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Efficient Photocatalytic CO2 Reduction by a Ni(II) Complex Having Pyridine Pendants through Capturing a Mg2+ Ion as a Lewis-Acid Cocatalyst

  • Dachao Hong
    Dachao Hong
    Interdisciplinary Research Center for Catalytic Chemistry, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan
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    Orcidhttp://orcid.org/0000-0003-0581-1315
    • , 
  • Takuya Kawanishi
    Takuya Kawanishi
    Interdisciplinary Research Center for Catalytic Chemistry, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565, Japan
    Department of Chemistry, Faculty of Pure and Applied Sciences, University of Tsukuba, CREST, Japan Science and Technology Agency (JST), 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, Japan
    More by Takuya Kawanishi
    • , 
  • Yuto Tsukakoshi
    Yuto Tsukakoshi
    Department of Chemistry, Faculty of Pure and Applied Sciences, University of Tsukuba, CREST, Japan Science and Technology Agency (JST), 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, Japan
    More by Yuto Tsukakoshi
    • , 
  • Hiroaki Kotani
    Hiroaki Kotani
    Department of Chemistry, Faculty of Pure and Applied Sciences, University of Tsukuba, CREST, Japan Science and Technology Agency (JST), 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, Japan
    More by Hiroaki Kotani
    Orcidhttp://orcid.org/0000-0001-7737-026X
    • , 
  • Tomoya Ishizuka
    Tomoya Ishizuka
    Department of Chemistry, Faculty of Pure and Applied Sciences, University of Tsukuba, CREST, Japan Science and Technology Agency (JST), 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, Japan
    More by Tomoya Ishizuka
    Orcidhttp://orcid.org/0000-0002-3897-026X
    • , and 
  • Takahiko Kojima*
    Takahiko Kojima
    Department of Chemistry, Faculty of Pure and Applied Sciences, University of Tsukuba, CREST, Japan Science and Technology Agency (JST), 1-1-1 Tennoudai, Tsukuba, Ibaraki 305-8571, Japan
    *[email protected]
    More by Takahiko Kojima
    Orcidhttp://orcid.org/0000-0001-9941-8375
Cite this: J. Am. Chem. Soc. 2019, 141, 51, 20309–20317
Publication Date (Web):November 15, 2019
https://doi.org/10.1021/jacs.9b10597
Copyright © 2019 American Chemical Society
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Abstract

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We have synthesized a new Ni(II) complex having an S2N2-tetradentate ligand with two noncoordinating pyridine pendants as binding sites of Lewis-acidic metal ions in the vicinity of the Ni center, aiming at efficient CO production in photocatalytic CO2 reduction. In the presence of Mg2+ ions, enhancement of selective CO formation was observed in photocatalytic CO2 reduction by the Ni complex with the pyridine pendants through the formation of a Mg2+-bound species, as compared to the previously reported Ni complex without the Lewis-acid capturing sites. A higher quantum yield of CO evolution for the Mg2+-bound Ni complex was determined to be 11.1%. Even at lower CO2 concentration (5%), the Ni complex with the pendants exhibited comparable CO production to that at the CO2-saturated concentration (100%). The Mg2+-bound Ni complex was evidenced by mass spectrometry and 1H NMR measurements. The enhancement of CO2 reduction by the Mg2+-bound species should be derived from cooperativity between the Ni and Mg centers for the stabilization of a Ni–CO2 intermediate by a Lewis-acidic Mg2+ ion captured in the vicinity of the Ni center, as supported by DFT calculations. The detailed mechanism of photocatalytic CO2 reduction by the Ni complex with the pyridine pendants in the presence of Mg2+ ions is discussed based on spectroscopic detection of the intermediate and kinetic analysis.

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Cited By

This article is cited by 24 publications.

