Kinetic-Thermodynamic Promotion Engineering toward High-Density Hierarchical and Zn-Doping Activity-Enhancing ZnNiO@CF for High-Capacity Desalination

doi:10.1007/s40820-024-01371-y

Abstract

Abstract:

Despite the promising potential of transition metal oxides (TMOs) as capacitive deionization (CDI) electrodes, the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity, posing a major obstacle. Herein, we prepared the kinetically favorable Zn_xNi_1 − xO electrode in situ growth on carbon felt (Zn_xNi_1 − xO@CF) through constraining the rate of OH⁻ generation in the hydrothermal method. Zn_xNi_1 − xO@CF exhibited a high-density hierarchical nanosheet structure with three-dimensional open pores, benefitting the ion transport/electron transfer. And tuning the moderate amount of redox-inert Zn-doping can enhance surface electroactive sites, actual activity of redox-active Ni species, and lower adsorption energy, promoting the adsorption kinetic and thermodynamic of the Zn_0.2Ni_0.8O@CF. Benefitting from the kinetic-thermodynamic facilitation mechanism, Zn_0.2Ni_0.8O@CF achieved ultrahigh desalination capacity (128.9 mg_NaCl g⁻¹), ultra-low energy consumption (0.164 kW h kg_NaCl⁻¹), high salt removal rate (1.21 mg_NaCl g⁻¹ min⁻¹), and good cyclability. The thermodynamic facilitation and Na⁺ intercalation mechanism of Zn_0.2Ni_0.8O@CF are identified by the density functional theory calculations and electrochemical quartz crystal microbalance with dissipation monitoring, respectively. This research provides new insights into controlling electrochemically favorable morphology and demonstrates that Zn-doping, which is redox-inert, is essential for enhancing the electrochemical performance of CDI electrodes.

Key words: Zinc-nickel metal oxide, High-density hierarchical, Capacitive deionization, Zinc-doping

Jie Ma, Siyang Xing, Yabo Wang, Jinhu Yang, Fei Yu. Kinetic-Thermodynamic Promotion Engineering toward High-Density Hierarchical and Zn-Doping Activity-Enhancing ZnNiO@CF for High-Capacity Desalination[J]. Nano-Micro Letters, 2024, 16(1): 143-.

Jie Ma, Siyang Xing, Yabo Wang, Jinhu Yang, Fei Yu. [J]. Nano-Micro Letters, 2024, 16(1): 143-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-024-01371-y

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/143

Figures/Tables 5

Fig. 1 a Schematic illustration of the layer Zn_xNi_1 − xO@CF preparation. SEM of the b Zn_0.2Ni_0.8O@CF-2, c Zn_0.2Ni_0.8O@CF-4 and d Zn_0.2Ni_0.8O@CF-6. e EDS mapping image of Zn_0.2Ni_0.8O@CF-4, f N₂ adsorption/desorption isotherms and g XRD patterns of Zn_xNi_1 − xO@CF with different Zn-doping. XPS spectrum of Ni 2p h and Zn 2p i for Zn_0.2Ni_0.8O@CF

Fig. 2 a CV curves of NiO@CF, Zn_0.1Ni_0.9O@CF, Zn_0.2Ni_0.8O@CF and Zn_0.4Ni_0.6O@CF and b specific capacity of various scan rates. c CV curves of Zn_0.2Ni_0.8O@CF measured at different scan rates and d after 100 cycles at 10 mV s⁻¹. e Normalized contribution ratios of surface-/diffusion-controlled capacities and f GCD profiles of Zn_0.2Ni_0.8O@CF. g Nyquist plots and h simulated internal and charge transfer resistance of NiO@CF and Zn_0.2Ni_0.8O@CF

Fig. 3 a Schematic diagram of CDI process. b SAC of Zn_0.2Ni_0.8O, NiO and CF electrodes at different current densities. c The profiles of the conductivity, voltage, and current at various specific current. d SAC of Zn_0.2Ni_0.8O at different cut-off voltages. e Ragone plots of various electrodes. f CE and SEC of Zn_0.2Ni_0.8O. g Comparison of SAC and SEC between Zn_0.2Ni_0.8O and other state-of-the-art materials. h Cycling and regeneration performance of Zn_0.2Ni_0.8O at 1500 mA m⁻² over 100 cycles. Inset is the real-time conductivity and voltage profiles

Fig. 4 a Calculation of b-values of Zn_0.2Ni_0.8O based on CV curves. b The relationship between 1/q^∗ and v^1/2 and between q^∗ and v^−1/2. c △f/5 responses of Zn_0.2Ni_0.8O from EQCM-D during CV at different scan rates. The simultaneous d mass change and current response and e change in electrode mass versus charge passed during Zn_0.2Ni_0.8O electrode adsorption/desorption processes at 10 mV s⁻¹ between − 0.4 ~ 0.8 V. Blue region highlights the process of adsorption and yellow highlights the process of desorption

Fig. 5 a Ex situ XPS spectra/data of Ni 2p_3/2 of NiO and Zn_0.2Ni_0.8O electrodes in original states and in completely adsorption/desorption states after the third desalination cycle at ± 1.4 V at 1000 mA cm⁻². b Side view of relaxed adsorption configurations for corresponding E_ads for Na⁺ on NiO and Zn_0.2Ni_0.8O with (225) surfaces, along with the Bader charge and difference charge density analysis. c E_ads and Bader charge for single Na⁺ analysis of the electrodes

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