In Situ Modulation of NiFeOOH Coordination Environment for Enhanced Electrocatalytic‐Conversion of Glucose and Energy‐Efficient Hydrogen Production
Ning Wei, Sufeng Zhang, Xue Yao, Qinglu Li, Nan Li, Jingrui Li, Dingjie Pan, Qiming Liu, Shaowei Chen, Scott Renneckar
Abstract
Abstract Glucose electrocatalytic‐conversion reaction (GCR) is a promising anode reaction to replace the slow oxygen evolution reaction (OER), thus promoting the development of hydrogen production by electrochemical water splitting. Herein, NiFe‐based metal‐organic framework (MOF) is used as a precursor to prepare W‐doped nickel‐iron phosphide (W‐NiFeP) nanosheet arrays by ion exchange and phosphorylation, which exhibit a high electrocatalytic activity toward the hydrogen evolution reaction (HER), featuring an overpotential of only −179 mV to achieve the current density of 100 mA cm −2 in alkaline media. Notably, electrochemical activation of W‐NiFeP facilitates the in situ formation of phosphate groups producing W,P‐NiFeOOH, which, in conjunction with the W co‐doped amorphous layers, leads to a high electrocatalytic performance toward GCR, due to enhanced proton transfer and adsorption of reaction intermediates, as confirmed in experimental and theoretical studies. Thus, the two‐electrode electrolyzer of the W‐NiFeP/NF||W,P‐NiFeOOH/NF for HER||GCR needs only a low cell voltage of 1.56 V to deliver 100 mA cm −2 at a remarkable hydrogen production efficiency of 1.86 mmol h −1 , with a high glucose conversion (98.0%) and formic acid yields (85.2%). Results from this work highlight the significance of the development of effective electrocatalysts for biomass electrocatalytic‐conversion in the construction of high‐efficiency electrolyzers for green hydrogen production.