Natural polymer/wide-bandgap inorganic hybrids for visible-light-driven CO2 photoreduction: Unraveling the multiple effects of interfacial chemical bonding.

[Display omitted] • Novel CNC#BOC hybrid was constructed via an innovative interfacial bonding tactic. • CNC#BOC shows high activity for selective CO 2 photoreduction under blue LED light. • Interfacial bonding promotes light harvesting, OV stability, and electron transfer. • Both DFT and experimental studies verify the multiple roles of interfacial bonding. • This work broadens the potential applications of renewable biomass nanocomposites. Biomass-derived nanocomposites represent a developing class of multifunctional materials with biomimetic implications. Here, cellulose nanocrystal interfacially bonded Bi 2 O 2 CO 3 hybrids (CNC#BOC) were fabricated via a hydrothermal approach for visible-light CO 2 photoreduction. The as-synthesized CNC#BOC demonstrated superb photocatalytic activity with a CO production rate of 15.22 μmol g-1 h−1, a selectivity of ∼ 97 %, and excellent cycling stability. Theoretical calculations and experimental studies indicated the existence of covalent bonds between the BOC and CNC, resulting in LMCT photosensitization, a narrowed bandgap energy, plentiful and stable OVs, high reactants affinity, fast electron transfer channels, and facile formation of *COOH intermediate. This study introduces a novel covalent bonding tactic for developing natural polymer-based catalysts for selective CO 2 photoreduction, which is expected to broaden the applications of environmentally friendly biomass composites. [ABSTRACT FROM AUTHOR]