As promising hydrogen energy carrier, formic acid (HCOOH) plays an indispensable role in building a complete industry chain of a hydrogen economy. Currently, the biomass upgrading assisted water electrolysis has emerged as an attractive alternative for co‐producing green HCOOH and H2 in a cost‐effective manner, yet simultaneously affording high current density and Faradaic efficiency (FE) still remains a big challenge. Here, the ternary NiVRu‐layered double hydroxides (LDHs) nanosheet arrays for selective glycerol oxidation and hydrogen evolution catalysis are reported, which yield an industry‐level 1 A cm−2 at voltage of 1.933 V, meanwhile showing considerable HCOOH and H2 productivities of 12.5 and 17.9 mmol cm−2 h−1, with FEs of almost 80% and 96%, respectively. Experimental and theoretical results reveal that the introduced Ru atoms can tune the local electronic structure of Ni‐based LDHs, which not only optimizes hydrogen adsorption kinetics for HER, but also reduces the reaction energy barriers for both the conversion of NiII into GOR‐active NiIII and carboncarbon (CC) bond cleavage. In short, this work highlights the potential of large‐scale H2 and HCOOH productions from integrated electrocatalytic system and provides new insights for designing advanced electrocatalyst for low‐cost and sustainable energy conversion.

Electrochemical Biomass Upgrading Coupled with Hydrogen Production under Industrial‐Level Current Density

La-doped NiFe-LDH coupled with hierarchical vertically aligned MXene frameworks for efficient overall water splitting

FeOOH-containing hydrated layered iron vanadate electrocatalyst for superior oxygen evolution reaction and efficient water splitting

Ultrathin defective high-entropy layered double hydroxides for electrochemical water oxidation

Recent progress on self-supported two-dimensional transition metal hydroxides nanosheets for electrochemical energy storage and conversion

In-situ optimizing the valence configuration of vanadium sites in NiV-LDH nanosheet arrays for enhanced hydrogen evolution reaction

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In-situ optimizing the valence configuration of vanadium sites in NiV-LDH nanosheet arrays for enhanced hydrogen evolution reaction