Cation and anion-codoped Cr,S-NiFe nanosheet arrays as efficient electrocatalysts for boosting electrocatalytic glucose conversion coupled with H2 generation

Coupling hydrogen production with electrocatalytic biomass conversion driven by intermittent renewable energy sources is an efficient way to obtain hydrogen energy and high-value-added chemicals. However, developing robust multifunctional electrocatalysts with explicit structure-property relationships remains a considerable challenge. Herein, a cation and anion codoping strategy for synergistically modulating the electronic structure of NiFe layered double hydroxide was dexterously developed, visibly promoting the exposure of catalytic active sites and thus enhancing the performance of the electrocatalytic conversion of glucose coupled with hydrogen production. The experimental results proved that the incorporation of heteroatoms Cr and S promoted the reversible Ni(OH) 2 (Ni 2+ )/NiOOH (Ni 3+ ) redox transition and significantly enhanced the charge transfer and adsorption capacity of glucose. For the electrocatalytic glucose conversion reaction (GCR), the voltage required to achieve 10 mA cm −2 was only 1.219 V, lower than that required in the oxygen evolution reaction. Notably, the as-prepared Cr,S-NiFe/NF exhibited remarkable performance in a double-electrode electrolyzer for GCR and hydrogen evolution reaction, requiring only an ultralow voltage of 1.337 V to deliver 10 mA cm −2 while producing value-added formate at the anode, and a nine times higher hydrogen production rate than that of conventional water electrolysis was achieved. This electrocatalyst for biomass conversion coupled with hydrogen production exhibited improved hydrogen production efficiency and yielded value-added chemicals.