2D-on-2D Al-Doped NiCo LDH Nanosheet Arrays for Fabricating High-Energy-Density, Wide Voltage Window, and Ultralong-Lifespan Supercapacitors.

Battery-type electrode materials with high capacity, wide potential windows, and good cyclic stability are crucial to breaking through energy storage limitations and achieving high energy density. Herein, a novel 2D-on-2D Al-doped NiCo layered double hydroxide (NiCoAlx LDH) nanosheet arrays with high-mass-loading are grown on a carbon cloth (CC) substrate via a two-step hydro/solvothermal deposition strategy, and the effect of Al doping is employed to modify the deposition behavior, hierarchical morphology, phase stability, and multi-metallic synergistic effect. The optimized NiCoAl0.1 LDH electrode exhibits capacities of 5.43, 6.52, and 7.25 C cm-2 (9.87, 10.88, and 11.15 F cm-2) under 0-0.55, 0-0.60, and 0-0.65 V potential windows, respectively, illustrating clearly the importance of the wide potential window. The differentiated deposition strategy reduces the leaching level of Al3+ cations in alkaline solutions, ensuring excellent cyclic performance (108% capacity retention after 40 000 cycles). The as-assembled NiCoAl0.1 LDH//activated carbon cloth (ACC) hybrid supercapacitor delivers 3.11 C cm-2 at 0-2.0 V, a large energy density of 0.84 mWh cm-2 at a power density of 10.00 mW cm-2, and excellent cyclic stability with ≈135% capacity retention after 150 000 cycles.

CoNi2 S4 Electrode with High Mass-Loading for High-Energy-Density Supercapacitor: Role of S-Containing Anions Exchange.

Anion exchange is recognized as an effective method to regulate the composition, electronic conductivity, and electrochemical behavior of the transition metal-based compounds. In this work, anion exchange is adopted as a rational post-treatment route to facilitate the capacitive activity of CoNi2 S4 nanoparticle arrays grown on carbon cloth (CC) with high mass-loading. As soaked in saturated Na2 S solution, the CoNi2 S4 /CC electrode showed an increased capacity from 483 C g-1 to 841 C g-1 at 10 mA cm-2 with excellent rate performance and stable cycling performance, which was superior to the CoNi2 S4 /CC electrode activated by NaBH4 reduction. Anion exchange was beneficial for enhancing the crystallinity, retaining the adhesion of nanoarrays, and realizing low resistance nature in a mild route. The as-assembled CoNi2 S4 /CC//activated CC hybrid supercapacitor delivered a high areal capacitance of 1.28 F cm-2 at 5 mA cm-2 , and achieved an energy density of 0.58 mWh cm-2 at a power density of 4.5 mW cm-2 with excellent cycle stability with 90.6 % capacity retention after 10000 cycles.

Anion Exchange of Ni-Co Layered Double Hydroxide (LDH) Nanoarrays for a High-Capacitance Supercapacitor Electrode: A Comparison of Alkali Anion Exchange and Sulfuration.

A facile and new anion exchange process is presented, which involves the conversion of NiCo-CO3 layered double hydroxide (LDH) nanosheet arrays in an alkaline solution. The anion exchange between CO3 2- and OH- results in the construction of a reservoir for OH- anions, and the decoration of thin nanoflakes on the surface of nanosheets effectively enlarges the surface area of NiCo LDH nanoarrays. The capacitance of the as-soaked NiCo LDH nanoarrays electrode increases from 1.78 F cm-2 (684 F g-1 ) to 6.22 F cm-2 (2391 F g-1 ) at 2 mA cm-2 after soaking for 12 h. Moreover, the soaked NiCo-OH LDH electrode exhibits an enhanced rate capacity, high coulombic efficiency, and good cycling stability compared with the Ni-Co-S nanosheet electrode synthesized through a hydrothermal sulfuration process. The as-assembled all-solid-state NiCo LDH//active carbon asymmetric supercapacitor shows a maximum energy density of 83.4 W h kg-1 at a power density of 1066 W kg-1 .

Quasi-Parallel NiFe Layered Double Hydroxide Nanosheet Arrays for Large-Current-Density Oxygen Evolution Electrocatalysis.

Designing advanced electrocatalysts for oxygen evolution at large current density (>500 mA cm-2 ) is critical to practical water splitting applications. Herein, a novel quasi-parallel NiFe layered double hydroxide (NiFe LDH) nanosheet arrays with pattern alignment on Ni foam was developed. The initial α-Ni(OH)2 layer induced effective coprecipitation between Ni2+ and Fe3+ for the formation of LDH phase, guaranteeing the electronic pulling effect among metal cations and enhancing the interaction between active materials and substrate for excellent adhesion and electrical conductivity. Quasi-parallel NiFe LDH nanoarrays exhibited outstanding oxygen evolution activity with a small Tafel slope of 30.1 mV dec-1 and overpotentials of 196, 255, and 284 mV at a current density of 10, 500, and 1000 mA cm-2 in 1.0 m KOH solution, respectively, and high stability over 40 h at 750 mA cm-2 . This work presents a new strategy towards fabricating electrode materials with exceptional performance.

In situ fabrication of Ni-Co (oxy)hydroxide nanowire-supported nanoflake arrays and their application in supercapacitors.

Three-dimensional (3D) hybrid nanostructured arrays grown on a flexible substrate have recently attracted great attention owing to their potential application as supercapacitor electrodes in portable and wearable electronic devices. Here, we report an in situ conversion of Ni-Co active electrode materials for the fabrication of high-performance electrodes. Ni-Co carbonate hydroxide nanowire arrays on carbon cloth were initially synthesized via a hydrothermal method, and they were gradually converted to Ni-Co (oxy)hydroxide nanowire-supported nanoflake arrays after soaking in an alkaline solution. The evolution of the supercapacitor performance of the soaked electrode was investigated in detail. The areal capacitance increases from 281 mF cm-2 at 1 mA cm-2 to 3710 and 3900 mF cm-2 after soaking for 36 h and 48 h, respectively. More interestingly, the electrode also shows an increased capacitance with charge/discharge cycles due to the long-time soaking in KOH solution, suggesting novel cycling durability. The enhancement in capacitive performance should be related to the formation of a unique nanowire-supported nanoflake array architecture, which controls the agglomeration of nanoflakes, making them fully activated. As a result, the facile in situ fabrication of the hybrid architectural design in this study provides a new approach to fabricate high-performance Ni/Co based hydroxide nanostructure arrays for next-generation energy storage devices.

Synthesis of cellulose dehydroabietate in ionic liquid [bmim]Br.

A new type of cellulose derivative, cellulose dehydroabietate (CDA), was synthesized by the O-acylation reaction of cellulose with dehydroabietic acid chloride (DHAC) using ionic liquid 1-butyl-3-methylimidazolium bromide ([bmim]Br) as a solvent and 4-dimethyl-aminopyridine (DMAP) as a catalyst. The resulting CDA was characterized by means of FT-IR, X-ray diffraction (XRD), scanning electron microscopy (SEM), thermal gravimetric analysis (TGA), and elemental analysis. Also, some properties of CDA were determined. These results showed that CDA has better solubility, water-repellency, and resistance to acids and bases than raw cellulose, and these properties increase with the DS of CDA.