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Peer-reviewedCC BYAdvanced Science

Metal‐Support Interaction Triggered Electronic Reconstruction in Pd/CoN‐Co 4 N Catalysts for Optimizing MEK Oxidation and Poisoning Resistance

4 affiliations
  1. 1Shaanxi Key Laboratory of Liquid Crystal Polymer Intelligent Display Technological Institute of Materials & Energy Science (TIMES) Xijing University Xi'an P. R. China
  2. 2State Key Laboratory of Multiphase Flow in Power Engineering School of Energy and Power Engineering Xi'an Jiaotong University Xi'an Shaanxi P. R. China
  3. 3College of Engineering Xi'an International University Xi'an P. R. China
  4. 4National Engineering Laboratory for VOCs Pollution Control Material & Technology University of Chinese Academy of Sciences Beijing P. R. China

Abstract

The development of noble metal catalysts integrating high activity with strong poisoning resistance remains highly desirable yet challenging. Herein, the metallic electron‐donating property of a cobalt nitride support is leveraged to enhance the electron metal‐support interaction (EMSI) with Pd, concurrently improving the activity and poisoning resistance of Pd/CoN‐Co 4 N in methyl ethyl ketone (MEK) oxidation. Over which, 90% of MEK is oxidized at ca . 172 °C by Pd/CoN‐Co 4 N, versus only 48% conversion over Pd/Co 3 O 4 . Crucially, Pd/CoN‐Co 4 N exhibits exceptional resistance to H 2 S and 1,2‐dichloroethane poisoning, with performance showing almost no degradation upon H 2 S exposure, which completely deactivates Pd/Co 3 O 4 . The strong EMSI induces a profound electronic redistribution, facilitating electron transfer from the support to Pd and generating electron‐rich Pd 0 in situ . This modulates the Pd d ‐band center toward the Fermi level, enhancing MEK and O 2 adsorption/activation and promoting deep oxidation of carboxylate intermediates. Furthermore, the enhanced EMSI creates abundant Lewis acid sites by modulating the charge density of Co atoms. These sites serve as sacrificial adsorption sites for electron‐rich poison molecules, thus shielding the Pd sites and facilitating rapid contaminant desorption. This work provides atomic‐level insight into EMSI on non‐oxide supports and proposes a design principle for robust catalysts toward environmental purification.

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BibTeX
@article{wang2026metalsupport,
  title = {{Metal‐Support Interaction Triggered Electronic Reconstruction in Pd/CoN‐Co 4 N Catalysts for Optimizing MEK Oxidation and Poisoning Resistance}},
  author = {Yadi Wang and Chaoqian Ai and Cai Wang and Zeyu Jiang and Jialei Wan and Jingjing Wang and Xiangbo Feng and Chi He},
  journal = {Advanced Science},
  year = {2026},
  month = jun,
  doi = {10.1002/advs.75899},
  url = {https://doi.org/10.1002/advs.75899},
  note = {CC BY},
}
RIS
TY  - JOUR
TI  - Metal‐Support Interaction Triggered Electronic Reconstruction in Pd/CoN‐Co 4 N Catalysts for Optimizing MEK Oxidation and Poisoning Resistance
AU  - Yadi Wang
AU  - Chaoqian Ai
AU  - Cai Wang
AU  - Zeyu Jiang
AU  - Jialei Wan
AU  - Jingjing Wang
AU  - Xiangbo Feng
AU  - Chi He
PY  - 2026
DA  - 2026/06/02
JO  - Advanced Science
DO  - 10.1002/advs.75899
UR  - https://doi.org/10.1002/advs.75899
AB  - The development of noble metal catalysts integrating high activity with strong poisoning resistance remains highly desirable yet challenging. Herein, the metallic electron‐donating property of a cobalt nitride support is leveraged to enhance the electron metal‐support interaction (EMSI) with Pd, concurrently improving the activity and poisoning resistance of Pd/CoN‐Co 4 N in methyl ethyl ketone (MEK) oxidation. Over which, 90% of MEK is oxidized at ca . 172 °C by Pd/CoN‐Co 4 N, versus only 48% conversion over Pd/Co 3 O 4 . Crucially, Pd/CoN‐Co 4 N exhibits exceptional resistance to H 2 S and 1,2‐dichloroethane poisoning, with performance showing almost no degradation upon H 2 S exposure, which completely deactivates Pd/Co 3 O 4 . The strong EMSI induces a profound electronic redistribution, facilitating electron transfer from the support to Pd and generating electron‐rich Pd 0 in situ . This modulates the Pd d ‐band center toward the Fermi level, enhancing MEK and O 2 adsorption/activation and promoting deep oxidation of carboxylate intermediates. Furthermore, the enhanced EMSI creates abundant Lewis acid sites by modulating the charge density of Co atoms. These sites serve as sacrificial adsorption sites for electron‐rich poison molecules, thus shielding the Pd sites and facilitating rapid contaminant desorption. This work provides atomic‐level insight into EMSI on non‐oxide supports and proposes a design principle for robust catalysts toward environmental purification.
SN  - 2198-3844
ER  -