In-situ Pt reduction induced topological transformation of NiFe-MOF for industrial seawater splitting

doi:10.1016/S1872-2067(24)60271-8

Chinese Journal of Catalysis ›› 2025, Vol. 72: 211-221.DOI: 10.1016/S1872-2067(24)60271-8

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In-situ Pt reduction induced topological transformation of NiFe-MOF for industrial seawater splitting

Guohao Na^a^,¹, Hongshun Zheng^a^,¹, Mingpeng Chen^a^,^*(), Huachuan Sun^a, Yuewen Wu^a, Dequan Li^a, Yun Chen^a, Boran Zhao^a, Bo Zhao^a, Tong Zhou^a, Tianwei He^a, Yuxiao Zhang^a, Jianhong Zhao^a, Yumin Zhang^a, Jin Zhang^a, Feng Liu^a, Hao Cui^a, Qingju Liu^a^,^*()

^aYunnan Key Laboratory for Micro/Nano Materials & Technology, National Center for International Research on Photoelectric and Energy Materials, School of Materials and Energy, Yunnan University, Kunming 650091, Yunnan, China
^bYunnan Precious Metals Laboratory Co., Ltd., Kunming 650106, Yunnan, China

Received:2024-12-03 Accepted:2025-02-03 Online:2025-05-18 Published:2025-05-20
Contact: *E-mail: mpchen@ynu.edu.cn (M. Chen), qjliu@ynu.edu.cn (Q. Liu).
About author:¹Contributed equally to this work.
Supported by:
National Key Research and Development Program of China(2022YFB3803600);National Natural Science Foundation of China(22368050);National Natural Science Foundation of China(22378346);Key Research and Development Program of Yunnan Province(202302AF080002);Yunnan Basic Applied Research Project(202401AU070229);Yunnan Basic Applied Research Project(202401AT070460);Scientific Research Fund Project of Yunnan Education Department(2024J0013);Scientific Research Fund Project of Yunnan Education Department(2024J0014);Scientific and Technological Project of Yunnan Precious Metals Laboratory(YPML-20240502008);Scientific and Technological Project of Yunnan Precious Metals Laboratory(YPML-2023050259);Scientific and Technological Project of Yunnan Precious Metals Laboratory(YPML-2023050260);Science and Technology Projects of Universities Serving Key Industries in Yunnan Province(FWCY-BSPY2024023);Yunnan Provincial Department of Education Scientific Research Fund-supported project and Yunnan University Graduate Research Innovation Fund-supported project(KC-24248426)

Abstract

Abstract:

Metal-support interaction (MSI) is regarded as an indispensable manner to stabilize active metals and modulate catalytic activity, which shows great potentials in developing of efficient hydrogen evolution reaction (HER) electrode with high activity and strong robustness. Herein, this work presents a novel heterostructure with ultrafine platinum quantum dots (Pt QDs) on defective catalytic supports derived from metal-organic frameworks (MOFs). It is indicated substantial oxygen vacancies can be generated and Pt-Pt bonds can be optimized through topological transformation. The resulting Pt/T-NiFe-BDC (BDC: C₈H₆O₄) exhibits competitive HER activity in alkaline seawater, attaining ultralow overpotentials of 158 and 266 mV at 500 and 1000 mA cm^-2 with fast kinetics and outstanding stability. An asymmetric water electrolyzer using Pt/T-NiFe-BDC as a cathode only requires a voltage of 1.89 V to generate an industrial density of 1000 mA cm^-2 and shows no attenuation in 500-h continuous test at 500 mA cm^-2. Theoretical calculations and in-situ spectroscopic analysis reveal the reversible hydrogen spillover mechanism, in which oxygen vacancies facilitate the sluggish water dissociation and Pt QDs promote the H* combination. This study provides a new paradigm to engineer metal-supported catalysts for efficient and robust seawater splitting.

Key words: Seawater splitting, Hydrogen evolution reaction, Topological transformation, Metal support interaction, Reversible hydrogen spillover

Guohao Na, Hongshun Zheng, Mingpeng Chen, Huachuan Sun, Yuewen Wu, Dequan Li, Yun Chen, Boran Zhao, Bo Zhao, Tong Zhou, Tianwei He, Yuxiao Zhang, Jianhong Zhao, Yumin Zhang, Jin Zhang, Feng Liu, Hao Cui, Qingju Liu. In-situ Pt reduction induced topological transformation of NiFe-MOF for industrial seawater splitting[J]. Chinese Journal of Catalysis, 2025, 72: 211-221.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(24)60271-8

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Figures/Tables 6

Fig. 1. Schematic illustration of the synthetic procedure of Pt/T-NiFe-BDC.

Fig. 2. (a) SEM image of NiFe-BDC. SEM (b), TEM (c), HAADF-STEM (d,e) images of Pt/T-NiFe-BDC. (f) Size distribution of Pt QDs. (g) EDS elemental mapping images of Pt, O, Fe, and Ni.

Fig. 3. (a) EPR spectra of NiFe-BDC, Pt/T-NiFe-BDC, Pt/NiFe-LDH and Pt/NiFe-BDC. High-resolution XPS spectra of O 1s (b), Fe 2p (c), Ni 2p (d). Pt L3-edge XANES spectra (e), R-space spectra (f), and k2-weighted wavelet transforms (WT) (g) of Pt/T-NiFe-BDC, Pt/NiFe-LDH, Pt foil, and PtO2.

Fig. 4. HER Performance. LSV curves (a), comprehensive comparisons of HER performance (b), and Tafel plots (c) of Pt/T-NiFe-BDC, Pt/NiFe-LDH, Pt/NiFe-BDC and Pt/C in 1 mol L-1 KOH. LSV curves (d) and Tafel plots (e) of the as-prepared catalysts in alkaline seawater. (f) Stability test at 500 mA cm-2. (g) Comparison of the overpotentials for HER in alkaline seawater.

Fig. 5. LSV curves (a) and comprehensive comparisons (b) of NiFe-BDC, NiFe-LDH, RuO2 and NF in 1 mol L-1 KOH for OER. (c) Polarization curves of NiFe-BDC and NiFe-LDH in alkaline water/seawater. Cell voltage curves (d) and long-term stability test (e) of Pt/T-NiFe-BDC||NiFe-BDC at 500 mA cm-2 in alkaline seawater. (f) Comparison of cell voltages between Pt/T-NiFe-BDC||NiFe-BDC and recently reported electrolyzer.

Fig. 6. (a) Top view of Pt/T-NiFe-BDC (atoms in orange, green, gray, red and white represent Fe, Ni, Pt, O and H, respectively). (b) The calculated PDOS of Pt QDs in Pt/T-NiFe-BDC and Pt-NiFe-LDH. (c) Relative energies of the HER process on Pt/T-NiFe-BDC-Ov, Pt/T-NiFe-BDC-PtQD and Pt/NiFe-LDH- PtQD in alkaline media. (d) Corresponding illustrations of the HER process on Pt/T-NiFe-BDC-OV in alkaline media. In-situ Raman spectra of Pt/T-NiFe-BDC (e) and Pt/NiFe-LDH (f). (g) The positions and ratios of ??3 peaks at various potentials.

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In-situ Pt reduction induced topological transformation of NiFe-MOF for industrial seawater splitting

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