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Phosphorus-doped ultrathin hollow carbon nitride nanosphere catalyst for hydrogen production by efficient photocatalytic cracking of water

A technology of photocatalysis and carbon nitride, applied in the direction of physical/chemical process catalysts, hydrogen production, nitrogen compounds, etc. High charge recombination rate, etc., to achieve excellent activity and stability, cheap raw materials, and simple preparation process

Active Publication Date: 2021-04-30
BEIJING UNIV OF TECH
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

At present, the main problems include: (1) the specific surface area of ​​the catalyst is low; (2) the response to visible light is weak; (3) the charge recombination rate is high
[0004] At the same time, through literature research, it was found that there is no report on the preparation of this kind of phosphorus-doped ultra-thin hollow carbon nitride nanosphere catalyst and its application in photocatalytic water splitting to produce hydrogen.

Method used

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  • Phosphorus-doped ultrathin hollow carbon nitride nanosphere catalyst for hydrogen production by efficient photocatalytic cracking of water
  • Phosphorus-doped ultrathin hollow carbon nitride nanosphere catalyst for hydrogen production by efficient photocatalytic cracking of water
  • Phosphorus-doped ultrathin hollow carbon nitride nanosphere catalyst for hydrogen production by efficient photocatalytic cracking of water

Examples

Experimental program
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Embodiment 1

[0019] Embodiment 1: According to Synthesis of SiO 2 template. The specific process is as follows: at 35°C, add 9 mL of ammonia water to a mixture of 150 mL of ethanol and 20 mL of deionized water, and stir magnetically for 1 hour to obtain a transparent precursor solution; under vigorous stirring, 11 mL of tetraethyl orthosilicate (TEOS ) was quickly added to the above precursor solution, and stood for 1h to obtain a white suspension; then, under vigorous stirring, 12.5mL tetraethyl orthosilicate (TEOS) and 6mL octadecyltrimethoxysilane (C 18 The mixed solution of TMOS) was added dropwise to the above suspension, and left to stand at room temperature for 3h; the resulting reaction solution was centrifuged, dried and roasted, and the roasting program was: the rate of 5 ° C / min was raised from room temperature to 550 ° C , kept warm for 6h, then cooled to room temperature to obtain a white solid; the above sample was acidified with 1M HCl solution at 80°C for 24h; finally ...

Embodiment 2

[0020] Example 2: Preparation of hollow carbon nitride nanospheres (H-CNS) by negative pressure ultrasonic method. The specific steps are as follows: 1gSiO 2 The template and 5 mL of cyanamide were mixed in a pressure-resistant bottle connected to a vacuum tube, and were subjected to ultrasonic treatment at 60 °C for 3 h and magnetic stirring at 80 °C for 3 h; then the sample was dried and calcined in a tube furnace, the roasting procedure was as follows: N 2 Under the atmosphere, the rate was raised from room temperature to 550 °C at a rate of 5 °C / min, kept for 2 hours, and finally cooled to room temperature to obtain a yellow sample; the ground sample was washed with 4M NH 4 HF 2 Treat at room temperature for 12h to remove SiO 2 Template; centrifuged and washed with distilled water and ethanol, dried at 60°C to obtain hollow carbon nitride nanospheres (H-CNS).

Embodiment 3

[0021] Example 3: A phosphorus-doped ultrathin hollow carbon nitride nanosphere (x wt% P / UH-CNS, x=0-10) catalyst was prepared by chemical vapor deposition. The specific steps are as follows: add 300mg of H-CNS powder, 3mg of iodine and a certain amount (1-10wt%) of purified red phosphorus into a quartz ampoule, vacuumize and seal it with an acetylene flame; Heating at a rate of 450°C for 4 hours; cooling at a rate of 1°C / min to 280°C and holding for 4 hours; then cooling slowly to room temperature at a rate of 0.2°C / min; 2 , washed with distilled water and ethanol, and dried at 60°C to obtain x wt% P / UH-CNS (x=0-10) catalyst.

[0022] The present invention has the characteristics of simple preparation process, cheap raw material price, high yield, regular and controllable product appearance, etc. The 2wt% P / UH-CNS catalyst prepared by the present invention exhibits excellent photocatalytic cracking water hydrogen production activity .

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Abstract

The invention discloses a phosphorus-doped ultrathin hollow carbon nitride nanosphere catalyst for hydrogen production by efficient photocatalytic cracking of water, and belongs to the field of catalytic chemistry and nanoscience. The catalyst is prepared according to the following steps: firstly, by taking tetraethyl orthosilicate and octadecyltrimethoxysilane as precursors and ethanol, ammonia water and water as solvents, preparing a SiO2 template by utilizing a method; then taking cyanamide as a precursor, and preparing a hollow carbon nitride nanosphere (H-CNS) carrier through a negative pressure ultrasonic method; and finally, with red phosphorus as a phosphorus source and a chemical vapor deposition method, depositing phosphorus atoms on the H-CNS carrier, so as to obtain the phosphorus-doped P / UH-CNS composite catalyst. In the preparation process, the pressure difference generated on the inner surface and the outer surface of the H-CNS carrier can thin the shell of the originally loose H-CNS carrier. The material is novel, the preparation process is simple, the product morphology is regular and controllable, and the catalyst shows good photocatalytic hydrogen production activity and stability.

Description

technical field [0001] The invention relates to a phosphorus (P)-doped ultra-thin hollow carbon nitride nanosphere (UH-CNS) catalyst for efficient photocatalytic cracking of water to produce hydrogen. The present invention uses cyanamide and red phosphorus as precursors to prepare hollow carbon nitride nanospheres (H-CNS) and phosphorus-doped ultrathin hollow carbon nitride nanospheres ( P / UH-CNS), and finally achieve efficient photocatalytic water splitting to hydrogen production. It belongs to the field of catalytic chemistry and nanoscience. Background technique [0002] Since the 21st century, with the rapid development of society and economy, the excessive dependence of the industrial economy on fossil energy has led to the continuous consumption of fossil fuels in the earth, and the energy crisis and environmental pollution have become the focus of the world. Solar energy is an inexhaustible renewable energy. At the same time, hydrogen energy also has the advantages ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24C01B3/04C01B21/082B82Y40/00
CPCB01J27/24C01B3/042C01B21/0605B82Y40/00C01B2203/1088C01P2004/34B01J35/39B01J35/51Y02E60/36
Inventor 邓积光吕思洁敬林戴洪兴刘雨溪李双王治伟
Owner BEIJING UNIV OF TECH
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