Artificial spherical chromatophore nanomicelles for selective CO2 reduction in water

Junlai Yu; Libei Huang; Qingxuan Tang; Shang-Bo Yu; Qiao-Yan Qi; Jiangshan Zhang; Danying Ma; Yifei Lei; Jianjun Su; Yun Song; Jean-Charles Eloi; Robert L. Harniman; Ufuk Borucu; Long Zhang; Minghui Zhu; Feng Tian; Lili Du; David Lee Phillips; Ian Manners; Ruquan Ye; Jia Tian

doi:10.1038/s41929-023-00962-z

Artificial spherical chromatophore nanomicelles for selective CO₂ reduction in water

Junlai Yu, Libei Huang, Qingxuan Tang, Shang-Bo Yu, Qiao-Yan Qi, Jiangshan Zhang, Danying Ma, Yifei Lei, Jianjun Su, Yun Song, Jean-Charles Eloi, Robert L. Harniman, Ufuk Borucu, Long Zhang, Minghui Zhu, Feng Tian, Lili Du^*, David Lee Phillips^*, Ian Manners, Ruquan Ye^*Jia Tian^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

85 Citations (Scopus)

Abstract

In nature, photosynthetic organelles harness solar radiation to produce energy-rich compounds from water and atmospheric CO₂ via exquisite supramolecular assemblies. Although artificial photocatalytic cycles have been shown to occur at higher intrinsic efficiencies, the low selectivity and stability in water for multi-electron CO₂ reduction hamper their practical applications. The creation of water-compatible artificial photocatalytic systems mimicking the natural photosynthetic apparatus for selective and efficient solar fuel production represents a major challenge. Here we show a highly stable and efficient artificial spherical chromatophore nanomicelle system self-assembled from Zn porphyrin amphiphiles with a Co catalyst in water for CO₂-to-methane conversion with a turnover number >6,600 and 89% selectivity over 30 days. The hierarchical self-assembly induced a spherical antenna effect that could facilitate the photocatalytic process with an initial 15% solar-to-fuel efficiency. Furthermore, it has a capability to efficiently reduce atmospheric CO₂ into methane with high selectivity in water. © The Author(s), under exclusive licence to Springer Nature Limited 2023.

Original language	English
Pages (from-to)	464–475
Journal	Nature Catalysis
Volume	6
Issue number	6
Online published	18 May 2023
DOIs	https://doi.org/10.1038/s41929-023-00962-z
Publication status	Published - Jun 2023

Funding

J.T. acknowledges the funding support from National Key Research and Development Program of China (2022YFA1206200); Shanghai Institute of Organic Chemistry and Shanghai Branch, CAS; Shanghai Rising-Star Program (22QA1411200); and the National Natural Science Foundation of China (no. 22271306). J.T. acknowledges the Marie-Curie Fellowship. I.M. acknowledges the Canada 150 Research Chair and NSERC Discovery Grant. R.Y. acknowledges the funding support from Young Scientists Fund of the National Natural Science Foundation of China (grant no. 21905240); the Shenzhen Research Institute, City University of Hong Kong; the State Key Laboratory of Marine Pollution (SKLMP) Seed Collaborative Research Fund; the Guangdong Basic and Applied Basic Research Fund (2022A1515011333); the Shenzhen Science and Technology Program (JCYJ20220818101204009); Hong Kong Research Grant Council (21300620) and the State Key Laboratory of Marine Pollution Internal Research Fund (SKLMP/IRF/0029). D.L.P. and L.D. thank the University of Hong Kong Development Fund 2013-2014 project ‘New Ultrafast Spectroscopy Experiments for Shared Facilities’. We thank the Shanghai Synchrotron Radiation Facility for providing the BL16B1 and BL10U1 beamline for collecting the synchrotron X-ray scattering data. We acknowledge access and support of the GW4 Facility for High-Resolution Electron Cryo-Microscopy, funded by the Wellcome Trust (202904/Z/16/Z and 206181/Z/17/Z) and BBSRC (BB/R000484/1). We thank Y. Zhang and X. Jin for the useful discussions. We thank M. Sener and D. H. Fackler for permission to use the visual molecular dynamics model in Fig. 1c.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

LIGHT-HARVESTING COMPLEX
VISIBLE-LIGHT
HYDROGEN-PRODUCTION
CRYSTAL-STRUCTURE
EFFICIENCIES
PHOTOCATALYSIS
PHOTOSYNTHESIS
ARCHITECTURE
EXCITATION
CATALYST

RGC Funding Information

RGC-funded

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10.1038/s41929-023-00962-z

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Yu, J., Huang, L., Tang, Q., Yu, S.-B., Qi, Q.-Y., Zhang, J., Ma, D., Lei, Y., Su, J., Song, Y., Eloi, J.-C., Harniman, R. L., Borucu, U., Zhang, L., Zhu, M., Tian, F., Du, L., Phillips, D. L., Manners, I., ... Tian, J. (2023). Artificial spherical chromatophore nanomicelles for selective CO₂ reduction in water. Nature Catalysis, 6(6), 464–475. https://doi.org/10.1038/s41929-023-00962-z

