Abstract
AbstractA sunlight‐powered process is reported that employs carbon dots (CDs) as light absorbers for the conversion of lignocellulose into sustainable H2 fuel and organics. This photocatalytic system operates in pure and untreated sea water at benign pH (2–8) and ambient temperature and pressure. The CDs can be produced in a scalable synthesis directly from biomass itself and their solubility allows for good interactions with the insoluble biomass substrates. They also display excellent photophysical properties with a high fraction of long‐lived charge carriers and the availability of a reductive and an oxidative quenching pathway. The presented CD‐based biomass photoconversion system opens new avenues for sustainable, practical, and renewable fuel production through biomass valorization.
Highlights
Photocatalysis allows for the utilization of solar energy to produce renewable H2, but most reported systems still require preciousmetal components, purified water or an expensive sacrificial electron donor (ED).[1]
The non-toxic, biocompatible carbon dots (CDs) are employed as light absorbers, together with a Ni bis(diphosphine) H2 evolution cocatalyst (NiP,[12] Figure S2), to produce H2 and organics in purified and untreated water (Figure 1b) under benign conditions
The α-cel-CD/NiP system provides a benchmark activity of 13,450 μmol H2–1 h–1 (Figure S3), which is the highest reported so far for carbonaceous photoabsorbers using comparable conditions (Table S5).[10-11, 14]
Summary
Photocatalysis allows for the utilization of solar energy to produce renewable H2, but most reported systems still require preciousmetal components, purified water or an expensive sacrificial electron donor (ED).[1]. PR of α-cellulose and xylan produced 5.0±0.2 and 3.6±0.3 μmol H2, respectively, similar to a heterogeneous CNx/NiP system.[8a] in contrast to heterogeneous systems that show substrate-dependent H2 yields, homogeneous CDs photoreform soluble and insoluble biomass with a similar efficiency.
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