非对称电化学去离子体系中层状双金属氢氧化物电极的磷酸盐吸附性能优化

doi:10.1016/j.actphy.2026.100330

Abstract

Abstract:

Uncontrolled discharge of phosphate-containing wastewater causes severe aquatic eutrophication, posing a critical challenge to global water security. Electrochemical deionization (EDI) is a promising approach for phosphate removal, but its practical application is hindered by limited electrode capacity and capacity mismatch in asymmetric systems. Herein, cubic CoFe-layered double hydroxide (LDH) and nanospike coaxial CoAl LDH were in-situ grown on conductive carbon cloth (CC) via a one-step hydrothermal method as freestanding anodes for asymmetric EDI systems. The CoAl LDH electrode exhibits superior electrochemical performance and phosphate adsorption capacity compared to CoFe LDH, owing to its unique hierarchical structure and crystal structure that enables faster ion transport kinetics and richer active sites. By optimizing the cathode/anode mass ratio to 2 : 1, the capacity mismatch issue of the asymmetric system is effectively mitigated, and the optimized EDI system with CoAl LDH/CC anode delivers a high phosphate adsorption capacity of 41.9 mg P g⁻¹ at 1.2 V, along with excellent long-term stability (87% capacity retention after 120 h continuous operation). This work provides valuable insights for the development of high-performance EDI systems for phosphate removal.

Key words: Phosphate removal, Electrochemical deionization, Layered double hydroxide, Freestanding electrode

Cite this article

Ziquan Wang, Zhujie Liang, Xing Liu, Yihuang Lin, Jiangluo Liu, Zengye Chen, Libo Deng. Maximizing the phosphate adsorption capacity of layered double hydroxides in asymmetric electrochemical deionization systems[J]. Acta Phys. -Chim. Sin. 2026, 42(10), 100330. doi: 10.1016/j.actphy.2026.100330

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URL: https://www.whxb.pku.edu.cn/EN/10.1016/j.actphy.2026.100330

https://www.whxb.pku.edu.cn/EN/Y2026/V42/I10/100330

Figures/Tables 6

Fig 1

(a) Schematic of the synthetic route of LDH/CC and the working mechanism of the EDI cell for phosphate removal; (b) Low-magnified and (c) high-magnified FE-SEM images and elemental mappings (Co, Fe) of CoFe LDH/CC; (d) Low-magnified and (e) high-magnified FE-SEM images and elemental mappings (Co, Al) of CoAl LDH/CC."

Fig 1

Fig 2

XRD patterns of different (a) CoFe LDH/CC and (b) CoAl LDH/CC samples; (c) XPS survey spectra of CoFe LDH/CC and CoAl LDH/CC; High-resolution (d) Co 2p and (e) Fe 2p spectra of CoFe LDH/CC; (f) High-resolution Al 2p spectrum of CoAl LDH/CC."

Fig 2

Fig 3

(a) CV curves of various CoFe LDH/CC samples tested at a scan rate of 100 mV s−1; (b) CV curves of CoFe LDH/CC-2 tested at various scan rates; (c) Contributions of capacitive and diffusion-controlled capacitance at various scan rates, data are derived from Fig. 3b; (d) Nyquist plots of various CoFe LDH/CC samples; (e) CV curves of various CoAl LDH/CC samples tested at a scan rate of 100 mV s−1; (f) CV curves of CoAl LDH/CC-2 tested at various scan rates; (g) Contributions of capacitive and diffusive capacitance at various scan rates, data are derived from Fig. 3f; (h) Nyquist plots of various CoAl LDH/CC samples."

Fig 3

Fig 4

P adsorption capacity of CoFe LDH/CC-2 tested at various (a) voltages and (b) feed-solution pH values; (c) Variation of P adsorption capacity versus time and (d) P adsorption capacity of various materials; (e) Long-term stability of the EDI system operated at 1.2 V using CoAl LDH/CC-2 as anode; (f) Performance comparison plots between this work and previous studies (The data were extracted from references [9, 12b, 12c, 13a, 19b, 24])."

Fig 4

Fig 5

(a) Schematic diagram of the cell for electrode potential distribution measurements; (b) The potential of the working electrode (LDH/CC) varied with time; (c) CV curves of CoAl LDH/CC and YP-50F obtained at various potential windows in the three-electrode cell, the scan rate is 20 mV s−1; (d) Specific charge and cathode/anode charge ratio (Qc/Qa) obtained at various cathode/anode mass ratios (mc/ma); (e) Concentration variation profiles and (f) adsorption capacity of the EDI systems with various cathode/anode mass ratios."

Fig 5

Fig 6

(a) XRD patterns and (b) FTIR spectra of the samples before and after adsorption; (c) High-resolution P 2p XPS spectra of the samples after adsorption; (d) Raw data and pseudo-second-order kinetic model fitting results; (e) qe and k2 values derived from Fig. 6d; (f) Raw data and Langmuir model fitting results; (g) Optimized structures and calculated phosphate adsorption energies of CoFe LDH and CoAl LDH."

Fig 6

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