ZnOHF纳米棒用于电催化二氧化碳还原制一氧化碳

王栋; 钟达忠; 郝根彦; 李晋平; 赵强

doi:10.1016/S1872-5813(21)60082-8

ZnOHF纳米棒用于电催化二氧化碳还原制一氧化碳

doi: 10.1016/S1872-5813(21)60082-8

王栋^{1, 2,},
钟达忠^{1, 2},
郝根彦^{1, 2},
李晋平^{1, 2},
赵强^{1, 2, ,}

1.
太原理工大学化学化工学院，山西太原 030024
2.
气体能源高效清洁利用山西省重点实验室，山西太原 030024

基金项目: 国家自然科学基金（21878202，21975175），山西省回国留学人员科研资助（2017-041），山西省自然科学基金（201801D121052）资助

详细信息

作者简介:
王栋：wangdong0512@link.tyut.edu.cn

通讯作者:
E-mail: zhaoqiang@tyut.edu.cn

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- 被引次数: 0
出版历程
- 收稿日期: 2021-03-09
- 修回日期: 2021-04-01
- 网络出版日期: 2021-04-22
- 刊出日期: 2021-09-30

ZnOHF nanorods for efficient electrocatalytic reduction of carbon dioxide to carbon monoxide

WANG Dong^{1, 2
,},
ZHONG Da-zhong^{1, 2},
HAO Gen-yan^{1, 2},
LI Jin-ping^{1, 2},
ZHAO Qiang^{1, 2
, ,}

1.
College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan 030024
2.
Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization，Taiyuan 030024, China

Funds: The project was supported by the National Natural Science Foundation of China (21878202, 21975175), the Research Project Supported by Shanxi Scholarship Council of China (2017-041) and the Natural Science Foundation of Shanxi Province (201801D121052)

摘要

摘要: 通过电催化的方式将二氧化碳资源化利用是缓解或解决目前人类面临的生态危机的理想途径之一。开发廉价高效的催化剂是推动电催化二氧化碳还原走向工业化的关键。一氧化碳是重要的工业原料，利用CO₂还原制备CO具有重要的研究意义，但能够将CO₂转化为CO的高活性贵金属催化剂难以大规模应用，地球储量丰富的Zn基催化剂是具有潜力的替代者。然而，Zn基催化剂还原活性仍然难以满足现实需求且种类不够丰富。作者将ZnOHF材料引入到电催化CO₂还原中，通过简单水热合成法制备了不同尺寸的ZnOHF纳米棒并利用流动型电解池测试其性能。纳米棒较大的比表面积以及材料表面F原子的存在使其具有良好的催化活性，流动型电解池的使用加速了反应传质过程，在−1.28 V (vs. RHE)电势下，R2-ZnOHF纳米棒的CO法拉第效率最高为76.4 %，CO分电流密度为57.53 mA/cm²。
- ZnOHF /
- 二氧化碳还原 /
- 一氧化碳 /
- 电催化 /
- 流动型电解池
Abstract: The utilization of carbon dioxide as a resource through electrocatalysis is one of the ideal ways to alleviate or solve the current ecological crisis mankind facing. The development of inexpensive and efficient catalysts is the key to promoting the industrialization of electrocatalytic carbon dioxide reduction. CO is an important industrial raw material, as a result, CO₂ reduction to CO has important research significance. However, high-active noble metal catalysts that can convert CO₂ to CO are difficult to apply in large scale. Zn-based catalysts are potential substitutes. However, the reduction activity of Zn-based catalysts still can not meet the actual needs. In this paper, ZnOHF material is employed in the electrocatalytic CO₂ reduction for the first time. ZnOHF nanorods of different sizes are prepared through a simple hydrothermal synthesis method and tested in a Flow-Cell. The large specific surface area of the nanorods and the existence of F atoms on the surface of the material lead to good catalytic activity. The Flow-Cell accelerates the reaction mass transfer process. At –1.28 V (vs. RHE), the R2-ZnOHF nanorods have the highest CO Faraday efficiency of 76.4% with the CO current density of 57.53 mA/cm².
- ZnOHF /
- carbon dioxide reduction /
- carbon monoxide /
- electrocatalysis /
- flow electrolytic cell

HTML全文

FIG. 922. FIG. 922.

