Abstract

Biomass electrocatalytic-conversion coupled with hydrogen generation exhibits low energy consumption, efficient hydrogen production and green syntheses of value-added chemicals. However, constructing electrocatalysts with precise electronic modulation and structures for efficient biomass electrocatalytic conversion coupled hydrogen production remains challenging. Herein, a bacterial cellulose substrate was combined in situ with a Mn-doped NiFe Prussian blue analogue (PBA) precursor, and one-step carbonization-phosphorylation was developed for the preparation of Mn-doped nickel iron phosphate (MNFP) embedded in a P, N codoped carbon (PNC) substrate grown directly on P-doped carbonized bacterial cellulose (MNFP-PNC/PCBC). Benefiting from the three-dimensional network structure of P-doped carbonized bacterial cellulose (PCBC) and atomic doping, MNFP-PNC/PCBC exhibited an optimized electronic structure, abundant active sites and excellent electrical conductivity. Therefore, the voltages required with hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and glucose electrocatalytic-conversion (GCR) to drive a current density of 50 mA cm−2 were 0.214, 1.5, and 1.34 V, respectively. Moreover, the required cell voltage of the novel electrolyser containing MNFP-PNC/PCBC as electrodes can be further reduced to 1.55 V at 50 mA cm−2 compared to overall water splitting, resulting in more than 8-time improvement in hydrogen production efficiency and production of value-added formate. This work provides a unique approach for electrocatalytic-conversion of biomass coupled with electrocatalytic hydrogen generation.

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