (sTDA))-xTB methods,[34,35,36] which, a er a calibration procedure, gives results that are comparable with density functional theory (DFT) at a fraction of the computational cost
Besides successfully demonstrating the utility of our low-cost computational work ow for screening polymer photocatalysts, we demonstrated that conformational degrees of freedom have little in uence on optoelectronic properties of polymers that are pertinent to their photocatalytic activity
Summary
Starting with the original work from Fujishima and Honda on the photoelectrolysis of water[1] using a TiO2 photoanode, hydrogen evolution and water splitting photocatalysis generally involves the use of an inorganic semiconductor as a photoelectrode or photocatalyst. Carbon nitride was the rst polymeric material reported to evolve both hydrogen and oxygen under illumination in the presence of a sacri cial electron/hole donor[4] and was later shown to perform overall water splitting.[5,6,7] Recently, conjugated polymer photoanodes were shown to be able to oxidise water as part of a photoelectrochemical cell.[8]. While a much less mature technology than use of inorganic semiconductors, organic polymer photocatalysts offer some very attractive features. In contrast to their inorganic counterparts, polymeric photocatalysts are generally based on the most abundant of elements, C, H, N, S, O; though some polymers are, for the
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