FIG. 922. FIG. 922.

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图 1 （a）：样品的制备流程图；（b）：Zn₄CO₃(OH)₆、R1-ZnOHF、R2-ZnOHF及R3-ZnOHF的XRD衍射谱图

Figure 1 (a): Sample preparation flow chart; (b): XRD patterns of Zn₄CO₃(OH)₆, R1-ZnOHF, R2-ZnOHF and R3-ZnOHF

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图 2 （a）Zn₄CO₃(OH)₆、（b）R1-ZnOHF、（c）R2-ZnOHF及（d）R3-ZnOHF的扫描电镜照片

Figure 2 SEM of (a) Zn₄CO₃(OH)₆, (b) R1-ZnOHF, (c) R2-ZnOHF and (d) R3-ZnOHF

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图 3 Zn₄CO₃(OH)₆、R1-ZnOHF、R2-ZnOHF及R3-ZnOHF的（a）红外谱图和（b）N₂吸附-脱附曲线

Figure 3 (a) FT-IR spectra and (b) N₂ adsorption/desorption isotherms of Zn₄CO₃(OH)₆, R1-ZnOHF, R2-ZnOHF and R3-ZnOHF

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图 4 （a）：R1-ZnOHF、（b）：R2-ZnOHF、（c）：R3-ZnOHF的XPS全谱图（表格为各元素含量及结合能位置）；（d）：R1-ZnOHF、R2-ZnOHF和R3-ZnOHF的表面F原子含量柱状对比

Figure 4 XPS survey spectra of (a): R1-ZnOHF; (b): R2-ZnOHF; (c): R3-ZnOHF (the table shows the content and binding energy position of each element); (d): surface F atom content for R1-ZnOHF, R2-ZnOHF and R3-ZnOHF

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图 5 R2-ZnOHF的（a）透射电镜照片，（b）高倍透射照片，（c）EDS元素分布

Figure 5 (a) Transmission electron microscope image, (b) High resolution transmission image, (c) EDS mapping of R2-ZnOHF

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图 6 （a）R1-ZnOHF、（b）R2-ZnOHF及（c）R3-ZnOHF的CO和H₂法拉第效率；（d）R1-ZnOHF、R2-ZnOHF及R3-ZnOHF不同电位下CO法拉第效率柱状对比

Figure 6 CO and H₂ Faraday efficiency of (a) R1-ZnOHF, (b) R2-ZnOHF and (c) R3-ZnOHF; (d) CO Faraday efficiency comparison chart of R1-ZnOHF, R2-ZnOHF and R3-ZnOHF at different potentials

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图 7 R1-ZnOHF、R2-ZnOHF及R3-ZnOHF的（a）总电流密度，（b）CO分电流密度，（c）H₂分电流密度，（d）EIS谱图

Figure 7 (a) Total current density, (b) CO partial current density, (c) H₂ partial current density, (d) EIS spectra of R1-ZnOHF, R2-ZnOHF and R3-ZnOHF

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图 8 Zn₄CO₃(OH)₆和R2-ZnOHF的（a）CO法拉第效率对比，（b）H₂分电流密度对比；H型电解池和流动型电解池中R2-ZnOHF的（c）CO法拉第效率，（d）总电流密度

Figure 8 (a) CO Faraday efficiency comparison and (b) H₂ partial current density comparison of Zn₄CO₃(OH)₆ and R2-ZnOHF; (c) CO Faraday efficiency and (d) Total current density in H-type cell and Flow cell of R2-ZnOHF

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图 9 （a）反应后R2-ZnOHF的XRD谱图；（b）反应后R2-ZnOHF的扫描电镜照片；（c）稳定性测试，电解液为0.1 mol/L KHCO₃

Figure 9 (a) XRD pattern and (b) Scanning electron micrograph of R2-ZnOHF after reaction; (c) Stability Test of R2-ZnOHF in H-type cell, the electrolyte is 0.1 mol/L KHCO₃

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