Scalable synthesis of a cost-effective NiFeCuComedium-entropy alloy aerogel with lattice distortion and dynamic surface self-reconstruction for efficient water electrolysis
Source abstract
Abstract
The rational design of medium-entropy alloy aerogels (MEAA) with tailored electronic structures efficiently addresses the sluggish kinetics of the oxygen evolution reaction (OER). Here, we report a scalable synthesis of an all-non-precious metal NiFeCuCo MEAA featuring a three-dimensional interconnected “pearl-like” structure and a high BET-specific surface area (106.41 m2·g− 1). NiFeCuCo MEAA is dominated by FeNi alloys with embedded Cu and Co atoms, inducing significant lattice distortions and atomic disorder. This entropy-driven engineering optimizes the electronic structure and enhances intrinsic catalytic activity. The scalable synthesis achieves a yield of 7.2 ± 0.3 g per batch, highlighting its industrial scalability. The NiFeCuCo MEAA demonstrates exceptional OER performance with a 200 mV overpotential at 10 mA·cm− 2, and a Tafel slope of 48.86 mV·dec− 1. In-situ Raman spectroscopy reveals surface self-reconstruction to NiOOH during operation, which enhances catalytic performance and protects the internal structure against corrosion, ensuring high durability. Density functional theory calculations confirm that Ni-site–dominated electronic structure optimization reduces the binding energy of *O, which improves the OER activity. When NiFeCuCo MEAA is integrated at the anode in an anion-exchange membrane water electrolyzer, the current density is up to 1.35 A·cm− 2, with a cell efficiency of 79.8% and a stable operation of 100 h.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Electrocatalysts for Energy Conversion · Ammonia Synthesis and Nitrogen Reduction · Advanced battery technologies research
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (50)
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1. Lin LH, Ma YW, Vequizo JM et al (2024) Efficient and stable visible-light-driven Z-scheme overall water splitting using an oxysulfide H2 evolution photocatalyst. Nat Commun 15:39710.1038/s41467-024-44706-4 ↗
2. Xu YM, Mao ZX, Zhang JF et al (2024) Strain-modulated Ru-O covalency in Ru-Sn oxide enabling efficient and stable water oxidation in acidic solution. Angew Chem Int Ed 63:e20231602910.1002/anie.202316029 ↗
3. Zhang JC, Weatherspoon E, Alsubaie AS et al (2025) Phosphorus-doped nickel-cobalt layered hydroxide supported three-dimensional substrate as efficient oxygen evolution electrocatalyst. Adv Compos Hybrid Ma 8:7210.1007/s42114-024-01164-2 ↗
4. Park YS, Choi GH, Jung JY et al (2024) Engineering durable anion exchange membrane water electrolyzers through suppressed electrochemical corrosion of a NiFe-graphitic carbon shell anode catalyst. ACS Catal 14:9969–998410.1021/acscatal.4c02696 ↗
5. Xie XY, Zhang YX, Qin Y et al (2025) Bifunctional mixed-valence ruthenium heterostructure for robust electrocatalytic water splitting in acid media. Adv Compos Hybrid Mater 8:13310.1007/s42114-025-01234-z ↗
6. Wu XD, Liu L, Yuan K et al (2024) Modulating electronic structure and atomic insights into the novel hierarchically porous PdCuFe trimetallic alloy aerogel for efficient oxygen reduction. Small 19:230724310.1002/smll.202307243 ↗
7. Zhu B, Huang SD, Seo O et al (2025) Stabilizing the unstable: enhancing OER durability with 3d-orbital transition metal multielemental alloy nanoparticles by atomically dispersed 4d-orbital Pd for a 100-fold extended lifetime. J Am Chem Soc 147:11250–1125610.1021/jacs.4c18109 ↗
8. Arindam M, Ankita P, Aniruddha K et al (2025) Hyper-cross-linked polymer-derived carbon-coated Fe-Ni alloy/CNT as a bifunctional electrocatalyst for rechargeable Zinc-air batteries. J Phys Chem Lett 16:1051–106510.1021/acs.jpclett.4c03361 ↗
9. Kim J, Yu JM, Jang W et al (2025) Enhancing water oxidation catalysis by controlling metal cation distribution in layered double hydroxides. Adv Funct Mater 34:2420810
10. Enkhtuvshin E, Yeo S, Choi H et al (2025) Surface reconstruction of Ni-Fe layered double hydroxide inducing chloride ion blocking materials for outstanding overall seawater splitting. Adv Funct Mater 33:221406910.1002/adfm.202214069 ↗
