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Vol. 18 (2026)

Enhancing the Selective OH− Adsorption for Durable Alkaline Seawater Oxidation at Industrial Current Densities

https://doi.org/10.1007/s40820-026-02133-8
Shangshu Hu
Key Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, 341119 Ganzhou, People’s Republic of China
Jiao Yang
Institute of Applied Physics and Materials Engineering, University of Macau, 999078 Macao SAR, People’s Republic of China
Yujuan Zhuang
Key Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, 341119 Ganzhou, People’s Republic of China
Xueyao Li
Key Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, 341119 Ganzhou, People’s Republic of China
Han Xu
Jiangxi University of Science and Technology, 341000 Ganzhou, People’s Republic of China
Fuwang Hu
Key Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, 341119 Ganzhou, People’s Republic of China
Zhishuo Yan
Department of Electrical and Computer Engineering, North Dakota State University, Fargo 810052, USA
Chao Liu
Jiangxi University of Science and Technology, 341000 Ganzhou, People’s Republic of China
Jianmin Yu
Key Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, 341119 Ganzhou, People’s Republic of China
Lishan Peng
Key Laboratory of Rare Earths, Ganjiang Innovation Academy, Chinese Academy of Sciences, 341119 Ganzhou, People’s Republic of China

Corresponding Author: Lishan Peng

lspeng@gia.cas.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 288

Abstract

The oxygen evolution reaction (OER) in seawater electrolysis is pivotal for sustainable hydrogen production, yet severe chloride ion (Cl−)-induced corrosion at the anode critically limits catalyst durability. Herein, we design a heterostructured catalyst comprising NiFe-layered double hydroxide and Ce(OH)CO3 (denoted as NiFe-LDH/Ce(OH)CO3) that exhibits remarkable OER stability in alkaline-simulated seawater. Experimental results and density functional theory calculations reveal that Ce(OH)CO3 incorporation modulates interfacial charge redistribution and enhances the Lewis acidity of Ni and Fe sites, thereby tuning the adsorption energetics of Cl− and OH−. Time-of-flight secondary ion mass spectrometry further confirms the preferential adsorption of OH− over Cl−, effectively suppressing Cl−-induced corrosion. As a result, NiFe-LDH/Ce(OH)CO3 demonstrates exceptional long-term stability, maintaining continuous operation for over 450 h at 1 A cm−2 in alkaline seawater. When integrated into an anion exchange membrane electrolyzer, the catalyst achieves 1 A cm−2 at a low cell voltage of 1.92 V and operates stably for over 60 h. The system delivers an impressive energy efficiency of 68.59% in alkaline-simulated seawater, corresponding to a hydrogen production cost as low as $0.97 per gasoline gallon equivalent at 500 mA cm−2.


Highlights:
1 The introduced Ce(OH)CO3 optimizes charge distribution and enhances Lewis acidity of Ni/Fe sites, facilitating OH− adsorption.
2 The NiFe-layered double hydroxide/Ce(OH)CO3 enables stable alkaline seawater electrooxidation for over 450 h at a high current density of 1 A cm−2.
3 In an anion exchange membrane system, an energy efficiency of 65.21% is attained at 1 A cm−2, with hydrogen production at a cost of USD 1.03 per gasoline gallon equivalent.

