Biomimetic spatial compartmentalization directs C1 intermediate evolution for highly selective CO2 photomethanation
- 1Faculty of Chemistry and Chemical Engineering, Shantou University Shantou 515063 P. R. China +86 754 82902767 +86 754 86503791
- 2College of Chemical Engineering, Hebei Normal University of Science & Technology Qinhuangdao 066004 P. R. China
Abstract
Photoreduction of CO2 and H2O to CH4 offers a sustainable pathway for solar-to-chemical energy conversion. However, premature desorption of the CO* intermediate before coupling with protons (H*) to form a CHO* intermediate remains a major bottleneck, severely suppressing CH4 selectivity. Herein, we design a novel biomimetic “nucleus–cytoplasm” configuration photocatalyst, Pd1(C)/Ns/CNNs, where atomically dispersed Pd single atoms (Pd1(C)) serve as the cytoplasm for selective CO2 activation, while the adjacent Pd nanosheets (PdNs) act as the “nucleus” to supply H* and catalyze downstream hydrogenation. This configuration induces a short-range internal electric field, analogous to intracellular signaling, which synchronizes electron–H* transfer, facilitates directional CO* migration toward the “nucleus”, and restrains premature desorption, enabling CHO* formation seamlessly. Experimental results and density functional theory calculations show that Pd1(C) binds and activates CO2, while PdNs stabilize CO* and promote H2O dissociation to generate H*. Ab initio molecular dynamics simulations capture the CO*–H* coupling into CHO*, directly visualizing this key transformation step. As a result, the Pd1(C)/Ns/CNNs achieves an outstanding CH4 evolution rate of 876.8 µmol g−1 h−1 with nearly 100% selectivity. This work introduces a biologically inspired spatial design that regulates intermediate evolution via local electronic synergy, providing a new idea for highly efficient and selective CO2 photomethanation.
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BibTeX
@article{li2026biomimetic,
title = {{Biomimetic spatial compartmentalization directs C1 intermediate evolution for highly selective CO2 photomethanation}},
author = {Yang Li and Xiaoxue Zhao and Yujie Chen and Yanshan Chen and Jiahao Zheng and Zhi Liu},
journal = {Chemical Science},
year = {2026},
month = sep,
doi = {10.1039/d6sc04259g},
url = {https://doi.org/10.1039/d6sc04259g},
note = {CC BY-NC 3.0},
}
RIS
TY - JOUR
TI - Biomimetic spatial compartmentalization directs C1 intermediate evolution for highly selective CO2 photomethanation
AU - Yang Li
AU - Xiaoxue Zhao
AU - Yujie Chen
AU - Yanshan Chen
AU - Jiahao Zheng
AU - Zhi Liu
PY - 2026
DA - 2026/09/02
JO - Chemical Science
DO - 10.1039/d6sc04259g
UR - https://doi.org/10.1039/d6sc04259g
AB - Photoreduction of CO2 and H2O to CH4 offers a sustainable pathway for solar-to-chemical energy conversion. However, premature desorption of the CO* intermediate before coupling with protons (H*) to form a CHO* intermediate remains a major bottleneck, severely suppressing CH4 selectivity. Herein, we design a novel biomimetic “nucleus–cytoplasm” configuration photocatalyst, Pd1(C)/Ns/CNNs, where atomically dispersed Pd single atoms (Pd1(C)) serve as the cytoplasm for selective CO2 activation, while the adjacent Pd nanosheets (PdNs) act as the “nucleus” to supply H* and catalyze downstream hydrogenation. This configuration induces a short-range internal electric field, analogous to intracellular signaling, which synchronizes electron–H* transfer, facilitates directional CO* migration toward the “nucleus”, and restrains premature desorption, enabling CHO* formation seamlessly. Experimental results and density functional theory calculations show that Pd1(C) binds and activates CO2, while PdNs stabilize CO* and promote H2O dissociation to generate H*. Ab initio molecular dynamics simulations capture the CO*–H* coupling into CHO*, directly visualizing this key transformation step. As a result, the Pd1(C)/Ns/CNNs achieves an outstanding CH4 evolution rate of 876.8 µmol g−1 h−1 with nearly 100% selectivity. This work introduces a biologically inspired spatial design that regulates intermediate evolution via local electronic synergy, providing a new idea for highly efficient and selective CO2 photomethanation.
SN - 2041-6520
SN - 2041-6539
ER -