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Preparation method and application of boron-nitrogen co-coordinated copper monatomic catalyst

A catalyst and atomic technology, which is applied in the field of preparation of boron-nitrogen co-coordinated copper single-atom catalysts, can solve the problems of difficult stable conversion, limited composition, loss of high selectivity of single-atom centers, etc., and achieves easy separation and less special equipment , the effect of step simplification

Active Publication Date: 2022-07-29
YANGTZE DELTA REGION INST OF UNIV OF ELECTRONICS SCI & TECH OF CHINE HUZHOU
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] Currently in CO 2 Copper (Cu) is widely used in the field of electrochemical reduction, but the coordination structure of Cu-based single-atom catalysts reported in the literature is limited, and most of them are Cu-N coordinated with nitrogen (N) or oxygen (O). or Cu-O structure, applied to CO 2 Most of the products obtained during electrochemical reduction are carbon monoxide (CO), and the activity of the catalyst is also very limited, making it difficult to achieve a stable conversion of CO at a large current density. 2 , under a large working current, the single-atom structure of the catalyst is also easy to migrate and agglomerate into nanoparticles, thus losing the high selectivity of the original single-atom center

Method used

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  • Preparation method and application of boron-nitrogen co-coordinated copper monatomic catalyst

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Embodiment 1

[0033] Preparation of BCN-Cu single-atom catalyst

[0034] (1) Add 20.02g of urea, 2.01g of PEG-2000, 599mg of boric acid, 102mg of copper nitrate trihydrate, and 170ml of deionized water into a 250ml volume round-bottomed flask, put it in an ultrasonic machine and mix well to obtain Mixture A. The mixture A was placed in an oil bath for heating and reflux, the stirring speed was 725 rpm, and the temperature of the oil bath was set to 118 o C, reacted for 12.5h, cooled to room temperature naturally after the reflux reaction, and obtained mixed solution B after ultrasonic uniformity;

[0035](2) Transfer the mixed solution B into the flask used for rotary evaporation, and perform the rotary evaporation operation. The temperature of the rotary evaporator is controlled to 52 o C, the rotating speed is set to 38 rpm, after 2.2 hours of rotary evaporation, the solvent is completely evaporated, and the gray solid is fully separated from the mixed solution. Remove the flask used f...

Embodiment 2

[0038] Preparation of BCN-Cu single-atom catalyst

[0039] (1) Add 19.95g of urea, 2.01g of PEG-2000, 602mg of boric acid, 100mg of copper nitrate trihydrate, and 180ml of deionized water into a 250ml volume round-bottomed flask, put it in an ultrasonic machine and mix well to obtain mixed solution A. The mixed solution A was placed in the oil bath pot for heating and refluxing, the stirring speed was 750 rpm, and the oil bath pot temperature was set to 121 o C, react for 12h, naturally cool to room temperature after the reflux reaction, and obtain mixed solution B after ultrasonic uniformity;

[0040] (2) Transfer the mixed solution B into the flask used for rotary evaporation, and perform the rotary evaporation operation. The temperature of the rotary evaporator is controlled to 49 o C, the rotating speed is set to 41 rpm, after rotary evaporation for 2 hours, the solvent is completely evaporated, and the gray solid is fully separated from the mixed solution. Remove the f...

Embodiment 3

[0043] Preparation of BCN-Cu single-atom catalyst

[0044] (1) Add 13.85g of cyanamide, 1.98g of PEG-2000, 605mg of boric acid, 97mg of copper nitrate trihydrate, and 170ml of deionized water into a 250ml volume round-bottomed flask, put it in an ultrasonic machine and mix thoroughly to obtain a mixed solution A . The mixed solution A was placed in an oil bath for heating and reflux, the stirring speed was 800 rpm, and the temperature of the oil bath was set to 125 rpm. o C, react for 11.5h, naturally cool to room temperature after the reflux reaction, and obtain mixed solution B after sonicating uniformly;

[0045] (2) Transfer the mixed solution B into the flask used for rotary evaporation, and perform the rotary evaporation operation. The temperature of the rotary evaporator is controlled to 50 o C, the rotating speed is set to 42 rpm, and after 2 hours of rotary evaporation, the solvent is completely evaporated, and the dark gray solid is fully separated out from the mi...

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Abstract

The invention discloses a preparation method and application of a boron-nitrogen co-coordinated copper monatomic catalyst, urea / cyanamide, PEG-2000, boric acid, copper nitrate trihydrate and deionized water are mixed according to a certain mass volume ratio, reflux heating is performed, cooling is performed, rotary evaporation is performed until a solvent is volatilized and solute is crystallized and separated out, crystals obtained through rotary evaporation are fully and uniformly ground, and the boron-nitrogen co-coordinated copper monatomic catalyst is obtained. According to the BCN-Cu catalyst, B and N co-coordinated Cu monatomic catalyst is obtained by fully pyrolyzing carbon nanotubes in a tubular furnace in an argon atmosphere, in the BCN-Cu catalyst, the B and N co-uniformly doped carbon nanotubes form a carrier BCN, and Cu is dispersed on the surface of the BCN carrier in an atomic scale. According to the BCN-Cu monatomic catalyst, Cu monatomic is stabilized through common coordination of B and N, the electronic structure of the center of the Cu monatomic is effectively adjusted, and the BCN-Cu monatomic catalyst shows excellent activity and methane selectivity in the CO2 electrochemical reduction reaction.

Description

technical field [0001] The invention relates to the technical field of metal single-atom catalysts, in particular to a preparation method and application of a boron-nitrogen co-coordinated copper single-atom catalyst. Background technique [0002] Current CO 2 There are many conversion methods, among which the electrochemical reduction method is due to mild reaction conditions (normal temperature, normal pressure), good controllability (the reaction activation energy on the electrode surface can be directly controlled by controlling the electrode reaction potential), and a wide range of energy sources (reduction process. The electricity demand can come from renewable energy such as solar energy, wind energy, geothermal energy and tidal energy) and the advantages of environmental friendliness have attracted much attention. [0003] in CO 2 Compared with bulk electrode materials, metal nanocatalysts have been widely studied in electrochemical reduction reactions due to their...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C25B3/26C25B3/03C25B11/032C25B11/091
CPCC25B3/26C25B3/03C25B11/032C25B11/091
Inventor 夏川郑婷婷戴逸舟
Owner YANGTZE DELTA REGION INST OF UNIV OF ELECTRONICS SCI & TECH OF CHINE HUZHOU
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