Keywords

Seawater electrolysis NiFe-LDH Heterostructure Chloridion repulsion Stability
Hu, Shangshu, Jiao Yang, Yujuan Zhuang, Xueyao Li, Han Xu, Fuwang Hu, Zhishuo Yan, Chao Liu, Jianmin Yu, and Lishan Peng. 2026. “Enhancing the Selective OH− Adsorption for Durable Alkaline Seawater Oxidation at Industrial Current Densities”. Nano-Micro Letters 18 (March):288. https://doi.org/10.1007/s40820-026-02133-8.
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References
  1. P.A. Kempler, R.H. Coridan, L. Luo, Gas evolution in water electrolysis. Chem. Rev. 124(19), 10964–11007 (2024). https://doi.org/10.1021/acs.chemrev.4c00211
  2. M. Chen, N. Kitiphatpiboon, C. Feng, A. Abudula, Y. Ma et al., Recent progress in transition-metal-oxide-based electrocatalysts for the oxygen evolution reaction in natural seawater splitting: A critical review. eScience 3(2), 100111 (2023). https://doi.org/10.1016/j.esci.2023.100111
  3. K. Christopher, R. Dimitrios, A review on exergy comparison of hydrogen production methods from renewable energy sources. Energy Environ. Sci. 5(5), 6640–6651 (2012). https://doi.org/10.1039/c2ee01098d
  4. Q. Kang, M. Su, Y. Luo, T. Wang, F. Gao et al., Chemical fermentation PoreCreation on multilevel bio-carbon structure with in situ Ni–Fe alloy loading for superior oxygen evolution reaction electrocatalysis. Nano-Micro Lett. 17(1), 269 (2025). https://doi.org/10.1007/s40820-025-01777-2
  5. Y. Liu, Y. Wang, P. Fornasiero, G. Tian, P. Strasser et al., Long-term durability of seawater electrolysis for hydrogen: from catalysts to systems. Angew. Chem. Int. Ed. 63(47), e202412087 (2024). https://doi.org/10.1002/anie.202412087
  6. J. Chen, X. Shi, S. Feng, J. Li, X. Gao et al., Design of highly active and durable oxygen evolution catalyst with intrinsic chlorine inhibition property for seawater electrolysis. Nano Mater. Sci. 6(4), 413–418 (2024). https://doi.org/10.1016/j.nanoms.2023.10.003
  7. R. Fan, C. Liu, Z. Li, H. Huang, J. Feng et al., Ultrastable electrocatalytic seawater splitting at ampere-level current density. Nat. Sustain. 7(2), 158–167 (2024). https://doi.org/10.1038/s41893-023-01263-w
  8. C. Zhao, Z. Ding, K. Zhang, Z. Du, H. Fang et al., Comprehensive chlorine suppression: advances in materials and system technologies for direct seawater electrolysis. Nano-Micro Lett. 17(1), 113 (2025). https://doi.org/10.1007/s40820-025-01653-z
  9. Y. Yao, C. Zou, S. Sun, Y. Guo, S. Hong et al., Ultrastable seawater oxidation at ampere-level current densities with corrosion-resistant CoCO3/CoFe layered double hydroxide electrocatalyst. Small 21(4), e2409627 (2025). https://doi.org/10.1002/smll.202409627
  10. Y. Song, K. Ji, H. Duan, M. Shao, Hydrogen production coupled with water and organic oxidation based on layered double hydroxides. Exploration 1(3), 20210050 (2021). https://doi.org/10.1002/EXP.20210050
  11. Y. Yao, S. Sun, H. Zhang, Z. Li, C. Yang et al., Enhancing the stability of NiFe-layered double hydroxide nanosheet array for alkaline seawater oxidation by Ce doping. J. Energy Chem. 91, 306–312 (2024). https://doi.org/10.1016/j.jechem.2024.01.011
