络合物法制备镍-氮共掺杂炭基二氧化碳电催化剂

doi:10.19964/j.issn.1006-4990.2020-0389

Abstract

Abstract:

Transition metal-nitrogen co-doped carbon-based catalysts have attracted widely attention in electrocatalytic CO₂ reduction reaction（CO₂RR）.To solve the problems of catalytic activity and selectivity of catalysts,two kinds of Ni-N co-do-ped porous carbon-based catalysts were prepared by using triethylenediamine,a small molecule complex,formed by the coor-dination reaction between ethylenediamine and nickel nitrate and hydrophilic GO and hydrophobic carbon black were select-ed as the support,respectively.The existing forms of nickel species in different processing stages were discussed by X-ray diffraction and transmission electron microscopy.The CO₂RR performance showed that the CO current density had been enhanced when the catalyst with different metal loadings on the same carbon support was pickled to remove nickel nanoparticles,which indicated that the nickel species in high dispersion were beneficial to the electrocatalytic reduction of CO₂.At the potential of -0.8 V(vs.RHE),the catalysts with different carbon supports reached a CO Faradic efficiency of 90%.Compared with hydrophilic carbon materials as supports,hydrophobic carbon materials as supports had higher carbon monoxide partial current density,which indicated that hydrophobic carbon supports were conducive to the loading and dispersion of transition metal complexes in the framework of the support,and then inhibited the loss of active substances in the subsequent treatment process,so as to obtain high activity Ni-N co-doped carbon based electrocatalysts.

Key words: CO₂ electroreduction, carbon-based electrocatalysts, Ni-N co-doped carbon materials, complex, hydrophobicity

CLC Number:

O643.36

Chang Ruopeng,Hu Xu,He Lei,Hao Guangping. Preparation of nickel-nitrogen co-doped carbon-based carbon dioxide electrocatalyst through complex-assisted method[J]. Inorganic Chemicals Industry, 2021, 53(9): 97-103.

Figures/Tables 8

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References 19

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过渡金属盐	配比	过渡金属盐-哌嗪配体络合物		过渡金属盐-乙二胺配体络合物
过渡金属盐	配比	状态	实物图	状态	实物图
Cu（NO₃）₂·3H₂O	1:3	[Cu（piperazine）₃]（NO₃）₂青蓝色沉淀		[Cu（en）₃]（NO₃）₂黑紫色沉淀
Fe（NO₃）₃·9H₂O	1:3	[Fe（piperazine）₃]（NO₃）₂棕色沉淀		[Fe（en）₃]（NO₃）₂棕色沉淀
Co（NO₃）₂·6H₂O	1:3	[Co（piperazine）₃]（NO₃）₂黑色沉淀		[Co（en）₃]（NO₃）₂黑色沉淀
Mn（CH₃COO）₂·4H₂O	1:3	[Mn（piperazine）₃]（ac）₂棕黄色沉淀		[Mn（en）₃]（ac）₂棕黄色沉淀
Ni（NO₃）₂·6H₂O	1:1	[Ni（piperazine）_x]（NO₃）₂,x=1、3,翠绿色沉淀		[Ni（en）_x]（NO₃）₂,x=1、3,紫色均匀溶液
Ni（NO₃）₂·6H₂O	1:3
Ni（NO₃）₂·6H₂O	1:5
Ni（NO₃）₂·6H₂O	1:7

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Preparation of nickel-nitrogen co-doped carbon-based carbon dioxide electrocatalyst through complex-assisted method

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