Dual-Molten-Salt Etching Strategy Enables Built-in Electric Field in Mo-MXene/NiFeSe Heterostructure for Superior OER Performance

Abstract

Transition metal selenides have emerged as potential catalysts for the oxygen evolution reaction, yet their practical implementation faces two fundamental challenges: irreversible nanoparticle aggregation under operational conditions and unfavorable adsorption energetics for critical oxygen intermediates. Herein, a strategy that integrates dual-molten-salt etching with hydrothermal selenization has been developed to tightly anchor FeNiSe nanoparticles onto a porous Mo-based MXene substrate (Mo-MXene/NiFeSe). The hierarchical porous architecture of Mo-MXene/NiFeSe facilitates rapid mass and charge transport. The NiFeSe nanoparticles are chemically anchored within the conductive Mo-MXene matrix via in-situ formed Mo–O–Fe/Ni bonds, effectively preventing agglomeration during the catalytic process. Additionally, the work function gradient between Mo-MXene and NiFeSe induces charge redistribution, creating a built-in electric field that optimizes intermediate adsorption kinetics and enhances charge transport efficiency. Therefore, Mo-MXene/NiFeSe achieves an ultralow overpotential of 231 mV to reach current density of 10 mA cm⁻² and sustain 91% of its initial current density over 55 h in alkaline electrolyte. Density functional theory (DFT) calculations reveal that the adsorption free energy of *OOH for Mo-MXene/NiFeSe is significantly reduced, effectively lowering the kinetic barrier of the rate-determining step. This work provides both fundamental insights into built-in electric field-enhanced catalysis and a practical strategy for developing high-performance and durable oxygen evolution reaction electrocatalysts.

Keywords

built-in electric field / dual-molten-salt etching / Mo-MXene / oxygen evolution reaction / transition metal selenides

References

[1] Z. J. Zhang, N. Yu, Y. L. Dong, G. Q. Han, H. Hu, Y. M. Chai, B. Dong, Chem. Eng. J. 2024, 498, 155736.

[2] X. J. Zeng, Q. Q. Zhang, C. L. Jin, H. Huang, Y. F. Gao, Energy Environ. Mater. 2024, 7, e12628.

[3] D. Ontiveros, S. Vela, F. Viñes, C. Sousa, Energy Environ. Mater. 2024, 7, e12774.

[4] X. J. Zeng, Y. N. Tan, L. Xia, Q. Q. Zhang, G. D. Stucky, Chem. Commun. 2023, 59, 880.

[5] Q. Q. Zhang, X. J. Zeng, Z. L. Zhang, C. L. Jin, Y. Y. Cui, Y. F. Gao, J. Colloid Interface Sci. 2024, 675, 357.

[6] A. Farhan, W. Qayyum, U. Fatima, S. Nawaz, A. Balčiūnaitė, T. H. Kim, V. Srivastava, J. Vakros, Z. Frontistis, G. Boczkaj, Small 2024, 20, 2402015.

[7] W. Ou, X. Ye, Y. H. Zhou, Coord. Chem. Rev. 2023, 493, 215274.

[8] P. Wang, S. Q. Zhang, Z. B. Wang, Y. H. Mo, X. Y. Luo, F. Yang, M. L. Lv, Z. X. Li, X. W. Liu, J. Mater. Chem. A 2023, 11, 5476.

[9] E. Sadeghi, S. Chamani, N. S. Peighambardoust, U. Aydemir, Energy Environ. Mater. 2025, 8, e12873.

[10] L. Chen, Y. Luo, Z. P. Yu, Y. K. Cheng, Y. Zheng, L. He, J. H. Xiong, W. W. Kong, Tungsten 2024, 6, 859.

[11] X. J. Zeng, D. R. Duan, X. F. Zhang, X. H. Li, K. Li, R. H. Yu, M. Moskovits, J. Mater. Chem. C 2022, 10, 4140.

[12] Y. T. Deng, S. T. Xiao, Y. J. Zheng, X. Rong, M. R. Bai, Y. J. Tang, T. Ma, C. Cheng, C. S. Zhao, Chem. Eng. J. 2023, 451, 138514.

