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Full-pH electrocatalytic hydrogen evolution molybdenum disulfide modified sulfur and molybdenum co-doped graphite-phase carbon nitride heterostructure material, and preparation method thereof

A graphite-phase carbon nitride and molybdenum disulfide technology is applied in electrodes, electrolytic processes, electrolytic components, etc., which can solve the problems of limited industrial use, difficult reaction, and low catalytic activity of catalysts, and achieve excellent electrocatalytic hydrogen evolution activity, high Atom utilization efficiency, effect of improving catalytic activity

Active Publication Date: 2021-04-13
SHAANXI UNIV OF SCI & TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004]However, the high potential required for electrocatalytic hydrogen evolution reaction in alkaline electrolyte aqueous solution is compared with that in acidic aqueous electrolyte solution, due to the initial adsorption of H2O dissociation is slow, the reaction is difficult, and the Volmer process related to H2O dissociation always inhibits the hydrogen formation / desorption process, so lead to low catalytic activity of the catalyst in alkaline electrolyte aqueous solution
[0005]In recent years, non-metallic layered graphitic carbon nitride materials have been widely used due to their abundant N ligands, tunable active sites and excellent stability. As a metal-free catalyst carrier, it is widely used in the fields of electrocatalytic water splitting and redox reaction, but its low conductivity and low dissociation efficiency limit its industrial application.

Method used

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Embodiment 1

[0036] The invention provides a method for preparing a molybdenum disulfide modified sulfur and molybdenum co-doped graphite phase carbon nitride heterostructure material with full pH electrocatalytic hydrogen evolution, comprising the following steps:

[0037] Step 1: Dissolve 1g of melamine and 0.05g of thiourea in 20mL of deionized water in turn, stir for 1.5h at a water bath temperature of 60°C, take out the mixed solution and put it in an oven, and dry it at 60°C to obtain a reaction precursor mixture a.

[0038] Step 2: Put the precursor mixture A in an alumina porcelain boat, and then place the porcelain boat in an atmosphere furnace for calcination. Before calcination, pass argon for 30 minutes, and then heat up at a rate of 2.3°C / min under argon The temperature was raised from room temperature to 500° C. for 3 h, and after the calcination was completed, the furnace was cooled to room temperature, and the intermediate product B was obtained by grinding.

[0039] Step ...

Embodiment 2

[0044] The invention provides a method for preparing a molybdenum disulfide modified sulfur and molybdenum co-doped graphite phase carbon nitride heterostructure material with full pH electrocatalytic hydrogen evolution, comprising the following steps:

[0045] Step 1: Dissolve 1g of melamine and 0.05g of thiourea in 30mL of deionized water in turn, stir for 1 hour at a water bath temperature of 80°C, take out the mixed solution and put it in an oven, and dry it at 60°C to obtain a reaction precursor mixture A .

[0046] Step 2: Put the precursor mixture A in an alumina porcelain boat, and then place the porcelain boat in an atmosphere furnace for calcination. Before calcination, pass argon for 30 minutes, and then heat up at a rate of 2.3°C / min under argon The temperature was raised from room temperature to 550° C. for 4 h, and after the calcination, the furnace was cooled to room temperature, and the intermediate product B was obtained by grinding.

[0047] Step 3: Add 1 g ...

Embodiment 3

[0052] The invention provides a method for preparing a molybdenum disulfide modified sulfur and molybdenum co-doped graphite phase carbon nitride heterostructure material with full pH electrocatalytic hydrogen evolution, comprising the following steps:

[0053] Step 1: Dissolve 1g of melamine and 0.05g of thiourea in 40mL of deionized water in turn, stir for 1 hour at a water bath temperature of 90°C, take out the mixed solution and put it in an oven, and dry it at 60°C to obtain a reaction precursor mixture A .

[0054] Step 2: Put the precursor mixture A in an alumina porcelain boat, and then place the porcelain boat in a tube furnace for calcination. Before calcination, pass argon for 30 minutes, and then raise the temperature at 3°C / min under argon The rate was raised from room temperature to 600°C for 4 hours of calcination. After the calcination was completed, it was cooled to room temperature with the furnace and ground to obtain the intermediate product B.

[0055] St...

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Abstract

The invention discloses a full-pH electrocatalytic hydrogen evolution molybdenum disulfide modified sulfur and molybdenum co-doped graphite-phase carbon nitride heterostructure material and a preparation method thereof. Firstly, melamine is taken as a precursor for synthesizing graphite-phase carbon nitride, and ammonium molybdate and thiourea are taken as metal sources; in the melamine polycondensation process, non-metallic elements are introduced through a two-step heat treatment method, metal atoms are anchored, generation of by-products is avoided, and the doping effect is adjusted by adjusting the adding proportion of metal and non-metal precursors; secondly, uniform growth of molybdenum disulfide nanosheets at nucleation sites on the surface of the substrate and strong coupling of the molybdenum disulfide nanosheets and a sulfur and molybdenum co-doped graphite phase carbon nitride material are realized by controlling the proportions of ammonium molybdate, thiourea and sulfur and molybdenum co-doped graphite phase carbon nitride by adopting a hydrothermal method. The method disclosed by the invention is simple to operate and good in repeatability, the formation and regulation of the structure can be efficiently realized, the effective transfer of active sites under different pH values can be realized, and the efficient proceeding of the electro-catalytic hydrogen evolution reaction is realized.

Description

technical field [0001] The invention belongs to the technical field of electrocatalytic materials, and in particular relates to a molybdenum disulfide modified sulfur and molybdenum co-doped graphite phase carbon nitride heterostructure material and a preparation method thereof for full pH electrocatalytic hydrogen evolution. Background technique [0002] Hydrogen production by electrolysis of water is a convenient way to produce hydrogen. The specific operation is to pass direct current into the electrolytic cell filled with aqueous electrolyte solution, and the water molecules will electrochemically react on the electrodes to decompose into hydrogen and oxygen. Among them, the electrolyte in the aqueous electrolyte solution includes acidic electrolytes, such as sulfuric acid, and alkaline electrolytes, such as sodium hydroxide and potassium hydroxide. In order to accelerate the reaction of charge transfer on the electrode and electrolyte interface, a catalyst is usually add...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C25B11/091C25B1/04
CPCC25B1/04Y02E60/36
Inventor 李军奇张贝祎庞凌燕刘俊莉刘辉
Owner SHAANXI UNIV OF SCI & TECH
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