11. Song LM, Zhang D, Miao HF et al (2024) Interstitial atom-doped NiFe alloy as pre-catalysts boost direct seawater oxygen evolution. Appl Catal B-environ Energy 234:2123376
12. Chu F, He JH, Wang JZ et al (2025) Medium-entropy alloy design enables highly efficient catalytic methanolysis of ammonia borane. Appl Catal B-environ Energy 368:12514010.1016/j.apcatb.2025.125140 ↗
13. Tajuddin AH, Wakisaka M, Ohto T et al (2023) Corrosion-resistant and high-entropic non-noble-metal electrodes for oxygen evolution in acidic media. Adv Mater 35:220746610.1002/adma.202207466 ↗
14. Long MR, Lai SY, Miao KH et al (2025) IrPdCuFeNiCoMo based core-shell icosahedron nanocrystals and nanocages for efficient and robust acidic oxygen evolution. Angew Chem Int Ed 64:e20241995610.1002/anie.202419956 ↗
15. Kobayshi T, Chida Y, Todoroki N et al (2024) Enhanced oxygen reduction reaction activity on the melamine-modified Pt-high-entropy alloy single-crystal lattice stacking surface. ACS Catal 14:11512–1152110.1021/acscatal.4c02191 ↗
16. Maulana AL, Han S, Shan Y et al (2025) Stabilizing Ru in multicomponent alloy as acidic oxygen evolution catalysts with machine learning-enabled structural insights and screening. J Am Chem Soc 147:10268–1027810.1021/jacs.4c16638 ↗
17. Wang XY, Xu XQ, Nie Y et al (2023) Electronic-state modulation of metallic Co-sssisted Co7Fe3 alloy heterostructure for highly efficient and stable overall water splitting. Adv Sci 10:230196110.1002/advs.202301961 ↗
18. Zhu TR, Zhao R, Xu YT et al (2025) Anion vacancies coupling with heterostructures enable advanced aerogel cathode for ultrafast aqueous zinc-ion storage. Adv Mater 37:241958210.1002/adma.202419582 ↗
19. Long H, Qian YX, Gang SF et al (2025) High-Performance thermoelectric composite of Bi2Te3 nanosheets and carbon aerogel for harvesting of environmental electromagnetic energy. ACS Nano 19:1819–183110.1021/acsnano.4c16834 ↗
20. Xiao RF, Zhou XY, Yang TT et al (20205) Biomimetic gradient aerogel fibers for sustainable energy harvesting from human sweat via the hydrovoltaic effect. Nano Energy 13:6110759
21. Espinosa-Lagunes FI, Martínez-Lázaro A, Luna-Bárcenas G et al (2025) FeNiCo aerogel for oxygen evolution reaction in alkaline systems: microfluidic and anion exchange membrane electrolyzers. Renew Energy 245:12279110.1016/j.renene.2025.122791 ↗
22. Liu L, Huang HZ, Tai JX et al (2025) The catalytic activity of reduced graphene aerogel anchored with CoFe2O4 spinel via self-assembly technique for enhanced oxygen evolution reaction. Carbon 219:11884710.1016/j.carbon.2024.118847 ↗
23. Xin YM, Hua QQ, Li CJ et al (2024) Enhancing electrochemical performance and corrosion resistance of nickel-based catalysts in seawater electrolysis: focusing on OER and HER. J Mater Chem A 12:23147–2317810.1039/D4TA03393K ↗
24. Osmieri L, Yu HR, Hermann RP et al (2024) Aerogel-derived nickel-iron oxide catalysts for oxygen evolution reaction in alkaline media. Appl Catal B Environ Energy 348:12384310.1016/j.apcatb.2024.123843 ↗
25. Nairan A, Feng Z, Zheng RM et al (2024) Engineering metallic alloy electrode for robust and active water electrocatalysis with large current density exceeding 2000 mA cm– 2. Adv Mater 36:240144810.1002/adma.202401448 ↗
26. Kumar A, Gil-Sepulcre M, Lee JS et al (2024) Iridium single-atom-ensembles stabilized on Mn-substituted spinel oxide for durable acidic water electrolysis. Adv Mater 36:240164810.1002/adma.202401648 ↗
27. Wetzel A, Morell D, von der Au M et al (2024) Transpassive metal dissolution vs. oxygen evolution reaction: implication for alloy stability and electrocatalysis. Angew Chem Int Ed 63:e20231705810.1002/anie.202317058 ↗
28. Du YX, Liu D, Du R et al (2025) Sub-1 Nm nanowire aerogels. Adv Funct Mater 35:241365110.1002/adfm.202413651 ↗
29. Chen XF, Wang Q, Cheng ZY et al (2021) Direct observation of chemical short-range order in a medium-entropy alloy. Nature 592:712–71610.1038/s41586-021-03428-z ↗
30. Kim J, Kim MC, Han SS et al (2024) Accessible Ni-Fe-oxalate framework for electrochemical Urea oxidation with radically enhanced kinetics. Adv Funct Mater 36:231562510.1002/adfm.202315625 ↗
