Harnessing Visible Light for CO<sub>2</sub> Conversion: The Role of Highly Reduced Phosphomolybdate Crystals as Powerful Photocatalysts

Heterogeneous photocatalysts, characterized by well-defined atomic structures and the capacity for rapid, directional electron transfer, are pivotal in the exploration and development of highly efficient systems for visible-light-driven diluted CO<sub>2</sub> reduction. Herein, we constructed highly reduced phosphomolybdates crystalline materials <b>1</b>-<b>3</b> to help this process, with the formula of [Co<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>][Co<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>(H<sub>2</sub>O)<sub>2</sub>][Co(H<sub>7</sub>P<sub>4</sub>Mo<sub>6</sub>O<sub>31</sub>)<sub>2</sub>]·8H<sub>2</sub>O (<b>1</b>), [Ni<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>(H<sub>2</sub>O)<sub>2</sub>][Ni<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>][Ni(H<sub>2</sub>O)<sub>4</sub>][Ni(H<sub>6</sub>P<sub>4</sub>Mo<sub>6</sub>O<sub>31</sub>)<sub>2</sub>]·3H<sub>2</sub>O·2C<sub>2</sub>H<sub>5</sub>OH (<b>2</b>), and [Zn<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>2</sub>][Zn<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>][Zn<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>2</sub>(H<sub>2</sub>O)<sub>2</sub>][Zn(H<sub>5</sub>P<sub>4</sub>Mo<sub>6</sub>O<sub>31</sub>)<sub>2</sub>] (<b>3</b>) [C<sub>8</sub>N<sub>3</sub>H<sub>7</sub> = 2-(1H-pyrazol-3-yl)pyridine]. Specifically, catalyst <b>1</b> demonstrated a CO production rate of 3276.4 μmol g<sup>-1</sup> h<sup>-1</sup> in an environment with 20% CO<sub>2</sub> concentration, and an impressively elevated rate of 10740.3 μmol g<sup>-1</sup> h<sup>-1</sup> in a pure CO<sub>2</sub> atmosphere. Steady-state photoluminescence spectroscopy revealed that the directional migration of photoelectrons from the Ru complexes to the catalyst was instrumental in enhancing the catalytic activity. This study provides valuable insights into the rational operation of low-concentration CO<sub>2</sub> conversion treatment and the design and synthesis of photocatalysts.

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Journal
Inorganic Chemistry
Published
2024-10-25
DOI
https://doi.org/10.1021/acs.inorgchem.4c03810
Citations
1
Primary Topic
Advanced Photocatalysis Techniques
Type
article
Field-Weighted Citation Impact
0.10

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article

Harnessing Visible Light for CO2 Conversion: The Role of Highly Reduced Phosphomolybdate Crystals as Powerful Photocatalysts

Yan Xu, Hua Mei, Jianbo Yang, Yin-Hua Zhu et al.
1 citations
Inorganic Chemistry
Advanced Photocatalysis Techniques
0.10
article

Harnessing Visible Light for CO2 Conversion: The Role of Highly Reduced Phosphomolybdate Crystals as Powerful Photocatalysts

Yan Xu, Hua Mei, Jianbo Yang, Yin-Hua Zhu, Zhiming Dong
article en
1 citations

Abstract

Heterogeneous photocatalysts, characterized by well-defined atomic structures and the capacity for rapid, directional electron transfer, are pivotal in the exploration and development of highly efficient systems for visible-light-driven diluted CO<sub>2</sub> reduction. Herein, we constructed highly reduced phosphomolybdates crystalline materials <b>1</b>-<b>3</b> to help this process, with the formula of [Co<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>][Co<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>(H<sub>2</sub>O)<sub>2</sub>][Co(H<sub>7</sub>P<sub>4</sub>Mo<sub>6</sub>O<sub>31</sub>)<sub>2</sub>]·8H<sub>2</sub>O (<b>1</b>), [Ni<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>(H<sub>2</sub>O)<sub>2</sub>][Ni<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>][Ni(H<sub>2</sub>O)<sub>4</sub>][Ni(H<sub>6</sub>P<sub>4</sub>Mo<sub>6</sub>O<sub>31</sub>)<sub>2</sub>]·3H<sub>2</sub>O·2C<sub>2</sub>H<sub>5</sub>OH (<b>2</b>), and [Zn<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>2</sub>][Zn<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>4</sub>][Zn<sub>2</sub>(C<sub>8</sub>N<sub>3</sub>H<sub>7</sub>)<sub>2</sub>(H<sub>2</sub>O)<sub>2</sub>][Zn(H<sub>5</sub>P<sub>4</sub>Mo<sub>6</sub>O<sub>31</sub>)<sub>2</sub>] (<b>3</b>) [C<sub>8</sub>N<sub>3</sub>H<sub>7</sub> = 2-(1H-pyrazol-3-yl)pyridine]. Specifically, catalyst <b>1</b> demonstrated a CO production rate of 3276.4 μmol g<sup>-1</sup> h<sup>-1</sup> in an environment with 20% CO<sub>2</sub> concentration, and an impressively elevated rate of 10740.3 μmol g<sup>-1</sup> h<sup>-1</sup> in a pure CO<sub>2</sub> atmosphere. Steady-state photoluminescence spectroscopy revealed that the directional migration of photoelectrons from the Ru complexes to the catalyst was instrumental in enhancing the catalytic activity. This study provides valuable insights into the rational operation of low-concentration CO<sub>2</sub> conversion treatment and the design and synthesis of photocatalysts.

Inorganic ChemistryVol. 63(44)
Nanjing Tech University (CN), State Key Laboratory of Materials-Oriented Chemical Engineering
Nanjing Tech University
Openalex Percentile: Top 64%
Advanced Photocatalysis Techniques
0.10
DOISourceOpenAlex
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