[13] J. Han, M. M. Bai, T. T. Ai, W. W. Bao, X. L. Wei, X. Y. Zou, Z. F. Deng, Y. Wang, W. H. Li, J. G. Hou, L. J. Kou, Rare Metals 2025, 44, 1096.

[14] H. M. Wang, Y. H. Wei, G. C. Wang, Y. R. Pu, L. Yuan, C. Liu, Q. Wang, Y. Zhang, H. Wu, Adv. Sci. 2022, 9, 2201823.

[15] W. X. Chen, W. Wei, F. Li, Y. J. Wang, M. Liu, S. Dong, J. H. Cui, Y. Y. Zhang, R. Wang, K. Ostrikov, S. Q. Zang, Adv. Funct. Mater. 2024, 34, 2310690.

[16] J. Yu, R. Ran, Y. J. Zhou, M. Ni, Z. P. Shao, Energy Environ. Mater. 2020, 3, 121.

[17] Y. Li, M. S. Hassan, X. Zhao, A. L. Rogach, Adv. Mater. 2025, 37, 2418146.

[18] L. Zeng, L. Ana, Z. J. Zhang, J. Zheng, W. X. Chen, C. Liu, Y. Y. Zheng, D. Dang, Z. Q. Liu, Chem. Eng. J. 2024, 491, 152084.

[19] L. Yan, Y. H. Chen, J. C. Xie, H. Li, Rare Metals 2025, 44, 1067.

[20] X. J. Zeng, X. Jiang, Y. Ning, F. Y. Hu, B. B. Fan, J. Adv. Ceram. 2023, 12, 1562.

[21] X. Jiang, Y. N. Tan, S. A. Cheng, X. J. Zeng, Nano Res. 2025, 18, 94907512.

[22] X. J. Zeng, Y. F. Ye, Y. Q. Wang, R. H. Yub, M. Moskovitsc, G. D. Stucky, J. Adv. Ceram. 2023, 12, 553.

[23] F. Y. Hu, X. H. Wang, S. Bao, L. M. Song, S. Zhang, H. H. Niu, B. B. Fan, R. Zhang, H. X. Li, Chem. Eng. J. 2022, 440, 135855.

[24] Z. L. Zhang, T. Liang, C. L. Jin, S. Y. Zhang, Y. Y. Cui, J. X. Chen, X. J. Zeng, J. Mater. Chem. A 2024, 12, 14517.

[25] Q. X. Deng, M. Q. Wang, X. L. Liu, H. S. Fan, Y. F. Zhang, H. Y. Yang, J. Colloid Interface Sci. 2022, 626, 700.

[26] R. Z. Gu, T. Zhou, Z. H. Wang, Z. Chen, J. W. Tao, Z. W. Fan, L. Y. Guo, Y. S. Liu, Int. J. Hydrogen Energy 2023, 48, 27642.

[27] J. Zhang, S. Zhang, Z. H. Zhang, J. F. Wang, Z. H. Zhang, G. H. Cheng, J. Alloys Compd. 2023, 939, 168753.

[28] S. Liu, W. T. Cai, M. M. Jin, T. X. Zhang, Z. W. Zhang, Q. Z. Liu, X. J. Liu, X. B. Zhang, F. M. Wang, Adv. Funct. Mater. 2025, 35, 2421447.

[29] S. C. Zhang, C. H. Tan, R. P. Yan, X. F. Zou, F. L. Hu, Y. Mi, C. Yan, S. L. Zhao, Angew. Chem. Int. Ed. 2023, 62, e202302795.

[30] W. J. Zhang, L. Yang, Z. Li, G. Z. Nie, X. J. Cao, Z. Z. Fang, X. J. Wang, S. Ramakrishna, Y. Z. Long, L. F. Jiao, Angew. Chem. Int. Ed. 2024, 136, e202400888.

[31] J. C. Zhang, X. Y. Wang, F. X. Du, J. Y. Wu, S. F. Xiao, Y. R. Zhou, H. Wu, Z. H. Shao, W. T. Cai, Y. Y. Li, Small 2024, 20, 2400304.

