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A sulfur-modified mof-derived metal-doped porous carbon material and its preparation method and application

A technology of porous carbon material and metal doping, applied in the direction of fuel cell half-cells and secondary battery-type half-cells, fuel cell-type half-cells and primary battery-type half-cells, structural parts, etc., can solve Reduce catalyst selectivity, reduce energy utilization efficiency and stability of zinc-air batteries, etc., achieve high half-wave potential, high peak potential, and easy-to-control conditions

Active Publication Date: 2022-07-26
ZHEJIANG UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004] In order to overcome the existence of 2e in traditional MOF-derived metal-doped porous carbon materials, the present invention - ORR reaction, will reduce the catalyst for 4e - The selectivity of ORR, thereby reducing the energy utilization efficiency and stability of zinc-air batteries, provides a sulfur-modified MOF-derived metal-doped porous carbon material and its preparation method. This method has easy-to-obtain raw materials and simple operation. No special requirements for equipment, easy to industrialize

Method used

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  • A sulfur-modified mof-derived metal-doped porous carbon material and its preparation method and application
  • A sulfur-modified mof-derived metal-doped porous carbon material and its preparation method and application
  • A sulfur-modified mof-derived metal-doped porous carbon material and its preparation method and application

Examples

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Embodiment 1

[0028] A preparation method of a sulfur-modified MOF-derived metal-doped porous carbon material, comprising the following steps: Preparation of CoCuZn-MOF(111) precursor

[0029] Prepare a mixed solution containing 0.1 mmol / L metal salt and 10 mmol / L 2-methylimidazole, and the metal salt is Co with a substance ratio of 1:1:1 2+ , Cu 2+ , Zn 2+ , where Co 2+ The substance ratio with 2-methylimidazole is 1:8; the reaction is carried out at 25°C for 24h. After the reaction, washed three times with deionized water, and dried in vacuum at 60 °C to obtain a cuboctahedral CoCuZn-MOF (111) precursor with uniform size. The XRD pattern is as follows figure 1 shown.

[0030] Cu-Co-N 4 (111) Preparation of composite materials

[0031] The CoCuZn-MOF (111) precursor obtained above is annealed at a temperature of 800 °C, a heating rate of 3 °C / min, and an annealing time of 3 h. During the high-temperature annealing process, Zn in the MOF will evaporate, thereby obtaining porous MOF-d...

Embodiment 2

[0037] A preparation method of a sulfur-modified MOF-derived metal-doped porous carbon material, comprising the following steps:

[0038] (1) Preparation of CoCuZn-MOF(253) precursor

[0039] Prepare a mixed solution containing 0.1 mmol / L metal salt and 10 mmol / L 2-methylimidazole, and the metal salt is Co with a substance ratio of 2:5:3. 2+ , Cu 2+ , Zn 2+ , where Co 2+ The material ratio with 2-methylimidazole was 1:8; the reaction was performed at 0 °C for 24 h. After the reaction, it was washed three times with deionized water and dried under vacuum at 60 °C to obtain a regular dodecahedral CoCuZn-MOF (253) precursor with uniform size. The XRD pattern is as follows figure 1 shown.

[0040] (2)Cu-Co-N 4 (253) Preparation of composite materials

[0041] The CoCuZn-MOF (253) precursor obtained above was annealed at a temperature of 700 °C, a heating rate of 1 °C / min, and an annealing time of 2 h. During the high-temperature annealing process, Zn in the MOF would evapor...

Embodiment 3

[0047] A preparation method of a sulfur-modified MOF-derived metal-doped porous carbon material, comprising the following steps:

[0048] (1) Preparation of CoCuZn-MOF(523) precursor

[0049] Prepare a mixed solution containing 0.1 mmol / L metal salt and 10 mmol / L 2-methylimidazole, the metal salt is Co with a substance ratio of 5:2:3 2+ , Cu 2+ , Zn 2+ , where Co 2+ The material ratio with 2-methylimidazole is 1:8; the reaction is carried out at 50°C for 12h. After the reaction, it was washed three times with deionized water and dried in vacuum at 60 °C to obtain a cuboctahedral CoCuZn-MOF (523) precursor with uniform size. The XRD pattern is as follows figure 1 shown.

[0050] (2)Cu-Co-N 4 (523) Preparation of composite materials

[0051] The CoCuZn-MOF (523) precursor obtained above is annealed at a temperature of 1000 °C, a heating rate of 5 °C / min, and an annealing time of 4 h. During the high temperature annealing process, Zn in the MOF will evaporate, thereby obta...

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Abstract

The invention relates to the technical field of composite electrode materials, and for traditional MOF-derived metal-doped porous carbon materials, there are 2e ‑ The problem of ORR reaction is to provide a sulfur-modified MOF-derived metal-doped porous carbon material and a preparation method thereof. First, a mixed solution containing a metal salt and 2-methylimidazole is prepared, and the metal ions of the metal salt include Co 2+ , Cu 2+ , Zn 2+ , reacted to obtain CoCuZn-MOF precursor; then annealed to obtain Cu-Co-N 4 Derived carbon-based composite material, that is, MOF-derived metal-doped porous carbon material; followed by vulcanization treatment to introduce sulfur. The method is easy to obtain raw materials, simple to operate, has no special requirements for equipment, and is easy to industrialize. The present invention also provides the application of the sulfur-modified MOF-derived metal-doped porous carbon material in a zinc-air battery.

Description

technical field [0001] The invention relates to the technical field of composite electrode materials, in particular to a sulfur-modified MOF-derived metal-doped porous carbon material and a preparation method and application thereof. Background technique [0002] The oxygen reduction reaction (ORR) can proceed through two reaction pathways, namely the two-electron oxygen reduction reaction (2e - ORR) and the four-electron oxygen reduction reaction (4e - ORR), where 4e - ORR is usually used in fuel cells, metal-air batteries and other fields. but 4e - The ORR is kinetically very slow, the large overpotential severely limits the energy efficiency of Zn-air batteries, and more importantly 2e - ORR and 4e - The two ORRs are competitive responses to each other. Therefore, how to effectively regulate the response to 4e - ORR path to boost 4e - The reactivity and selectivity of the ORR process, thereby improving the energy utilization efficiency and stability of Zn-air batt...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): H01M4/86H01M4/96H01M12/06H01M12/08
CPCH01M4/8647H01M4/96H01M12/06H01M12/08
Inventor 郑冬冯锦秀曹澥宏刘文贤
Owner ZHEJIANG UNIV OF TECH
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