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Filling metal–organic framework mesopores with TiO2 for CO2 photoreduction

Author

Listed:
  • Zhuo Jiang

    (Wuhan University)

  • Xiaohui Xu

    (Wuhan University)

  • Yanhang Ma

    (ShanghaiTech University)

  • Hae Sung Cho

    (ShanghaiTech University)

  • Deng Ding

    (Wuhan University)

  • Chao Wang

    (Wuhan University)

  • Jie Wu

    (Wuhan University)

  • Peter Oleynikov

    (ShanghaiTech University)

  • Mei Jia

    (Xiamen University)

  • Jun Cheng

    (Xiamen University)

  • Yi Zhou

    (Wuhan University)

  • Osamu Terasaki

    (ShanghaiTech University)

  • Tianyou Peng

    (Wuhan University)

  • Ling Zan

    (Wuhan University)

  • Hexiang Deng

    (Wuhan University
    Wuhan University)

Abstract

Metal–organic frameworks (MOFs)1–3 are known for their specific interactions with gas molecules4,5; this, combined with their rich and ordered porosity, makes them promising candidates for the photocatalytic conversion of gas molecules to useful products6. However, attempts to use MOFs or MOF-based composites for CO2 photoreduction6–13 usually result in far lower CO2 conversion efficiency than that obtained from state-of-the-art solid-state or molecular catalysts14–18, even when facilitated by sacrificial reagents. Here we create ‘molecular compartments’ inside MOF crystals by growing TiO2 inside different pores of a chromium terephthalate-based MOF (MIL-101) and its derivatives. This allows for synergy between the light-absorbing/electron-generating TiO2 units and the catalytic metal clusters in the backbones of MOFs, and therefore facilitates photocatalytic CO2 reduction, concurrent with production of O2. An apparent quantum efficiency for CO2 photoreduction of 11.3 per cent at a wavelength of 350 nanometres is observed in a composite that consists of 42 per cent TiO2 in a MIL-101 derivative, namely, 42%-TiO2-in-MIL-101-Cr-NO2. TiO2 units in one type of compartment in this composite are estimated to be 44 times more active than those in the other type, underlining the role of precise positioning of TiO2 in this system.

Suggested Citation

  • Zhuo Jiang & Xiaohui Xu & Yanhang Ma & Hae Sung Cho & Deng Ding & Chao Wang & Jie Wu & Peter Oleynikov & Mei Jia & Jun Cheng & Yi Zhou & Osamu Terasaki & Tianyou Peng & Ling Zan & Hexiang Deng, 2020. "Filling metal–organic framework mesopores with TiO2 for CO2 photoreduction," Nature, Nature, vol. 586(7830), pages 549-554, October.
  • Handle: RePEc:nat:nature:v:586:y:2020:i:7830:d:10.1038_s41586-020-2738-2
    DOI: 10.1038/s41586-020-2738-2
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    Citations

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    Cited by:

    1. Yajuan Ma & Xiaoxuan Yi & Shaolei Wang & Tao Li & Bien Tan & Chuncheng Chen & Tetsuro Majima & Eric R. Waclawik & Huaiyong Zhu & Jingyu Wang, 2022. "Selective photocatalytic CO2 reduction in aerobic environment by microporous Pd-porphyrin-based polymers coated hollow TiO2," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    2. Shengyao Wang & Bo Jiang & Joel Henzie & Feiyan Xu & Chengyuan Liu & Xianguang Meng & Sirong Zou & Hui Song & Yang Pan & Hexing Li & Jiaguo Yu & Hao Chen & Jinhua Ye, 2023. "Designing reliable and accurate isotope-tracer experiments for CO2 photoreduction," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Jie Zhou & Jie Li & Liang Kan & Lei Zhang & Qing Huang & Yong Yan & Yifa Chen & Jiang Liu & Shun-Li Li & Ya-Qian Lan, 2022. "Linking oxidative and reductive clusters to prepare crystalline porous catalysts for photocatalytic CO2 reduction with H2O," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    4. Xinfeng Chen & Chengdong Peng & Wenyan Dan & Long Yu & Yinan Wu & Honghan Fei, 2022. "Bromo- and iodo-bridged building units in metal-organic frameworks for enhanced carrier transport and CO2 photoreduction by water vapor," Nature Communications, Nature, vol. 13(1), pages 1-14, December.
    5. Sanchita Karmakar & Soumitra Barman & Faruk Ahamed Rahimi & Darsi Rambabu & Sukhendu Nath & Tapas Kumar Maji, 2023. "Confining charge-transfer complex in a metal-organic framework for photocatalytic CO2 reduction in water," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    6. Jin Ming Wang & Qin Yao Zhu & Jeong Heon Lee & Tae Gyun Woo & Yue Xing Zhang & Woo-Dong Jang & Tae Kyu Kim, 2023. "Asymmetric gradient orbital interaction of hetero-diatomic active sites for promoting C − C coupling," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    7. Yan Shen & Chunjin Ren & Lirong Zheng & Xiaoyong Xu & Ran Long & Wenqing Zhang & Yong Yang & Yongcai Zhang & Yingfang Yao & Haoqiang Chi & Jinlan Wang & Qing Shen & Yujie Xiong & Zhigang Zou & Yong Zh, 2023. "Room-temperature photosynthesis of propane from CO2 with Cu single atoms on vacancy-rich TiO2," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    8. Yuan-Sheng Xia & Meizhong Tang & Lei Zhang & Jiang Liu & Cheng Jiang & Guang-Kuo Gao & Long-Zhang Dong & Lan-Gui Xie & Ya-Qian Lan, 2022. "Tandem utilization of CO2 photoreduction products for the carbonylation of aryl iodides," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    9. Ya Wang & Jian-Xin Wei & Hong-Liang Tang & Lu-Hua Shao & Long-Zhang Dong & Xiao-Yu Chu & Yan-Xia Jiang & Gui-Ling Zhang & Feng-Ming Zhang & Ya-Qian Lan, 2024. "Artificial photosynthetic system for diluted CO2 reduction in gas-solid phase," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    10. Hui Li & Caikun Cheng & Zhijie Yang & Jingjing Wei, 2022. "Encapsulated CdSe/CdS nanorods in double-shelled porous nanocomposites for efficient photocatalytic CO2 reduction," Nature Communications, Nature, vol. 13(1), pages 1-11, December.

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