  12. J. Mu, C. Yu, X. Song, L. Chen, J. Zhao et al., A super-chlorophobic yet weak-reconstructed electrocatalyst by fluorination engineering toward chlorine oxidation-free and high-stability seawater electrolysis. Adv. Funct. Mater. 35(23), 2423965 (2025). https://doi.org/10.1002/adfm.202423965
  13. B. Zhang, S. Liu, S. Zhang, Y. Cao, H. Wang et al., High corrosion resistance of NiFe-layered double hydroxide catalyst for stable seawater electrolysis promoted by phosphate intercalation. Small 18(45), e2203852 (2022). https://doi.org/10.1002/smll.202203852
  14. L.-J. Yang, H.-Y. Guan, S. Yuan, T. Sun, A.-N. Jiang et al., Research progress of chlorine corrosion resistance in seawater electrolysis: materials and technologies. Chem. Eng. J. 503, 158458 (2025). https://doi.org/10.1016/j.cej.2024.158458
  15. H. Qi, K. Huang, F. Pan, R. Ma, C. Lian et al., Boosting direct seawater electrolysis through intercalation engineering of layered double hydroxides. Ind. Eng. Chem. Res. 62(46), 19674–19682 (2023). https://doi.org/10.1021/acs.iecr.3c03014
  16. X. Fang, C. Ye, W. Zhuang, Y. Yang, S. Hong et al., High-coverage Ce(OH)₃-decorated NiFe layered double hydroxide for durable seawater oxidation at ampere-scale current densities. Small 21(31), e2505219 (2025). https://doi.org/10.1002/smll.202505219
  17. H. Chen, P. Liu, W. Li, W. Xu, Y. Wen et al., Stable seawater electrolysis over 10,000 H via chemical fixation of sulfate on NiFeBa-LDH. Adv. Mater. 36(45), e2411302 (2024). https://doi.org/10.1002/adma.202411302
  18. H. Liu, W. Shen, H. Jin, J. Xu, P. Xi et al., High-performance alkaline seawater electrolysis with anomalous chloride promoted oxygen evolution reaction. Angew. Chem. Int. Ed. 62(46), e202311674 (2023). https://doi.org/10.1002/anie.202311674
  19. P. Blöchl, Projector augmented-wave method. Phys. Rev. B 50(24), 17953–17979 (1994). https://doi.org/10.1103/physrevb.50.17953
  20. G. Kresse, J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set. Phys. Rev. B 54(16), 11169–11186 (1996). https://doi.org/10.1103/physrevb.54.11169
  21. J. Perdew, K. Burke, M. Ernzerhof, Generalized gradient approximation made simple. Phys. Rev. Lett. 77(18), 3865–3868 (1996). https://doi.org/10.1103/PhysRevLett.77.3865
  22. M.H. Weiler, R.L. Aggarwal, B. Lax, Interband magnetoreflectance in semiconducting Hg1−xCdxTe alloys. Phys. Rev. B 16(8), 3603–3607 (1977). https://doi.org/10.1103/physrevb.16.3603
  23. J.K. Nørskov, J. Rossmeisl, A. Logadottir, L. Lindqvist, J.R. Kitchin et al., Origin of the overpotential for oxygen reduction at a fuel-cell cathode. J. Phys. Chem. B 108(46), 17886–17892 (2004). https://doi.org/10.1021/jp047349j
  24. R. Xiang, C. Tong, Y. Wang, L. Peng, Y. Nie et al., Hierarchical coral-like FeNi(OH)x/Ni via mild corrosion of nickel as an integrated electrode for efficient overall water splitting. Chin. J. Catal. 39(11), 1736–1745 (2018). https://doi.org/10.1016/S1872-2067(18)63150-X
  25. W. Zhao, J. Deng, M. Li, G. Du, M. Fan et al., Rational synthesis of sea urchin-like NiCo-LDH/tannin carbon microsphere composites using microwave hydrothermal technique for high-performance asymmetric supercapacitor. Adv. Compos. Hybrid Mater. 8(2), 215 (2025). https://doi.org/10.1007/s42114-025-01220-5
