上海大学学报(自然科学版) ›› 2023, Vol. 29 ›› Issue (5): 960-972.doi: 10.12066/j.issn.1007-2861.2505

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富含介孔结构的氮化碳/碳纳米管复合催化剂高效电催化还原 CO2 为 CO 

刘丙泽, 钮东方   

  1. 华东理工大学 化工学院, 上海 200237
  • 收稿日期:2023-03-09 出版日期:2023-10-28 发布日期:2023-11-03
  • 通讯作者: 钮东方 (1982—), 副教授, 博士, 研究方向为电催化与电合成等. E-mail:dfniu@ecust.edu.cn
  • 基金资助:
    国家自然科学面上基金资助项目 (21972042) 

Highly efficient electrocatalytic reduction of CO2 to CO by nitrogen-doped carbon/carbon nanotube composite catalysts with abundant mesoporous structures

LIU Bingze, NIU Dongfang   

  1. School of Chemical Engineering, East China University of Science and Technology, Shanghai 200237, China
  • Received:2023-03-09 Online:2023-10-28 Published:2023-11-03

摘要:

氮掺杂材料中的吡啶氮被认为是电还原 CO2 为 CO 的最活跃的氮催化位点. 以双氰胺 (dicyandiamide, DCDA) 为氮源, 氧化碳纳米管 (carbon oxide nanotubes, CNTs-O) 为分散剂, 通过静电吸附-煅烧法制备了富含吡啶氮的氮化碳/碳纳米管 (CNx/CNTs) 介孔复合催化剂. 通过改变 DCDA 与 CNTs-O 的质量比, 合成了具有不同石墨化氮化碳 (g-C3N4) 含量的复合催化剂. 通过一系列表征及电化学测试得出, 当 DCDA/CNTs-O 质量比为 0.5 时,得到的 CN0.5/CNTs 具有最优的还原 CO2 为 CO 的电催化性能. 在 −1.0 V vs. RHE 下CN0.5/CNTs 的 CO 法拉第效率 (Faradaic efficiency, FE) 高达 94.1%, 生成 CO 的电流密度 为 −13.27 mA/cm2 , 通过 24 h 长时间电解后依然保持着较高的法拉第效率 (FECO > 85%).

关键词: 电还原 CO2, CO, 介孔, 石墨化氮化碳, 碳纳米管 

Abstract: Pyridine nitrogen in nitrogen-doped materials is considered to be the most active nitrogen catalytic site for electroreduction of CO2 to CO. Dicyandiamide (DCDA) was used as nitrogen source and carbon oxide nanotubes (CNTs-O) as dispersant to prepare nitrogen-doped carbon/carbon nanotube mesoporous composite catalyst with rich pyridinic nitrogen via electrophoretic deposition-calcination method. By changing the mass ratio of DCDA and CNTs-O, the composite catalysts with different contents of g-C3N4 were synthesized. Based on a series of characterization and electrochemical tests, it was determined that CN0.5/CNTs catalyst prepared at DCDA/CNTs-O mass ratio of 0.5 exhibited the best electrocatalytic performance for CO2 reduction to CO. The Faradaic efficiency (FE) of CO on CN0.5/CNTs at −1.0 V vs. RHE was as high as 94.1%, and the current density of CO generation was −13.27 mA/cm2 . The FE of CO was still maintained at a high level (>85%) after 24-h long-term electrolysis.

Key words: electroreduction of CO2 (CO2ER), CO, mesoporous, g-C3N4, carbon nanotubes (CNTs)

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