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abstract = "In nature, photosynthetic organelles harness solar radiation to produce energy-rich compounds from water and atmospheric CO2 via exquisite supramolecular assemblies. Although artificial photocatalytic cycles have been shown to occur at higher intrinsic efficiencies, the low selectivity and stability in water for multi-electron CO2 reduction hamper their practical applications. The creation of water-compatible artificial photocatalytic systems mimicking the natural photosynthetic apparatus for selective and efficient solar fuel production represents a major challenge. Here we show a highly stable and efficient artificial spherical chromatophore nanomicelle system self-assembled from Zn porphyrin amphiphiles with a Co catalyst in water for CO2-to-methane conversion with a turnover number >6,600 and 89% selectivity over 30 days. The hierarchical self-assembly induced a spherical antenna effect that could facilitate the photocatalytic process with an initial 15% solar-to-fuel efficiency. Furthermore, it has a capability to efficiently reduce atmospheric CO2 into methane with high selectivity in water. {\textcopyright} The Author(s), under exclusive licence to Springer Nature Limited 2023.",

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author = "Junlai Yu and Libei Huang and Qingxuan Tang and Shang-Bo Yu and Qiao-Yan Qi and Jiangshan Zhang and Danying Ma and Yifei Lei and Jianjun Su and Yun Song and Jean-Charles Eloi and Harniman, {Robert L.} and Ufuk Borucu and Long Zhang and Minghui Zhu and Feng Tian and Lili Du and Phillips, {David Lee} and Ian Manners and Ruquan Ye and Jia Tian",

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Yu, J, Huang, L, Tang, Q, Yu, S-B, Qi, Q-Y, Zhang, J, Ma, D, Lei, Y, Su, J , Song, Y, Eloi, J-C, Harniman, RL, Borucu, U, Zhang, L, Zhu, M, Tian, F, Du, L, Phillips, DL, Manners, I, Ye, R & Tian, J 2023, 'Artificial spherical chromatophore nanomicelles for selective CO₂ reduction in water', Nature Catalysis, vol. 6, no. 6, pp. 464–475. https://doi.org/10.1038/s41929-023-00962-z

TY - JOUR

T1 - Artificial spherical chromatophore nanomicelles for selective CO2 reduction in water

AU - Yu, Junlai

AU - Huang, Libei

AU - Tang, Qingxuan

AU - Yu, Shang-Bo

AU - Qi, Qiao-Yan

AU - Zhang, Jiangshan

AU - Ma, Danying

AU - Lei, Yifei

AU - Su, Jianjun

AU - Song, Yun

AU - Eloi, Jean-Charles

AU - Harniman, Robert L.

AU - Borucu, Ufuk

AU - Zhang, Long

AU - Zhu, Minghui

AU - Tian, Feng

AU - Du, Lili

AU - Phillips, David Lee

AU - Manners, Ian

AU - Ye, Ruquan

AU - Tian, Jia

PY - 2023/6

Y1 - 2023/6

N2 - In nature, photosynthetic organelles harness solar radiation to produce energy-rich compounds from water and atmospheric CO2 via exquisite supramolecular assemblies. Although artificial photocatalytic cycles have been shown to occur at higher intrinsic efficiencies, the low selectivity and stability in water for multi-electron CO2 reduction hamper their practical applications. The creation of water-compatible artificial photocatalytic systems mimicking the natural photosynthetic apparatus for selective and efficient solar fuel production represents a major challenge. Here we show a highly stable and efficient artificial spherical chromatophore nanomicelle system self-assembled from Zn porphyrin amphiphiles with a Co catalyst in water for CO2-to-methane conversion with a turnover number >6,600 and 89% selectivity over 30 days. The hierarchical self-assembly induced a spherical antenna effect that could facilitate the photocatalytic process with an initial 15% solar-to-fuel efficiency. Furthermore, it has a capability to efficiently reduce atmospheric CO2 into methane with high selectivity in water. © The Author(s), under exclusive licence to Springer Nature Limited 2023.

AB - In nature, photosynthetic organelles harness solar radiation to produce energy-rich compounds from water and atmospheric CO2 via exquisite supramolecular assemblies. Although artificial photocatalytic cycles have been shown to occur at higher intrinsic efficiencies, the low selectivity and stability in water for multi-electron CO2 reduction hamper their practical applications. The creation of water-compatible artificial photocatalytic systems mimicking the natural photosynthetic apparatus for selective and efficient solar fuel production represents a major challenge. Here we show a highly stable and efficient artificial spherical chromatophore nanomicelle system self-assembled from Zn porphyrin amphiphiles with a Co catalyst in water for CO2-to-methane conversion with a turnover number >6,600 and 89% selectivity over 30 days. The hierarchical self-assembly induced a spherical antenna effect that could facilitate the photocatalytic process with an initial 15% solar-to-fuel efficiency. Furthermore, it has a capability to efficiently reduce atmospheric CO2 into methane with high selectivity in water. © The Author(s), under exclusive licence to Springer Nature Limited 2023.

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SN - 2520-1158

VL - 6

SP - 464

EP - 475

JO - Nature Catalysis

JF - Nature Catalysis

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ER -

Artificial spherical chromatophore nanomicelles for selective CO₂ reduction in water

Abstract

Funding

UN SDGs

Research Keywords

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ECS: Investigating the Inductive Effect and Kinetics of Covalently Immobilized Molecular Catalysts for High-performance Electrochemical CO2 Reduction

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Artificial spherical chromatophore nanomicelles for selective CO2 reduction in water

Abstract

Funding

UN SDGs

Research Keywords

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

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Projects

ECS: Investigating the Inductive Effect and Kinetics of Covalently Immobilized Molecular Catalysts for High-performance Electrochemical CO2 Reduction

Cite this

Artificial spherical chromatophore nanomicelles for selective CO₂ reduction in water