Monatomic catalytic material NiPc-MPOP for high-efficiency photocatalytic reduction of carbon dioxide and preparation method thereof

A photocatalytic material, carbon dioxide technology, applied in the fields of carbon monoxide, chemical instruments and methods, catalytic reactions, etc., can solve the problems of uncontrollable catalytic site microenvironment, inability to fully explore the impact of SACs catalytic performance, and easy catalyst deactivation.

Active Publication Date: 2021-07-09
ZHENGZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

However, the current preparation of SACs has problems such as cumbersome synthesis process, uncontrollable microenvironment of catalytic sites, and easy deactivation of catalysts.
At the same time, du...

Method used

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  • Monatomic catalytic material NiPc-MPOP for high-efficiency photocatalytic reduction of carbon dioxide and preparation method thereof
  • Monatomic catalytic material NiPc-MPOP for high-efficiency photocatalytic reduction of carbon dioxide and preparation method thereof
  • Monatomic catalytic material NiPc-MPOP for high-efficiency photocatalytic reduction of carbon dioxide and preparation method thereof

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Experimental program
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Embodiment 1

[0023] Embodiment 1: Synthesis of NiPc-MPOP material of the present invention

[0024] 2,3,9,10,16,17,23,24-Nickel(II) octaaminophthalocyanine (13.8 mg, 0.02 mmol) and 2,6-diformylphenol (12 mg, 0.08 mmol) were added to N , in a mixed solvent of N-dimethylacetamide and mesitylene (v / v=3:2, 1 mL), the resulting mixture was sonicated for three minutes, and aniline (44 μL, 0.48 mmol) and 6.0 M aqueous acetic acid ( 0.2mL), sealed in a polytetrafluoroethylene reactor, and subjected to solvothermal reaction at 150°C for 7 days. After cooling to room temperature, the dark green single-center single-atom material NiPc-2HPOP was obtained by centrifugation, washing and drying. Add NiPc-2HPOP (100 mg) to Ni(OAc) 2 4H 2 O or Co(OAc) 2 4H 2 O in a saturated methanol solution (100 mL), stirred at room temperature for 3 days, centrifuged, washed, and dried to obtain dark green double-center single-atom material NiPc-NiPOP powder or NiPc-CoPOP powder. The material has good thermal stab...

Embodiment 2

[0032] Example 2: Photocatalytic CO by NiPc-MPOP 2 RR test

[0033] Photocatalytic CO 2 Reduction experiments were performed in 60 mL custom-made quartz reaction vials. According to a typical photocatalytic system, terpyridine ruthenium chloride ([Ru(bpy) 3 ] Cl 2 ), triethanolamine (TEOA) and the inventive material are used as photosensitizer, electron donor and catalyst, and accurately weighed photosensitizer (10mg), catalyst (2mg) are added in the reaction bottle. After adding 8 mL of acetonitrile and 2 mL of TEOA, the mouth of the reaction bottle was sealed with a silica gel stopper, and sealed again with a parafilm to ensure the airtightness of the reaction system. Ultrasonic the mixture for 3 to 5 minutes to disperse the components in the system evenly, and pass CO into the system for half an hour 2 gas to completely remove the air and make the CO 2 reaches saturation. White LED (400nm≤λ≤800nm) is used as light source for photocatalytic reaction. Absorb the upper...

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Abstract

The invention belongs to the crossing field of porous organic polymer materials and catalytic chemistry, and discloses a novel carbon dioxide reduction photocatalyst and a preparation method thereof. A series of porous organic polymers NiPc-MPOP which simultaneously contain M-N4 and M-N2O2 monatomic sites are designed and prepared. The polymer not only can synergistically improve the catalytic efficiency, but also provides a more direct opportunity to recognize the activity of a metal center. The photo-reduction result of CO2 shows that excellent CO generation capability (7.77 mmol g <-1 >) can be realized by introducing a catalytic center with Ni-N2O2 into an original phthalocyanine-based Ni-N4 framework, and the selectivity of H2 is as high as 96%. In combination with control experiments and theoretical researches, compared with the traditional Ni-N4 part, the Ni-N2O2 part is proved to be a part with higher CO2RR activity. By changing the coordination environment, the more effective monatomic catalyst is designed, and a new thought and theoretical basis are provided for design and synthesis of the efficient monatomic catalyst.

Description

technical field [0001] The invention belongs to the intersection field of porous organic polymer materials and catalytic chemistry, and specifically relates to a novel carbon dioxide reduction photocatalyst and a preparation method thereof. Background technique [0002] The combustion of fossil fuels (oil, coal, and natural gas) is often accompanied by a large amount of greenhouse gas (GHG) emissions, most of which are carbon dioxide (CO 2 ) into the atmosphere. Continued consumption of finite fossil fuels and CO 2 Excessive emissions have led to major problems such as energy shortages and the greenhouse effect. Therefore, utilizing solar energy or renewable electricity to convert CO 2 Conversion to carbon monoxide (CO) and other value-added chemicals (methane, methanol, formic acid, ethanol, etc.) has become a research hotspot in the field of energy catalysis. This strategy not only reduces atmospheric CO 2 content, alleviate the adverse effects of the greenhouse effec...

Claims

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Application Information

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IPC IPC(8): B01J31/22B01J35/10C01B32/40
CPCB01J31/2213B01J31/1815B01J35/004B01J35/1004C01B32/40B01J2531/845B01J2531/847B01J2231/625
Inventor 臧双全王珊王乾有董晓玉
Owner ZHENGZHOU UNIV
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