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  2. Liyan Zhang, Shiwei Li, Huiping Liu, Yuan-Sheng Cheng, Xian-Wen Wei, Xiaomin Chai, Guozan Yuan. Highly Efficient and Selective Visible-Light Driven CO2 Reduction by Two Co-Based Catalysts in Aqueous Solution. Inorganic Chemistry 2020, 59 (23) , 17464-17472. https://doi.org/10.1021/acs.inorgchem.0c02733
  3. Sung Eun Lee, Azam Nasirian, Ye Eun Kim, Pegah Tavakoli Fard, Youngmee Kim, Byeongmoon Jeong, Sung-Jin Kim, Jin-Ook Baeg, Jinheung Kim. Visible-Light Photocatalytic Conversion of Carbon Dioxide by Ni(II) Complexes with N4S2 Coordination: Highly Efficient and Selective Production of Formate. Journal of the American Chemical Society 2020, 142 (45) , 19142-19149. https://doi.org/10.1021/jacs.0c08145
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  6. Takahiko Kojima. Photocatalytic Carbon Dioxide Reduction Using Nickel Complexes as Catalysts. ChemPhotoChem 2021, 3 https://doi.org/10.1002/cptc.202000263
  7. Pingping Niu, Zhiming Pan, Sibo Wang, Xinchen Wang. Tuning Crystallinity and Surface Hydrophobicity of a Cobalt Phosphide Cocatalyst to Boost CO 2 Photoreduction Performance. ChemSusChem 2021, 115 https://doi.org/10.1002/cssc.202002755
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  9. Philipp Zimmermann, Deniz Ar, Marie Rößler, Patrick Holze, Beatrice Cula, Christian Herwig, Christian Limberg. Selective Transformation of Nickel‐Bound Formate to CO or C−C Coupling Products Triggered by Deprotonation and Steered by Alkali‐Metal Ions. Angewandte Chemie International Edition 2021, 60 (5) , 2312-2321. https://doi.org/10.1002/anie.202010180
  10. Minglun Cheng, Xiongfei Zhang, Yong Zhu, Mei Wang. Selective photocatalytic reduction of CO2 to CO mediated by a [FeFe]-hydrogenase model with a 1,2-phenylene S-to-S bridge. Chinese Journal of Catalysis 2021, 42 (2) , 310-319. https://doi.org/10.1016/S1872-2067(20)63644-0
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  13. Hao-Lin Wu, Xu-Bing Li, Chen-Ho Tung, Li-Zhu Wu. Bioinspired metal complexes for energy-related photocatalytic small molecule transformation. Chemical Communications 2020, 56 (99) , 15496-15512. https://doi.org/10.1039/D0CC05870J
  14. Jia‐Wei Wang, Jia‐Kai Sun, Dong‐Cheng Liu, Long Jiang. Visible‐Light‐Driven CO 2 Reduction Catalyzed by a Dinuclear Nickel Complex. European Journal of Inorganic Chemistry 2020, 2020 (47) , 4450-4453. https://doi.org/10.1002/ejic.202000816
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  16. Li-Qi Qiu, Kai-Hong Chen, Zhi-Wen Yang, Liang-Nian He. A rhenium catalyst with bifunctional pyrene groups boosts natural light-driven CO 2 reduction. Green Chemistry 2020, 22 (24) , 8614-8622. https://doi.org/10.1039/D0GC03111A
  17. Yusuke Kuramochi, Akiharu Satake. Photocatalytic CO 2 Reductions Catalyzed by meso ‐(1,10‐Phenanthrolin‐2‐yl)‐Porphyrins Having a Rhenium(I) Tricarbonyl Complex. Chemistry – A European Journal 2020, 26 (69) , 16365-16373. https://doi.org/10.1002/chem.202002558
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  19. Linnan Chen, Xuanwei Wang, Yawen Chen, Zanyong Zhuang, Fei-Fei Chen, Ying-Jie Zhu, Yan Yu. Recycling heavy metals from wastewater for photocatalytic CO2 reduction. Chemical Engineering Journal 2020, 402 , 125922. https://doi.org/10.1016/j.cej.2020.125922
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