3-D atomic Imaging of Catalyst Nanoparticles

• Applicant: Professorin Tong Li, Ph.D.
• Subject Area: Synthesis and Properties of Functional Materials
• Term: from 2018 to 2023
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 407513992

• Final Report Year: 2023

Final Report Abstract

Electrocatalytic water splitting provides a clean and affordable way to produce hydrogen, an essential chemical fuel in sustainable energy conversion/storage devices such as fuel cells. The noble metal-based electrocatalysts and Co-based oxides are promising for electrocatalytic reactions such as oxygen reduction (ORR) and oxygen evolution reactions (OER). However, the effects of the operating environment on the surface composition, structure, and stability of the noble metal catalysts are poorly understood at the atomic scale. This knowledge will be required to produce improved catalysts for future energy- and materials-efficient technologies. However, identifying the individual atoms' chemical nature and 3D location is a notorious challenge for conventional surface techniques, chemical spectroscopy, and electron microscopy. Atom probe tomography (APT) provides uniquely powerful insights into the atomic-scale chemistry and structure of materials in three dimensions (3D). In the proposed project, the applicant has employed atom probe tomography to produce atomic-scale data to establish structuresynthesis-performance relationships. In addition, the applicant developed a new multimodal approach by combining APT with high-resolution transmission electron microscopy (HRTEM), X-ray photoemission spectroscopy, and electrochemical measurements to shed light on the surface state change of the electrocatalysts during OER, whereby pronounced compositional and structural changes take place that can dramatically affect the activity and stability. New approaches to improve the sample preparation were developed to enhance the quality of the APT data obtained. The obtained atomic-scale information was closely correlated to activity and stability to elucidate reaction or degradation mechanisms, which will provide a rational guide to nano-engineering catalysts to develop cost-effective and high efficiency sustainable energy sources.

Publications

• Acidity enhancement through synergy of penta-and tetra-coordinated aluminum species in amorphous silica networks. Nature Communications, 11(1).
  Wang, Zichun; Li, Tong; Jiang, Yijiao; Lafon, Olivier; Liu, Zongwen; Trébosc, Julien; Baiker, Alfons; Amoureux, Jean-Paul & Huang, Jun
  
• Insights into the Formation, Chemical Stability, and Activity of Transient NiyP@NiOx Core–Shell Heterostructures for the Oxygen Evolution Reaction. ACS Applied Energy Materials, 3(3), 2304-2309.
  Wilde, Patrick; Dieckhöfer, Stefan; Quast, Thomas; Xiang, Weikai; Bhatt, Anjali; Chen, Yen-Ting; Seisel, Sabine; Barwe, Stefan; Andronescu, Corina; Li, Tong; Schuhmann, Wolfgang & Masa, Justus
  
• Atom probe tomography. Nature Reviews Methods Primers, 1(1).
  Gault, Baptiste; Chiaramonti, Ann; Cojocaru-Mirédin, Oana; Stender, Patrick; Dubosq, Renelle; Freysoldt, Christoph; Makineni, Surendra Kumar; Li, Tong; Moody, Michael & Cairney, Julie M.
  
• Atomic‐Precision Tailoring of Au–Ag Core–Shell Composite Nanoparticles for Direct Electrochemical‐Plasmonic Hydrogen Evolution in Water Splitting. Advanced Functional Materials, 31(30).
  Mo, Jiaying; Barbosa, Eduardo C. M.; Wu, Simson; Li, Yiyang; Sun, Yuancheng; Xiang, Weikai; Li, Tong; Pu, Shengda; Robertson, Alex; Wu, Tai‐sing; Soo, Yun‐liang; Alves, Tiago V.; Camargo, Pedro H. C.; Kuo, Winson & Tsang, Shik Chi Edman
  
• Rapid Interchangeable Hydrogen, Hydride, and Proton Species at the Interface of Transition Metal Atom on Oxide Surface. Journal of the American Chemical Society, 143(24), 9105-9112.
  Wu, Simson; Tseng, Kai-Yu; Kato, Ryuichi; Wu, Tai-Sing; Large, Alexander; Peng, Yung-Kang; Xiang, Weikai; Fang, Huihuang; Mo, Jiaying; Wilkinson, Ian; Soo, Yun-Liang; Held, Georg; Suenaga, Kazu; Li, Tong; Chen, Hsin-Yi Tiffany & Tsang, Shik Chi Edman
  
• Raw data. figshare. Figure
  W. Xiang; N. Yang; X. Li; J. Linnemann; U. Hagemann; O. Ruediger; M. Heidelmann; T. Falk; M. Aramini; S. DeBeer; M. Muhler; K. Tschulik & T. Li
  
• Sintering Activated Atomic Palladium Catalysts with High-Temperature Tolerance of ∼1,000°C. Cell Reports Physical Science, 2(1), 100287.
  Yang, Nating; Zhao, Yonghui; Zhang, Hao; Xiang, Weikai; Sun, Yuhan; Yang, Shuai; Sun, Yu; Zeng, Gaofeng; Kato, Kenichi; Li, Xiaopeng; Yamauchi, Miho; Jiang, Zheng & Li, Tong
  
• 3D atomic-scale imaging of mixed Co-Fe spinel oxide nanoparticles during oxygen evolution reaction. Nature Communications, 13(1).
  Xiang, Weikai; Yang, Nating; Li, Xiaopeng; Linnemann, Julia; Hagemann, Ulrich; Ruediger, Olaf; Heidelmann, Markus; Falk, Tobias; Aramini, Matteo; DeBeer, Serena; Muhler, Martin; Tschulik, Kristina & Li, Tong
  
• Atomic-scale characterization of (electro-)catalysts and battery materials by atom probe tomography. Cell Reports Physical Science, 3(12), 101188.
  Li, Tong; Devaraj, Arun & Kruse, Norbert