Skip to content
DraconiticResearch
Search Sources API
197,783 studies31 sourcesUpdated 26 min ago
Peer-reviewedCC BY-NC-NDJACS Au

Electron-Reservoir Multiple Bond in RhC⁻ for Dinitrogen Cleavage.

  • Shi-Hu Du1
  • Jun Li1
  • Shi-Jun Wang1
  • Hao Wu2
  • Wen-Wu Xu3
  • Hua Xie4
  • Ling Jiang4
  • Hong-Sheng Zhai5
  • Shi-Bo Cheng1
5 affiliations
  1. 1School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, China.
  2. 2School of Materials and Chemical Engineering, Ningbo University of Technology, Ningbo 315211, China.
  3. 3School of Physical Science and Technology, Ningbo University, Ningbo 315211, China.
  4. 4State Key Laboratory of Chemical Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
  5. 5Henan Key Laboratory of Infrared Spectrum Measures and Applications, School of Optoelectronic Engineering, Henan Normal University, Xinxiang 453007, China.
Read full textPDFDOICite

Abstract

Multiple bonds involving the main-group element represent a prominent class of interactions whose formation and cleavage involve substantial electron redistribution, yet its functional role in redox processes remains unexplored. Herein, we identify a triple-bond character in the RhC- anion, which was generated in the gas phase and characterized spectroscopically by mass spectrometry and photoelectron spectroscopy. Concurrently, the RhC- species is demonstrated to exhibit dinitrogen cleavage capability. Quantum chemical calculations reveal that the resulting products feature a pronounced weakening of the Rh-C interaction along with concomitant C-N bond formation. Electronic structure analysis further indicates that the Rh-C triple bond acts as an electron reservoir, and nitrogen reduction proceeds primarily through cleavage of the Rh-C bond, which releases stored electrons. This work establishes the functional application of metal-carbon multiple bonds in dinitrogen cleavage, demonstrating their unique capacity to couple structural dynamics with redox chemistry and thereby establishing a transformative mechanism for designing electron-reservoir catalysts in dinitrogen activation and beyond.

Related

  1. Oxidative C–C Bond Cleavage of 1,2-Diols by Mn-Doped CeO2 Catalysts
    Hiroki Miura, Yukino Nakamura, Tetsuya Shishido
    ChemRxivPreprintCC BYFull textGeneral chemistryChemRxiv
  2. Visible-Light-Driven C-F Bond Cleavage in Perfluoroalkyl Carboxylic Acids: Readily Accessible Ruthenium-Bipyridine Complexes as Effective Catalysts.
    Ashan S Wickramaarachchi, Ishan D Jayampathi, Maggie M Larson +2
    OrganometallicsPeer-reviewedCC BY-NC-NDFull textEnvironmental chemistryEurope PMCPMC
  3. Catalytic C–O Bond Cleavage of Vinyl Ethers via Dehydrovinylation and Tandem Tishchenko Coupling
    Ashish Parihar, Soham Chakraborty, Santanu Malakar +1
    ChemRxivPreprintCC BY-NC-NDFull textOrganic chemistryChemRxiv
  4. Zirconium-Mediated C–O Bond Cleavage of Alkenyl Ethers Enables Nickel-Catalyzed C(sp3)–C(sp3) and C(sp3)–C(sp2) Cross-Coupling
    Haowen Xu, Songlin Bai, Bin Yang +3
    ChemRxivPreprintCC BYFull textOrganic chemistryChemRxiv
  5. A DFT Study of Oxidative Lignin β-O-4 Bond Cleavage by Transition-Metal Catalysis
    Ellie Shen, Nick DeMello
    ChemRxivPreprintCC BYFull textGeneral chemistryChemRxiv

Cite

BibTeXRIS
BibTeX
@article{du2026electronreservoir,
  title = {{Electron-Reservoir Multiple Bond in RhC⁻ for Dinitrogen Cleavage.}},
  author = {Shi-Hu Du and Jun Li and Shi-Jun Wang and Hao Wu and Wen-Wu Xu and Hua Xie and Ling Jiang and Hong-Sheng Zhai and Shi-Bo Cheng},
  journal = {JACS Au},
  year = {2026},
  month = sep,
  doi = {10.1021/jacsau.6c01036},
  url = {https://europepmc.org/article/MED/42953623},
  note = {CC BY-NC-ND},
}
RIS
TY  - JOUR
TI  - Electron-Reservoir Multiple Bond in RhC⁻ for Dinitrogen Cleavage.
AU  - Shi-Hu Du
AU  - Jun Li
AU  - Shi-Jun Wang
AU  - Hao Wu
AU  - Wen-Wu Xu
AU  - Hua Xie
AU  - Ling Jiang
AU  - Hong-Sheng Zhai
AU  - Shi-Bo Cheng
PY  - 2026
DA  - 2026/09/18
JO  - JACS Au
DO  - 10.1021/jacsau.6c01036
UR  - https://europepmc.org/article/MED/42953623
AB  - Multiple bonds involving the main-group element represent a prominent class of interactions whose formation and cleavage involve substantial electron redistribution, yet its functional role in redox processes remains unexplored. Herein, we identify a triple-bond character in the RhC- anion, which was generated in the gas phase and characterized spectroscopically by mass spectrometry and photoelectron spectroscopy. Concurrently, the RhC- species is demonstrated to exhibit dinitrogen cleavage capability. Quantum chemical calculations reveal that the resulting products feature a pronounced weakening of the Rh-C interaction along with concomitant C-N bond formation. Electronic structure analysis further indicates that the Rh-C triple bond acts as an electron reservoir, and nitrogen reduction proceeds primarily through cleavage of the Rh-C bond, which releases stored electrons. This work establishes the functional application of metal-carbon multiple bonds in dinitrogen cleavage, demonstrating their unique capacity to couple structural dynamics with redox chemistry and thereby establishing a transformative mechanism for designing electron-reservoir catalysts in dinitrogen activation and beyond.
SN  - 2691-3704
ER  -