Nanochanneling and Local Crystallization Engineering Accelerate Multiphase Single‐Atom Catalysis for Rapid Water Decontamination
Date
2025
Authors
Liu, Y.
Wang, Y.
Wang, Y.
Miao, J.
Yang, J.
Hu, K.
Sun, H.
Xiao, J.
Chen, C.
Duan, X.
Editors
Advisors
Journal Title
Journal ISSN
Volume Title
Type:
Journal article
Citation
Angewandte Chemie International Edition, 2025; 137(27):e202504571-1-e202504571-11
Statement of Responsibility
Ya Liu, Yuxian Wang, Yunpeng Wang, Jie Miao, Jiajia Yang, Kunsheng Hu, Hongqi Sun, Jiadong Xiao, Chunmao Chen, Xiaoguang Duan, Shaobin Wang
Conference Name
Abstract
Precise engineering of single-atom catalysts (SACs) with optimal hierarchical structures and favorable local chemical environments remains a significant challenge to cater for multiphase heterogeneous processes. Here, we develop a universal strategy for synthesizing channel-digging microspherical SACs that markedly enhance gas–liquid–solid mass transfer and fine-tune the thermodynamics of catalytic ozonation. By catalytically graphitizing carbon microspheres and selectively etching amorphous carbon domains via mild combustion, we fabricate cross-linked hierarchical graphitic nanochannels confining transition metal (e.g., Co, Cr, Mn, Fe, Ni) single atoms (TMCSs-Air). This nanoenvironment engineering increases interfacial ozone (O₃) mass transfer by 3.2-fold and directs O₃ adsorption from a conventional “end-on” to a bidental “side-on” configuration. The enhanced inter-orbital electronic interactions lower the O₃ activation barrier and form highly oxidizing surface-confined O₃ (*O₃). Consequently, the CoCSs-Air catalyst achieves a 3.6-fold higher ozone utilization efficiency and a 4.2-fold greater turnover frequency (TOF = 1580 min⁻¹) compared with pristine Co-doped carbon microspheres (CoCSs). Technical and economic evaluations further confirm the feasibility of TMCSs-Air nanoreactors in treating real-world petrochemical wastewater, highlighting its broader potential in overcoming gas diffusion barriers and tuning reaction pathways for multiphase heterogeneous catalysis.
School/Discipline
Dissertation Note
Provenance
Description
German version
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Rights
© 2025 The Author(s). Angewandte Chemie published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.