Title: One-step architecture of bifunctional petal-like oxygen-deficient NiAl-LDHs nanosheets for high-performance hybrid supercapacitors and urea oxidation

Abstract: Nickel-based layered double hydroxides (LDHs) are promising electrode materials in the fields of energy storage (supercapacitors) and conversion (urea oxidation). The rational construction of atomic and electronic structure is crucial for nickel-based LDHs to realize their satisfactory electrochemical performance. Herein, we report a facile, ecofriendly, one-step synthesis process to construct petal-like oxygen-deficient NiAl-LDH nanosheets for hybrid super-capacitors (HSCs) and urea oxidation reaction (UOR). The asprepared NiAl-LDH nanosheets with rich oxygen vacancies possess a large specific surface area of 216.6 m2 g-1 and a desirable electronic conductivity of 3.45 * 10-4 S cm-1 to deliver an ultra-high specific capacitance of 2801 F g-1 (700 C g-1) at 1 A g-1. Furthermore, high specific energy of 50.0 W h kg-1 at 400 W kg-1 and excellent cycle stability with 91% capacitance retention after 10,000 cycles are achieved by the NiAl-LDHs/CFP (carbon fiber paper) (+)//YP-80F (a commercial activated carbon) (-) HSC. Besides, NiAl-LDH nanosheets also work as an efficient electrocatalyst for UOR, which only requires 1.42 V vs. reversible hydrogen electrode to drive 10 mA cm-2 in 1 mol L-1 KOH with 0.33 mol L-1 urea. This remarkable performance is superior to most reported values of previous candidates owing to the thin structure of NiAl-LDH nanosheets for exposing more active sites and abundant oxygen vacancies. In addition, various reaction parameters are investigated to optimize the electrochemical performance. In general, this work paves a new way for the architecture of multifunctional nanostructured energy materials.