31. Zuo SW, Wu ZP, Zhang GK et al (2024) Correlating structural disorder in metal (Oxy) hydroxides and catalytic activity in electrocatalytic oxygen evolution. Angew Chem Int Ed 63:e20231676210.1002/anie.202316762 ↗
32. Huang HG, Chen C, Chang C, Cet al (2024) Crystal-phase-engineered high-entropy alloy aerogels for enhanced ethylamine electrosynthesis from acetonitrile. Adv Mater 36:231414210.1002/adma.202314142 ↗
33. Li XM, Xie ZK, Roy S et al (2025) Amorphous high-entropy phosphidenanosheets with multi-atom catalytic sites for efficient oxygen evolution. Adv Mater 37:241029510.1002/adma.202410295 ↗
34. Li HF, Quan Q, Dong HL et al (2025) Hierarchical spin-polarized nanosheet array for boosting ampere-level water oxidation under magnetic field. Adv Funct Mater 35:242081010.1002/adfm.202420810 ↗
35. Aniskevich Y, Yu JH, Kim JY et al (2024) Tracking sodium cluster dynamics in hard carbon with a low specific surface area for sodium-ion batteries. Adv Energy Mater 14:230430010.1002/aenm.202304300 ↗
36. Liu Q, Wu DL, Wang T et al (2024) Pre-Oxidating and pre‐carbonizing to regulate the composition and structure of coal Tar pitch: the fabrication of porous carbon for supercapacitor applications. Adv Funct Mater 34:240055610.1002/adfm.202400556 ↗
37. Guan SQ, Xu BE, Yu XB et al (2024) Activation of lattice oxygen in nitrogen-doped high-entropy oxide nanosheets for highly efficient oxygen evolution reaction. ACS Catal 14:17806–1781710.1021/acscatal.4c05997 ↗
38. Yang X, Cheng J, Xu Y et al (2023) Heterogeneous ultra-thin FeCo-LDH@Co(OH)2 nanosheets facilitated electrons transfer for oxygen evolution reaction. Chem Eng J 472:14507610.1016/j.cej.2023.145076 ↗
39. Lang XK, Jia YZ, Fang Q et al (2025) Engineering CuIn microenvironment for efficient acidic electrochemical CO2 reduction to CO. Appl Catal B Environ Energy 371:12524410.1016/j.apcatb.2025.125244 ↗
40. Xie YH, Feng YM, Pan SY et al (2025) Electrochemical leaching of Ni dopants in IrRu alloy electrocatalyst boosts overall water splitting. Adv Funct Mater 34:240635110.1002/adfm.202406351 ↗
41. Demeyere T, Ellaby T, Sarwar M et al (2025) Bridging oxide thermodynamics and site-blocking: a computational study of ORR activity on platinum nanoparticles. ACS Catal 15:5674–568210.1021/acscatal.5c00321 ↗
42. Antony RP, Cechanaviciute IA, Quast T et al (2024) Deep reconstruction of Mo-based OER pre-catalysts in water electrolysis at high current densities. Chemcatchem 16:e20230102310.1002/cctc.202301023 ↗
43. Xiao LY, Bai X, Han JY et al (2023) Surface reconstruction and structural transformation of two-dimensional Ni-Fe MOFs for oxygen evolution in seawater media. Nano Res 17:2429–243710.1007/s12274-023-6088-x ↗
44. Xu ZZ, Meng M, Zhou G et al (2024) Half-metallization atom-fingerprints achieved at ultrafast oxygen-evaporated pyrochlores for acidic water oxidation. Adv Mater 36:240478710.1002/adma.202404787 ↗
45. Hou ZQ, Cui CH, Li YN et al (2023) Lattice-strain engineering for heterogenous electrocatalytic oxygen evolution reaction. Adv Mater 35:220987610.1002/adma.202209876 ↗
46. Zhang T, Zhao HF, Chen ZJ et al (2025) High-entropy alloy enables multi-path electron synergism and lattice oxygen activation for enhanced oxygen evolution activity. Nat Commun 16:332710.1038/s41467-025-58648-y ↗
47. Antink WH, Lee S, Lee HS et al (2024) High-valence metal-driven electronic modulation for boosting oxygen evolution reaction in high-entropy spinel oxide. Adv Funct Mater 34:230943810.1002/adfm.202309438 ↗
48. Zheng YJ, Geng W, Xiao ST et al (2024) Inside cover: interfacial Ir-V direct metal bonding enhanced hydrogen evolution activity in vanadium oxides supported catalysts. Angew Chem Int Edit 63:e20241279910.1002/anie.202412799 ↗
49. Chen ZW, Li J, Ou P et al (2024) Unusual sabatier principle on high entropy alloy catalysts for hydrogen evolution reactions. Nat Commun 15:35910.1038/s41467-023-44261-4 ↗
50. Yuan K, Zheng YL, Zhao YH et al (2025) Bimetallic self-supported AuCu alloy aerogel with abundant diffusion channels for regulating oxygen reduction reaction by electronic structure modulation for zinc-air battery application. Chem Eng J 505:15993010.1016/j.cej.2025.159930 ↗