Spontaneous‐Spin‐Polarized 2D π‐d Conjugated Frameworks Towards Enhanced Oxygen Evolution Kinetics

Author:

Lee Won Seok1,Maeda Hiroaki2,Kuo Yen‐Ting3,Muraoka Koki4,Fukui Naoya2,Takada Kenji2,Sasaki Sono56,Masunaga Hiroyasu7,Nakayama Akira4,Tian Hong‐Kang38ORCID,Nishihara Hiroshi2ORCID,Sakaushi Ken1ORCID

Affiliation:

1. Research Center for Energy and Environmental Materials National Institute for Materials Science 1‐1 Namiki Tsukuba Ibaraki 305‐0044 Japan

2. Research Institute for Science and Technology Tokyo University of Science 2641 Yamazaki Noda Chiba 278–8510 Japan

3. Department of Chemical Engineering National Cheng Kung University Tainan 70101 Taiwan

4. Department of Chemical System Engineering The University of Tokyo 7‐3‐1 Hongo, Bunkyo‐ku Tokyo 113–8656 Japan

5. Faculty of Fiber Science and Engineering Kyoto Institute of Technology Matsugasaki Hashikami‐cho 1 Sakyo‐ku Kyoto 606–8585 Japan

6. SPring‐8 Center RIKEN Kouto 1‐1‐1, Sayo‐cho, Sayo‐gun Hyogo 679–5148 Japan

7. Japan Synchrotron Radiation Research Institute (JASRI) 1‐1‐1 Kouto, Sayo‐cho Sayo‐gun Hyogo 679–5198 Japan

8. Hierarchical Green‐Energy Materials (Hi‐GEM) Research Center National Cheng Kung University Tainan 70101 Taiwan

Abstract

AbstractAlternative strategies to design sustainable‐element‐based electrocatalysts enhancing oxygen evolution reaction (OER) kinetics are demanded to develop affordable yet high‐performance water‐electrolyzers for green hydrogen production. Here, it is demonstrated that the spontaneous‐spin‐polarized 2D π‐d conjugated framework comprising abundant elements of nickel and iron with a ratio of Ni:Fe = 1:4 with benzenehexathiol linker (BHT) can improve OER kinetics by its unique electronic property. Among the bimetallic NiFex:y‐BHTs with various ratios with Ni:Fe = x:y, the NiFe1:4‐BHT exhibits the highest OER activity. The NiFe1:4‐BHT shows a specific current density of 140 A g−1 at the overpotential of 350 mV. This performance is one of the best activities among state‐of‐the‐art non‐precious OER electrocatalysts and even comparable to that of the platinum‐group‐metals of RuO2 and IrO2. The density functional theory calculations uncover that introducing Ni into the homometallic Fe‐BHT (e.g., Ni:Fe = 0:1) can emerge a spontaneous‐spin‐polarized state. Thus, this material can achieve improved OER kinetics with spin‐polarization which previously required external magnetic fields. This work shows that a rational design of 2D π‐d conjugated frameworks can be a powerful strategy to synthesize promising electrocatalysts with abundant elements for a wide spectrum of next‐generation energy devices.

Funder

Ministry of Education, Culture, Sports, Science and Technology

National Science and Technology Council

Japan Society for the Promotion of Science

Publisher

Wiley

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