Plasma radicals control synthesis of platinum supported on nitrogen-doped graphitic carbon for ambient-pressure ammonia synthesis
12 affiliations
- 1Department of Chemical and Biomolecular Engineering, National University of Singapore, Singapore, Singapore
- 2Key Laboratory of Thermo-Fluid Science and Engineering of MOE, School of Energy and Power Engineering, Xi’an Jiaotong University, Xi’an, China
- 3Institute for Aqua Regeneration, Shinshu University, Nagano, Japan
- 4Wenzhou Key Laboratory of Novel Optoelectronic and Nano Materials, Institute of Wenzhou, Zhejiang University, Wenzhou, China
- 5CSIRO Energy, Clayton South, VIC Australia
- 6State Key Laboratory of Electrical Insulation and Power Equipment, Centre for Plasma Biomedicine, School of Electrical Engineering, Xi’an Jiaotong University, Xi’an, China
- 7CSIRO Technology, Lindfield, NSW Australia
- 8Ningbo China Beacons of Excellence Research and Innovation Institute, University of Nottingham, Ningbo, China
- 9Department of Chemical Engineering, School of Engineering, The University of Manchester, Manchester, UK
- 10Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ USA
- 11Institute of Fluid Science, Tohoku University, Sendai, Japan
- 12Department of Chemical Engineering, University of California, Davis, CA USA
Abstract
Integrating isolated metal atoms and subnanometer clusters within highly doped, structurally ordered carbon frameworks remains challenging because thermal synthesis promotes dopant loss, metal migration, and structural disorder. We report a biphasic liquid–liquid solution plasma strategy that produces nitrogen-doped graphitic carbons with a record-high nitrogen content of 22.4 atomic% while stabilizing atomically dispersed platinum sites and subnanometer clusters. Analysis of 53 cyclic organic precursors by optical emission spectroscopy and machine learning identifies CN and C2 radicals as positive descriptors for nitrogen incorporation and graphitic ordering, whereas Hβ emission correlates with hydrogen termination and disorder. In ambient-pressure nonthermal plasma-assisted ammonia synthesis, this material used as a catalyst achieves 3.97 gNH3 kWh‒1 and sustained operation for 85 h without degradation. Infrared spectroscopy, isotope-switching experiments, and density functional theory are consistent with a proposed cooperative catalytic pathway involving nitrogen activation at isolated platinum sites, hydrogenation at platinum clusters, and a Mars–van Krevelen-like contribution from Pt–Nx–C motifs.
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BibTeX
@article{niu2026plasma,
title = {{Plasma radicals control synthesis of platinum supported on nitrogen-doped graphitic carbon for ambient-pressure ammonia synthesis}},
author = {Jiangqi Niu and Shan Ding and Xu Ma and Zheng Lian and Chayanaphat Chokradjaroen and Shijie Xian and Sana Ullah and Xiaohan Chen and Yunxia Yang and Rusen Zhou and Renwu Zhou and Anthony B. Murphy and Xiaolei Fan and Yiguang Ju and Bruce C. Gates and Sibudjing Kawi},
journal = {Nature Communications},
year = {2026},
month = sep,
doi = {10.1038/s41467-026-77160-5},
url = {https://doi.org/10.1038/s41467-026-77160-5},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - JOUR
TI - Plasma radicals control synthesis of platinum supported on nitrogen-doped graphitic carbon for ambient-pressure ammonia synthesis
AU - Jiangqi Niu
AU - Shan Ding
AU - Xu Ma
AU - Zheng Lian
AU - Chayanaphat Chokradjaroen
AU - Shijie Xian
AU - Sana Ullah
AU - Xiaohan Chen
AU - Yunxia Yang
AU - Rusen Zhou
AU - Renwu Zhou
AU - Anthony B. Murphy
AU - Xiaolei Fan
AU - Yiguang Ju
AU - Bruce C. Gates
AU - Sibudjing Kawi
PY - 2026
DA - 2026/09/10
JO - Nature Communications
DO - 10.1038/s41467-026-77160-5
UR - https://doi.org/10.1038/s41467-026-77160-5
AB - Integrating isolated metal atoms and subnanometer clusters within highly doped, structurally ordered carbon frameworks remains challenging because thermal synthesis promotes dopant loss, metal migration, and structural disorder. We report a biphasic liquid–liquid solution plasma strategy that produces nitrogen-doped graphitic carbons with a record-high nitrogen content of 22.4 atomic% while stabilizing atomically dispersed platinum sites and subnanometer clusters. Analysis of 53 cyclic organic precursors by optical emission spectroscopy and machine learning identifies CN and C2 radicals as positive descriptors for nitrogen incorporation and graphitic ordering, whereas Hβ emission correlates with hydrogen termination and disorder. In ambient-pressure nonthermal plasma-assisted ammonia synthesis, this material used as a catalyst achieves 3.97 gNH3 kWh‒1 and sustained operation for 85 h without degradation. Infrared spectroscopy, isotope-switching experiments, and density functional theory are consistent with a proposed cooperative catalytic pathway involving nitrogen activation at isolated platinum sites, hydrogenation at platinum clusters, and a Mars–van Krevelen-like contribution from Pt–Nx–C motifs.
SN - 2041-1723
ER -