Efficient Electrocatalytic Upgradation of Furan-Based
Biomass: Key Roles of a Two-Dimensional Mesoporous Poly(m‑phenylenediamine)-Graphene Heterostructure and a Ternary
Electrolyte
posted on 2022-02-11, 21:29authored byHaoran Wu, Yashi Zou, Haishan Xu, Liang Wu, Yiyong Mai
The
development of electrocatalytic systems for efficient biomass
conversion under mild conditions and understanding their mechanisms
are of profound significance but remain challenging. Here, we report
the development of a two-dimensional polymer-based mesoporous electrocatalyst
(meso-PA/PmPD/GO) for biomass conversion, which comprises phytic acid
(PA)-doped mesoporous poly(m-phenylenediamine) layers
coated on graphene oxide. Meanwhile, a ternary electrolyte containing
1-butyl-3-methylimidazolium tetrafluoroborate (BmimBF4),
acetonitrile, and H2O is selected. The combination of meso-PA/PmPD/GO
and the electrolyte realizes efficient conversion of two important
biomass derivatives. One involves the oxidation of furfuryl alcohol
to 6-hydroxy-2,3-dihydro-6H-pyrano-3-one with high
faradic efficiency (FE: 82.2%) and selectivity (86.1%). The other
involves the oxidation of furfural to 5-hydroxy-2(5H)-furanone with record-high FE (98.2%) and selectivity (93.1%). A
mechanistic study unveils that N-heterocyclic carbenes
(Bmim*) generated from BmimBF4 act as the reaction-determining
species. The synergistic effect of the PA doping and mesoporous polymeric
structure in meso-PA/PmPD/GO favors mass transport and electron–hole
separation/transfer to the reactants, thus boosting catalytic performance.