Janus carbon shells with inner–outer functional asymmetry enable local proton enrichment for promoting CO2 methanation
Abstract
Exploring non-copper electrocatalysts for CO₂-to-CH₄ electrosynthesis is important for reducing overreliance on copper and broadening the catalyst landscape. We report a strategy that enables CH₄ formation on cobalt phthalocyanine (CoPc) by regulating the local reaction microenvironment through the catalyst structure. Ultrathin hollow carbon nanospheres (HCNs) with a uniform size were synthesized and used as supports for CoPc, forming “Janus carbon shells” with inner–outer functional asymmetry. The resulting CoPc-HCN hybrid had a maximum CO₂-to-CH₄ selectivity of 15.1%, overcoming the conventional CO-selective behavior of CoPc. Mechanistic studies show that the hollow carbon structure induces a proton enrichment outside the shell through an inner–outer surface interaction. The inner carbon surface promotes the hydrogen evolution reaction (HER) and produces a proton-enriched environment near the CoPc-active outer surface, thereby enabling CO₂ methanation. This work highlights the critical role of catalyst structure in overcoming intrinsic selectivity limits of molecular catalysts.
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BibTeX
@article{liu2026janus,
title = {{Janus carbon shells with inner–outer functional asymmetry enable local proton enrichment for promoting CO2 methanation}},
author = {Tengyi Liu and Xiaofan Hou and Wijak Yospanya and Songbo Ye and Yasutaka Matsuo and Shimpei Ono and Reiko Oda and Hao Li and Hiroshi Yabu},
journal = {New Carbon Materials},
year = {2026},
month = oct,
doi = {10.1016/s1872-5805(26)61096-7},
url = {https://hal.science/hal-05826004v1},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Janus carbon shells with inner–outer functional asymmetry enable local proton enrichment for promoting CO2 methanation
AU - Tengyi Liu
AU - Xiaofan Hou
AU - Wijak Yospanya
AU - Songbo Ye
AU - Yasutaka Matsuo
AU - Shimpei Ono
AU - Reiko Oda
AU - Hao Li
AU - Hiroshi Yabu
PY - 2026
DA - 2026/10/20
JO - New Carbon Materials
DO - 10.1016/s1872-5805(26)61096-7
UR - https://hal.science/hal-05826004v1
AB - Exploring non-copper electrocatalysts for CO₂-to-CH₄ electrosynthesis is important for reducing overreliance on copper and broadening the catalyst landscape. We report a strategy that enables CH₄ formation on cobalt phthalocyanine (CoPc) by regulating the local reaction microenvironment through the catalyst structure. Ultrathin hollow carbon nanospheres (HCNs) with a uniform size were synthesized and used as supports for CoPc, forming “Janus carbon shells” with inner–outer functional asymmetry. The resulting CoPc-HCN hybrid had a maximum CO₂-to-CH₄ selectivity of 15.1%, overcoming the conventional CO-selective behavior of CoPc. Mechanistic studies show that the hollow carbon structure induces a proton enrichment outside the shell through an inner–outer surface interaction. The inner carbon surface promotes the hydrogen evolution reaction (HER) and produces a proton-enriched environment near the CoPc-active outer surface, thereby enabling CO₂ methanation. This work highlights the critical role of catalyst structure in overcoming intrinsic selectivity limits of molecular catalysts.
SN - 1872-5805
SN - 1872-5805
ER -