Long-range electronic interactions of tubular single-atom Cu-N3 catalysts for nanoconfined direct electron transfer oxidation
5 affiliations
- 1College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, China
- 2College of Geography and Environmental Sciences, Zhejiang Normal University, Jinhua, China
- 3College of Geography and Environmental Sciences, Zhejiang Normal University, Jinhua, China. [email protected]
- 4School of Chemical Engineering, Adelaide University, Adelaide, SA, Australia. [email protected]
- 5College of Environmental Science and Engineering, Hunan University and Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Changsha, China. [email protected]
Abstract
Leveraging atomically dispersed catalysts to selectively trigger nonradical oxidation can overcome the short lifetimes and poor selectivity of radical-based processes in water treatment. Here, we integrate long-range electronic modulation with nanoconfinement by embedding isolated Cu-N3 sites into carbon-doped tubular carbon nitride (CuTCN/C). Carbon atoms intrinsic to the support upshift the Cu d-band center, which strengthens peroxymonosulfate (PMS) adsorption and lowers the activation energy barrier. Moreover, surface mesopores greatly enrich local PMS concentration in the nanoconfined environment and accelerate interfacial electron migration to coordinate a direct electron transfer pathway. As a result, CuTCN/C delivers the highest activity among Cu single-atom catalysts, while operating with minimal PMS doses due to the remarkably accelerated mass transfer. Spectroscopic, electrochemical, DFT and MD analyses confirm the synergistic roles of electronic tuning and nanoconfinement in promoting oriented PMS activation as reactive surface complex that directly attacks surface-enriched pollutants with high PMS utilization efficiency. The continuous fluidized-bed tests demonstrate strong salt tolerance and long-term stability of the system, while life-cycle assessment confirms favorable environmental metrics in practical application. This dual engineering strategy of macroscopic morphological and microscopic electronic structure provides a blueprint for smart design of robust single-atom catalysts for selective and high-efficiency water purification. Atomically dispersed catalysts that enable selective nonradical oxidation can overcome the short lifetimes and poor selectivity of radical-based water treatment processes. Here, the authors combine long-range electronic modulation with nanoconfinement by embedding isolated Cu–N₃ sites in carbon-doped tubular carbon nitride, demonstrating strong potential for water purification.
Related
- Resonant photoelectron spectroscopy: a tool for characterising the electronic properties of catalysts in operation
- Dynamic Coordination Microenvironments of Fe Single-Atom Catalysts in Advanced Oxidation Processes: From Working-State Evolution to Pathway-Selective Regulation
- A Direct Route for Upcycling Electronic Waste Into High-Performance Palladium Catalysts
- Precise polymerization of phenolic pollutants by a nanoconfined reactor with Fe-Mo dual-site
- Physical Properties of Nanoconfined Methane Hydrate: Structure, Thermoelasticity, and Thermal Conductivity
BibTeX
@article{yan2026longrange,
title = {{Long-range electronic interactions of tubular single-atom Cu-N3 catalysts for nanoconfined direct electron transfer oxidation}},
author = {Huchuan Yan and Bisheng Li and Shiyu Liu and Mingzhu Zhou and Xuerong Zhou and Dengsheng Ma and Dongbo Wang and Hongjun Lin and Xiaoguang Duan and Cui Lai},
journal = {Nature Communications},
year = {2026},
month = may,
doi = {10.1038/s41467-026-73151-8},
url = {https://doi.org/10.1038/s41467-026-73151-8},
note = {CC BY-NC-ND},
}
RIS
TY - JOUR
TI - Long-range electronic interactions of tubular single-atom Cu-N3 catalysts for nanoconfined direct electron transfer oxidation
AU - Huchuan Yan
AU - Bisheng Li
AU - Shiyu Liu
AU - Mingzhu Zhou
AU - Xuerong Zhou
AU - Dengsheng Ma
AU - Dongbo Wang
AU - Hongjun Lin
AU - Xiaoguang Duan
AU - Cui Lai
PY - 2026
DA - 2026/05/20
JO - Nature Communications
DO - 10.1038/s41467-026-73151-8
UR - https://doi.org/10.1038/s41467-026-73151-8
AB - Leveraging atomically dispersed catalysts to selectively trigger nonradical oxidation can overcome the short lifetimes and poor selectivity of radical-based processes in water treatment. Here, we integrate long-range electronic modulation with nanoconfinement by embedding isolated Cu-N3 sites into carbon-doped tubular carbon nitride (CuTCN/C). Carbon atoms intrinsic to the support upshift the Cu d-band center, which strengthens peroxymonosulfate (PMS) adsorption and lowers the activation energy barrier. Moreover, surface mesopores greatly enrich local PMS concentration in the nanoconfined environment and accelerate interfacial electron migration to coordinate a direct electron transfer pathway. As a result, CuTCN/C delivers the highest activity among Cu single-atom catalysts, while operating with minimal PMS doses due to the remarkably accelerated mass transfer. Spectroscopic, electrochemical, DFT and MD analyses confirm the synergistic roles of electronic tuning and nanoconfinement in promoting oriented PMS activation as reactive surface complex that directly attacks surface-enriched pollutants with high PMS utilization efficiency. The continuous fluidized-bed tests demonstrate strong salt tolerance and long-term stability of the system, while life-cycle assessment confirms favorable environmental metrics in practical application. This dual engineering strategy of macroscopic morphological and microscopic electronic structure provides a blueprint for smart design of robust single-atom catalysts for selective and high-efficiency water purification. Atomically dispersed catalysts that enable selective nonradical oxidation can overcome the short lifetimes and poor selectivity of radical-based water treatment processes. Here, the authors combine long-range electronic modulation with nanoconfinement by embedding isolated Cu–N₃ sites in carbon-doped tubular carbon nitride, demonstrating strong potential for water purification.
SN - 2041-1723
ER -