RESUMO
Hydrogen production by electrocatalytic water splitting is considered to be an effective and environmental method, and the design of an electrocatalyst with high efficiency, low cost, and multifunction is of great importance. Herein, we developed a crystalline NiFe phosphide (NiFeP)/amorphous P-doped FeOOH (P-FeOOH) heterostructure (defined as P-NiFeOxHy) as a high-efficiency multifunctional electrocatalyst for water electrolysis. The NiFeP nanocrystals provide remarkable electronic conductivity and plenty of active sites, the amorphous P-FeOOH improves the adsorption energy of oxygen-containing species, and the crystalline/amorphous heterostructure with superhydrophilic and superaerophobic surface generates synergistic effects, providing plentiful active sites and efficient charge/mass transfer. Benefiting from this, the designed P-NiFeOxHy displays ultralow overpotentials of 159.2 and 20.8 mV to achieve 10 mA cm-2 for oxygen evolution reaction and hydrogen evolution reaction, and also shows the superior performance of urea oxidation reaction with a low voltage of 1.37 V at 10 mA cm-2 in 1 M KOH with 0.33 M urea. In-situ Raman spectra and ex-situ XPS analysis were also used to investigate the catalytic process and reveal the surface structure evolution of P-NiFeOxHy under electrochemical oxidation. Accordingly, the designed P-NiFeOxHy is employed as both cathode and anode to assemble into the urea-assisted water electrolysis device, which can reach 10 mA cm-2 with a low 1.36 V and could be further driven by a solar cell. The work reveals a design of superior activity, cost-effective and multifunctional electrocatalysts for water splitting.
RESUMO
To carry out effective resource reforming of sustainable electricity, hydrogen production by electrochemical water splitting provides an eco-friendly and economical way. Nevertheless, the oxygen evolution reaction (OER) at the anode is limited by the slow reaction process, which hinders the large-scale development and application of electrolysis technology. In this work, we present an electrocatalyst with superior OER performance, which attributed to the abundant active sites and good electronic conductivity. The two-dimensional CoMo Layered Double Hydroxide nanosheets are synthesized and deposited on conductive carbon nanotubes (CoMo LDH/CNTs), and then hybrid composites show better catalytic performance than their undecorated counterpart under identical conditions. Specifically, CoMo LDH/CNTs exhibit the low overpotential of 268 mV to obtain 10 mA cm-2and satisfactory stability (more than 40 h). We emphasize that this hybridization strategy with a conductive supporting framework could design more abundant and low-cost OER electrocatalysts to minimize electrical energy consumption, thereby achieving efficient conversion between energy sources.
RESUMO
The conventional hydrogen evolution from water electrolysis is severely impeded by the sluggish kinetics of oxygen evolution reaction (OER). In this work, an integrated electrolysis system of replacing the anodic OER with a thermodynamically favorable ethanol oxidation reaction (EOR) has been developed by using PdSbBi/C as an electrocatalyst. To maximize the EOR performance, the composition of PdSbBi nanoparticles is tuned by varying the ratio of Sb and Bi precursors. Ternary PdSbBi-based electrocatalysts exhibit enhanced activity and stability toward EOR compared to commercial Pd/C and binary catalysts. In particular, the Pd76Sb17Bi7/C catalyst delivers a very high specific activity up to 52.4 mA cm-2 and mass activity of 2.66 A mg-1Pd. Besides, this EOR process is demonstrated to have high selectivity with acetic acid as the oxidation product in the electrolyte. When coupled with a cathodic platinum mash, the two-electrode electrolyzer cell requires a voltage input of merely 0.61 V to afford a current density of 10 mA cm-2. Density functional theory calculations reveal that the presence of Sb and Bi can promote the adsorption of hydroxide ions and facilitate the removal of reaction intermediates in the EOR pathway. This work provides a novel catalyst for the energy-efficient coproduction of acetic acid and hydrogen fuel.