  26. S. Shen, Q. Li, H. Zhang, D. Yang, J. Gong et al., Negative-valent platinum stabilized by Pt─Ni electron bridges on oxygen-deficient NiFe-LDH for enhanced electrocatalytic hydrogen evolution. Adv. Mater. 37(15), e2500595 (2025). https://doi.org/10.1002/adma.202500595
  27. M. Ying, X. Lin, G. Yang, H. Ye, H. Pan et al., Rich oxygen vacancies on ultrathin NiFe layered double hydroxide nanosheets raised by cerium-assisted synthesis for enhanced electrocatalytic water oxidation. Colloids Surf. A Physicochem. Eng. Aspects 627, 127142 (2021). https://doi.org/10.1016/j.colsurfa.2021.127142
  28. Y. Zhu, J. Wang, G. Weiser, M. Klingenhof, T. Koketsu et al., Ru single atoms and sulfur anions dual-doped NiFe layered double hydroxides for high-current-density alkaline oxygen evolution reaction. Adv. Energy Mater. 15(23), 2500554 (2025). https://doi.org/10.1002/aenm.202500554
  29. Y. Dai, X. Tu, K. Yue, Y. Wan, P. Zhao et al., Anti-dissolving high entropy phosphorus sulfide for efficient and durable seawater electrolysis. Adv. Funct. Mater. 35(12), 2417211 (2025). https://doi.org/10.1002/adfm.202417211
  30. L. Peng, N. Yang, Y. Yang, Q. Wang, X. Xie et al., Atomic cation-vacancy engineering of NiFe-layered double hydroxides for improved activity and stability towards the oxygen evolution reaction. Angew. Chem. Int. Ed. 60(46), 24612–24619 (2021). https://doi.org/10.1002/anie.202109938
  31. N. Iyi, T. Matsumoto, Y. Kaneko, K. Kitamura, Deintercalation of carbonate ions from a hydrotalcite-like compound: enhanced decarbonation using acid−salt mixed solution. Chem. Mater. 16(15), 2926–2932 (2004). https://doi.org/10.1021/cm049579g
  32. M. Tipplook, T. Sudare, H. Shiiba, A. Seki, K. Teshima, Single-step topochemical synthesis of NiFe layered double hydroxides for superior anion removal from aquatic systems. ACS Appl. Mater. Interfaces 13(43), 51186–51197 (2021). https://doi.org/10.1021/acsami.1c13706
  33. M. Li, X. Wang, K. Liu, Z. Zhu, H. Guo et al., Ce-induced differentiated regulation of co sites via gradient orbital coupling for bifunctional water-splitting reactions. Adv. Energy Mater. 13(30), 2301162 (2023). https://doi.org/10.1002/aenm.202301162
  34. M. Liu, K.-A. Min, B. Han, L.Y.S. Lee, Interfacing or doping? role of Ce in highly promoted water oxidation of NiFe-layered double hydroxide. Adv. Energy Mater. 11(33), 2101281 (2021). https://doi.org/10.1002/aenm.202101281
  35. L.-B. Liu, Y.-F. Tang, S. Liu, M. Yu, Y. Sun et al., Unraveling the trade-off between oxygen vacancy concentration and ordering of perovskite oxides for efficient lattice oxygen evolution. Adv. Energy Mater. 15(5), 2402967 (2025). https://doi.org/10.1002/aenm.202402967
  36. Q. Peng, J. Zhu, F. Wei, T.T. Isimjan, T. Sun et al., Lattice strain induced Ni0.85Se/WO2.90 heterostructures accelerate dynamic reconstruction for efficient water oxidation. Appl. Catal. B Environ. 384, 126158 (2026). https://doi.org/10.1016/j.apcatb.2025.126158
  37. X. He, Y. Yao, M. Zhang, Y. Zhou, L. Zhang et al., Engineered PW12-polyoxometalate docked Fe sites on CoFe hydroxide anode for durable seawater electrolysis. Nat. Commun. 16(1), 5541 (2025). https://doi.org/10.1038/s41467-025-60620-9
  38. K. Yue, R. Lu, M. Gao, F. Song, Y. Dai et al., Polyoxometalated metal-organic framework superstructure for stable water oxidation. Science 388(6745), 430–436 (2025). https://doi.org/10.1126/science.ads1466
