ZnOHF nanorods for efficient electrocatalytic reduction of carbon dioxide to carbon monoxide
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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。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.
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Key words:
- ZnOHF /
- carbon dioxide reduction /
- carbon monoxide /
- electrocatalysis /
- flow electrolytic cell
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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
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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