Stable Metal–Organic Electrocatalysts for Anion-Exchange Membrane Water Electrolyzers by Defect Engineering
Developing efficient and durable catalysts for the alkaline oxygen evolution reaction (OER) is vital to achieving practical anion-exchange membrane water electrolyzers (AEMWEs) for green hydrogen production. Here, we break the activity-stability trade-off of electrocatalysis by defect engineering of Ni-based metal-organic electrocatalysts (Ni-benzenedicarboxylate; Ni-BDC) through coordinating ferrocenecarboxylates (Fc) to the metal sites. Experimental results collectively reveal that the defect MOF (Ni-BDC:Fc_5:1) exhibits a high OER turnover frequency of 0.75 O<sub>2</sub> s<sup>-1</sup> at 300 mV overpotential. Operando Raman spectroscopy and isotope-labeling electrochemical mass spectrometry measurements indicate the structure of Ni-BDC:Fc_5:1 is also more stable in service than that of pure Ni-BDC. The high activity and stability could be attributed to the moderate defects (i.e., unsaturated Ni sites) in the structure that not only increase the intrinsic activity and stability of the local active environment by inhibiting lattice oxygen exchange but also electrochemically activate the bulk of the catalysts by creating a porous network that facilitates internal H<sub>2</sub>O/OH<sup>-</sup> conduction with enhanced electronic conduction. Accordingly, an AEMWE employing Ni-BDC:Fc_5:1 as the OER catalyst delivers an industrial-level current density of 1 A cm<sup>-2</sup> at 1.73 V<sub>cell</sub> and can be steadily operated for more than 120 h.
Authors
- Davide Menga
- Haldrian Iriawan (ORCID: https://orcid.org/0000-0002-2997-1180)
- Yuriy Román‐Leshkov (ORCID: https://orcid.org/0000-0002-0025-4233)
- Jen-Hung Fang (ORCID: https://orcid.org/0000-0001-8665-4088)
- Sunmoon Yu (ORCID: https://orcid.org/0000-0001-7250-9365)
- Hongbin Xu (ORCID: https://orcid.org/0009-0007-6311-475X)
- Junxiang Liu (ORCID: https://orcid.org/0000-0002-8256-1770)
- Tongchao Liu (ORCID: https://orcid.org/0000-0002-6010-3891)
- Xiao Wang (ORCID: https://orcid.org/0000-0003-1624-8230)
- Junghwa Kim (ORCID: https://orcid.org/0000-0002-2615-963X)
- Lena Schröck
- Jiaqi Wang (ORCID: https://orcid.org/0000-0003-1176-704X)
- Zhen Zhang (ORCID: https://orcid.org/0000-0001-6335-9529)
- Shuo Wang (ORCID: https://orcid.org/0000-0002-7907-9676)
- Yang Shao‐Horn (ORCID: https://orcid.org/0000-0001-8714-2121)
- Ju Li (ORCID: https://orcid.org/0000-0002-7841-8058)
- Sungsik Lee (ORCID: https://orcid.org/0000-0002-1425-9852)
- Yilin Zhang (ORCID: https://orcid.org/0000-0001-5390-4116)
- Daniel J. Zheng (ORCID: https://orcid.org/0000-0002-9471-6856)
- Guanzhou Zhu (ORCID: https://orcid.org/0000-0001-5671-9637)
- Ethan Yupeng Zheng (ORCID: https://orcid.org/0009-0007-5536-285X)
Institutions
- Eastern Institute of Technology (NZ)
- Argonne National Laboratory (US)
- University of Nottingham Ningbo China (CN)
- Dimagi (United States) (US)
- Ningbo Institute of Industrial Technology (CN)
- Advanced Photon Source
- Massachusetts Institute of Technology (US)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2025-08-11
- DOI
- https://doi.org/10.1021/jacs.5c06156
- Citations
- 18
- Primary Topic
- Electrocatalysts for Energy Conversion
- Type
- article
- Field-Weighted Citation Impact
- 6.54
Funders
- Massachusetts Institute of Technology
- Basic Energy Sciences