  39. J. Wang, Y. Liu, G. Yang, Y. Jiao, Y. Dong et al., MXene-assisted NiFe sulfides for high-performance anion exchange membrane seawater electrolysis. Nat. Commun. 16(1), 1319 (2025). https://doi.org/10.1038/s41467-025-56639-7
  40. L. Zhang, J. Liang, L. Yue, K. Dong, J. Li et al., Benzoate anions-intercalated NiFe-layered double hydroxide nanosheet array with enhanced stability for electrochemical seawater oxidation. Nano Res. Energy 1, e9120028 (2022). https://doi.org/10.26599/nre.2022.9120028
  41. Y. Yu, W. Zhou, J. Yuan, X. Zhou, X. Meng et al., A hydrogen-bond network sieve enables selective OH−/Cl− discrimination for stable seawater splitting at 2.0 A cm−2. Energy Environ. Sci. 18(22), 9949–9958 (2025). https://doi.org/10.1039/d5ee04595a
  42. L. Liu, Y. Chen, Q. Zhang, Z. Liu, K. Yue et al., Superhydrophilic NiFe-LDH@ Co9S8–Ni3S2/NF heterostructures for high-current-density freshwater/seawater oxidation electrocatalysts. Appl. Catal. B Environ. Energy 354, 124140 (2024). https://doi.org/10.1016/j.apcatb.2024.124140
  43. M. Rong, Y. Mo, S. Zhou, X. Ma, S. Wang et al., Ce and MoS2 dual-doped cobalt aluminum layered double hydroxides for enhanced oxygen evolution reaction. Int. J. Hydrog. Energy 47(3), 1644–1655 (2022). https://doi.org/10.1016/j.ijhydene.2021.10.222
  44. F.O. Boakye, F.U. Zaman, H. Zhang, A. Saeed, F.T. Dajan et al., Functional interface optimization strategy for Fe3Se4/NiSe2 anchored on MXene for ultrastable seawater splitting at industrial-level current density. Adv. Funct. Mater. 35(32), 2424718 (2025). https://doi.org/10.1002/adfm.202424718
  45. R. Yuan, C. Liao, L. Cao, D. Li, S. Sun et al., Highly efficiency seawater electrolysis guided by coordinating catalysis of oxygen evolution reaction. Adv. Funct. Mater. 36(3), e08413 (2026). https://doi.org/10.1002/adfm.202508413
  46. Z. Cai, J. Liang, Z. Li, T. Yan, C. Yang et al., Stabilizing NiFe sites by high-dispersity of nanosized and anionic Cr species toward durable seawater oxidation. Nat. Commun. 15(1), 6624 (2024). https://doi.org/10.1038/s41467-024-51130-1
  47. N.-N. Liang, D.J. Kim, Z. Qiu, Y. Kweon, T.W. Kim et al., Defective antifluorite MnO2-layered RuO2 for direct seawater electrolysis at circum-neutral pH. Small 21(35), 2504249 (2025). https://doi.org/10.1002/smll.202504249
  48. W. Liu, J. Yu, T. Li, S. Li, B. Ding et al., Self-protecting CoFeAl-layered double hydroxides enable stable and efficient brine oxidation at 2 A cm−2. Nat. Commun. 15(1), 4712 (2024). https://doi.org/10.1038/s41467-024-49195-z
  49. Y. Yu, W. Zhou, X. Zhou, J. Yuan, X. Zhang et al., The corrosive Cl−–induced rapid surface reconstruction of amorphous NiFeCoP enables efficient seawater splitting. ACS Catal. 14(24), 18322–18332 (2024). https://doi.org/10.1021/acscatal.4c05704
  50. Q. Tu, W. Liu, M. Jiang, W. Wang, Q. Kang et al., Preferential adsorption of hydroxide ions onto partially crystalline NiFe-layered double hydroxides leads to efficient and selective OER in alkaline seawater. ACS Appl. Energy Mater. 4(5), 4630–4637 (2021). https://doi.org/10.1021/acsaem.1c00262
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