[32] P. F. Huang, H. J. Ying, S. L. Zhang, Z. Zhang, W. Q. Han, Adv. Energy Mater. 2022, 12, 2202052.

[33] J. N. Hu, C. Y. Liang, J. D. Li, C. W. Lin, Y. J. Liang, H. Wang, X. Li, Q. L. Wang, D. W. Dong, Carbon 2023, 204, 136.

[34] T. Z. Zhang, L. B. Chang, X. F. Zhang, H. J. Wan, N. Liu, L. J. Zhou, X. Xiao, Nat. Commun. 2022, 13, 6731.

[35] X. L. Zhang, Z. W. Ni, X. X. Bai, H. T. Shen, Z. R. Wang, C. L. Wei, K. D. Tian, B. J. Xi, S. L. Xiong, J. K. Feng, Adv. Energy Mater. 2023, 13, 2301349.

[36] Y. F. He, D. D. Liu, Q. Su, B. Zhong, L. Xia, X. X. Huang, J. Mater. Sci. Technol. 2024, 179, 187.

[37] V. Kamysbayev, A. S. Filatov, H. C. Hu, X. Rui, F. Lagunas, D. Wang, R. F. Klie, D. V. Talapin, Science 2020, 369, 979.

[38] K. Q. Zhao, Y. X. Zhang, X. L. Zhang, F. Xing, Y. H. Zhang, Y. Feng, T. Zhou, ACS Appl. Nano Mater. 2024, 22, 25880.

[39] F. Y. Hu, F. Zhang, X. H. Wang, Y. Y. Li, H. L. Wang, R. Zhang, H. X. Li, B. B. Fan, J. Adv. Ceram. 2022, 11, 1466.

[40] Q. Xi, F. X. Xie, J. X. Liu, X. C. Zhang, J. C. Wang, Y. W. Wang, Y. F. Wang, H. F. Li, Z. B. Yu, Z. J. Sun, X. Jian, X. M. Gao, J. Ren, C. M. Fan, R. Li, Small 2023, 19, 2300717.

[41] X. J. Zeng, C. Zhao, Y. H. Yin, T. L. Nie, N. H. Xie, R. H. Yu, G. D. Stucky, Carbon 2022, 193, 26.

[42] Y. F. He, Q. Su, D. D. Liu, L. Xia, X. X. Huang, D. Lan, Y. N. Liu, Y. D. Huang, B. Zhong, Chem. Eng. J. 2024, 491, 152041.

[43] Y. Fan, X. Q. Hao, N. X. Yi, Z. L. Jin, Appl. Catal. Environ. 2024, 357, 124313.

[44] X. J. Zeng, C. Zhao, X. Jiang, R. H. Yu, R. C. Che, Small 2023, 19, 2303393.

[45] A. S. Wang, W. Y. Wang, J. C. Xu, A. Zhu, C. N. Zhao, M. Yu, G. L. Shi, J. G. Yan, S. H. Sun, W. C. Wang, Adv. Energy Mater. 2023, 13, 2302537.

[46] Z. H. Feng, C. L. Dai, P. Shi, X. F. Lei, X. W. Liu, Small 2024, 20, 15.

[47] L. Y. Xu, J. Ouyang, Z. X. Cheng, Y. Huan, Adv. Ceram. 2025, 46, 195.

[48] Y. J. Zhong, L. Q. Zhao, D. Q. Guan, Z. H. Wang, H. W. Wu, J. Y. Liu, Z. P. Shao, Natl. Sci. Rev. 2025, 12, nwaf226.

[49] J. Wu, X. H. Gao, Z. W. Chen, Chem. Eng. J. 2024, 492, 152241.

[50] S. W. Tang, S. A. Cheng, C. Yu, Z. M. Wu, Y. N. Tan, X. J. Zeng, Sci. China Mater. 2025,

[51] Y. J. Zhong, X. M. Liu, P. Y. Liu, R. Ran, S. P. Jiang, H. W. Wu, Z. P. Shao, Adv. Energy Mater. 2020, 10, 2002992.

RIGHTS & PERMISSIONS

2026 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.