Authors
Jian Li, Wenli Zhang, Zhenfa Wu, Wenjuan Xue, Xiangyu Guo, Hongliang Huang, Jiandong Pang, Chongli Zhong
Published in
Angewandte Chemie (International ed. in English). Pages e6707086. Jul 02, 2026. Epub Jul 02, 2026.
Abstract
CH4-rich coal-bed methane (CBM) is often contaminated with N2, but their similar properties make conventional separation energy-intensive and inefficient. Herein, we report a photocatalytic strategy for selective N2 conversion over CH4, achieving simultaneous CBM purification and nitrogen valorization. A Co-Ni metal-organic framework (CoNi-PYZ) features isolated bimetallic sites, where ligand/Co units donate electrons to Ni, establishing spatially separated reduction and oxidation centers. This structural motif drives a photocatalytic cascade nitrogen fixation that N2 is first reduced to NH3 at the Ni sites; subsequently, the generated NH3 outcompetes CH4 for the Co sites, leading to its oxidation to NO3 -. This remarkable selectivity is governed by the high polarity and lone-pair electron donation of NH3, favoring its adsorption over nonpolar CH4. Notably, the optimal catalyst achieves high activity under mild conditions without sacrificial agents, delivering NH4 + and NO3 - production rates of 599.8 and 199.8 µmol g- 1 h- 1, respectively. Mechanism analysis reveals that ligand engineering optimizes the d-band center to balance adsorption and desorption, thereby minimizing the rate-determining step barriers for both half-reactions, consistent with the Sabatier principle. This work provides a reaction-driven alternative to traditional phase-separation, establishing a novel paradigm for CBM upgrading coupled with selective N2 transformation.
PMID:
42390844
Bibliographic data and abstract were imported from PubMed on 02 Jul 2026.
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