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Photocatalytic hydrogen-production system containing polycarbonyl diiron disulfur cluster compound modified by polymer polyethylenimine as well as preparation method of polycarbonyl diiron disulfur cluster compound and hydrogen-production method

A technology of polycarbonyl diiron disulfide clusters and polyethyleneimine, applied in the direction of organic compound/hydride/coordination complex catalysts, chemical instruments and methods, physical/chemical process catalysts, etc., can solve the problem of loss of catalytic activity, Problems such as catalyst instability, catalytic hydrogen production efficiency and low stability, etc., to achieve high stability, low-cost and easy-to-obtain components, and high hydrogen production efficiency

Active Publication Date: 2015-03-18
TECHNICAL INST OF PHYSICS & CHEMISTRY - CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004] The above research results are of great significance for the development of photocatalytic hydrogen production systems, but these systems generally have the following problems: first, the catalyst is unstable under light conditions, and most photocatalytic hydrogen production systems lose their catalytic activity after 10 hours of light; Second, the efficiency and stability of catalytic hydrogen production are not high, and the pH value of the system before light is mostly between 4.0 and 5.0 or under alkaline (pH=10) conditions, but under near-neutral conditions (pH=6 The photocatalytic hydrogen production system of ~7) efficient, stable and long-lived iron hydrogenase has not been reported in the literature

Method used

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  • Photocatalytic hydrogen-production system containing polycarbonyl diiron disulfur cluster compound modified by polymer polyethylenimine as well as preparation method of polycarbonyl diiron disulfur cluster compound and hydrogen-production method
  • Photocatalytic hydrogen-production system containing polycarbonyl diiron disulfur cluster compound modified by polymer polyethylenimine as well as preparation method of polycarbonyl diiron disulfur cluster compound and hydrogen-production method
  • Photocatalytic hydrogen-production system containing polycarbonyl diiron disulfur cluster compound modified by polymer polyethylenimine as well as preparation method of polycarbonyl diiron disulfur cluster compound and hydrogen-production method

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0047] A photocatalytic hydrogen production system containing PEI-modified polycarbonyl diiron disulfide cluster compounds: Among them, the concentration of water-soluble PEI-modified polycarbonyl diiron disulfide cluster polymers based on polycarbonyl diiron disulfide clusters: 1.46× 10 -6 M; CdSe quantum dot concentration: 0.08mg / mL; ascorbic acid (H 2 A) Concentration: 0.125M; the size of MPA-CdSe QDs is 2.5nm; the solvent is water; the total sample volume is 10ml; the pH of the sample before illumination is 6.5.

[0048] The method for preparing hydrogen by using the above photocatalytic hydrogen production system is: irradiate the sample with visible light of λ=410nm, and monitor the hydrogen production of the sample by TCD gas spectrometry; after 44 hours of light, the calculated hydrogen production of the sample is about 3.5mL (TON= 10607); the sample continued to produce hydrogen in the first 36 hours, indicating that the system was stable during the first 36 hours of...

Embodiment 2

[0053] A photocatalytic hydrogen production system containing PEI-modified polycarbonyl diiron disulfide cluster compounds: Among them, the concentration of water-soluble PEI-modified polycarbonyl diiron disulfide cluster polymers based on polycarbonyl diiron disulfide clusters: 1.46× 10 -6 M; CdSe quantum dot concentration: 0.08mg / mL; ascorbic acid (H 2 A) Concentration: 0.125M; the size of MPA-CdSe QDs is 2.5nm; the solvent is water; the total sample volume is 10ml; the pH of the sample before illumination is 4.0.

[0054] The method for preparing hydrogen by using the above photocatalytic hydrogen production system is: irradiate the sample with visible light of λ=410nm, and monitor the sample by gas spectrometer every 1 or 2 hours of light; after 7 hours of light, the calculated hydrogen production of the sample is about 1.4 mL (TON=4217); the sample continued to produce hydrogen in the first 5 hours, indicating that the system was stable during the first 5 hours of light....

Embodiment 3

[0057] A photocatalytic hydrogen production system containing PEI-modified polycarbonyl diiron disulfide cluster compounds: Among them, the concentration of water-soluble PEI-modified polycarbonyl diiron disulfide cluster polymers based on polycarbonyl diiron disulfide clusters: 1.46× 10 -6 M; CdSe quantum dot concentration: 0.08mg / mL; ascorbic acid (H 2 A) Concentration: 0.125M; the size of MPA-CdSe QDs is 2.5nm; the solvent is water; the total sample volume is 10ml; the pH of the sample before illumination is 9.5.

[0058] The method of preparing hydrogen by using the above photocatalytic hydrogen production system is: irradiate the sample with visible light of λ=410nm, and monitor the hydrogen production of the sample by TCD gas spectrometry; after 26 hours of light, the calculated hydrogen production of the sample is about 1.8mL (TON= 5282); the sample continued to produce hydrogen in the first 22 hours, indicating that the system was stable during the first 22 hours of l...

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Abstract

The invention discloses a photocatalytic hydrogen-production system containing a polycarbonyl diiron disulfur cluster compound modified by polymer polyethylenimine. The photocatalytic hydrogen-production system comprises the polycarbonyl diiron disulfur cluster compound modified by polymer polyethylenimine, a photosensitizer, an electronic sacrificial agent and an aqueous solvent. The invention also discloses a preparation method of the polycarbonyl diiron disulfur cluster compound covalently modified by polymer polyethylenimine and a hydrogen-production method by constructing the system through the compound. By the photocatalytic hydrogen-production system disclosed by the invention, hydrogen production can be efficiently performed, especially under neutral condition, the hydrogen-production efficiency under illumination is high, the system has high stability, based on the total volume of the system being 10mL, the hydrogen-production amount each time can reach up to 155mu mol, the hydrogen conversion rate calculated based on the catalyst is up to 10,607 and the composition of the system is cheap and easily available.

Description

technical field [0001] The invention relates to a photocatalytic hydrogen production system, a preparation method and a method for preparing hydrogen by using the photocatalytic system, in particular to a photocatalytic hydrogen production containing polycarbonyl diiron disulfide cluster compound modified by polymer polyethyleneimine System, preparation method and method for preparing hydrogen. Background technique [0002] The production of hydrogen by splitting water with sunlight is one of the most ideal methods to solve the energy crisis faced by human beings, because the solar energy involved in the whole reaction process is inexhaustible, and the water reserves on the earth are abundant and the cost is low. After hydrogen is utilized as an energy carrier, the product is water. The process is clean and the result is environmentally friendly. Water can enter the next process of photo-splitting water, forming a closed energy cycle. [0003] Iron hydrogenase is an active ...

Claims

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Application Information

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IPC IPC(8): C01B3/02B01J31/22C08G73/04
Inventor 吴骊珠梁文静王锋简经鑫佟振合
Owner TECHNICAL INST OF PHYSICS & CHEMISTRY - CHINESE ACAD OF SCI
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