富含碳空位多孔碳电催化还原脱氯邻二氯乙烷性能研究

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马航帆,李新勇.富含碳空位多孔碳电催化还原脱氯邻二氯乙烷性能研究[J].,2019,59(6):567-574

富含碳空位多孔碳电催化还原脱氯邻二氯乙烷性能研究

Performance study of carbon vacancy-rich porous carbon for electrocatalytic reduction dechlorination of 1,2-dichloroethane

DOI：10.7511/dllgxb201906003

中文关键词:电催化还原脱氯碳空位原位漫反射傅里叶红外光谱理论计算

英文关键词:eletrocatalytic reduction dechlorination carbon vacancy in-situ diffuse reflection using Fourier transform spectroscopy (DRIFTS)theoretical calculations

基金项目:国家重点研发计划项目(2016YFC0204200)；国家自然科学基金资助项目(21577012重大项目21590813).

作者	单位
马航帆,李新勇

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中文摘要:

寻求经济、高性能的碳基材料对于电催化还原脱氯很有吸引力，然而由于掺杂剂或边缘效应与固有拓扑缺陷之间的复杂相互作用，拓扑缺陷对催化活性的贡献目前研究较少．利用两步活化法成功构建了富含碳空位的疏水分级多孔碳材料(Vc-GC)，考察了其对邻二氯乙烷(DCE)的电催化还原脱氯性能，同时结合原位漫反射傅里叶红外光谱和理论计算分析了碳空位对材料催化活性的增强机制．结果表明，碳空位能有效调节材料的微观结构和电子云分布，增强材料对DCE的化学吸附作用，提高材料的吸附性能，且电子云重排提高了材料的导电性，进而促进电催化活性．其中Vc-GC的乙烯产率是低缺陷石墨碳(GC)和氧化活性炭(oAC)的1.4倍和3.6倍．同时，碳空位的存在能显著提高产物中乙烯的选择性，引入碳空位后，乙烯产率为氯乙烯产率的325.1倍，相比于oAC和GC分别提高了14倍和1.7倍．碳空位修饰显著提升了碳材料电催化活性，拓扑缺陷工程拓宽了进一步提高碳材料环境净化和能源转化性能的途径．

英文摘要:

Seeking economical, high-performance carbon-based materials is intriguing for electrocatalytic reduction dechlorination, however, contribution of topological defects has been explored little owing to intricate interaction between the dopants or edge effects and intrinsic topological defects. A hydrophobic graded porous carbon material rich in carbon vacancies (Vc-GC) is successfully constructed by two-step activation method, and the electrocatalytic reduction dechlorination of 1, 2-dichloroethane (DCE) is investigated systematically. What′s more, in-situ diffuse reflection using Fourier transform spectroscopy (DRIFTS) and theoretical calculations are carried out to analyze the promotion mechanism of carbon vacancies on the catalytic activity of the material. The results show that the carbon vacancy can effectively modulate the microstructure and electron cloud of carbon material, which can enhance the chemical adsorption of the material to DCE and improve the adsorption performance of the material. Besides, the electron cloud rearrangement is beneficial to enhance the conductivity of the material thereby the electrocatalytic activity is promoted, wherein the ethylene yield of Vc-GC is 1.4 times and 3.6 times that of low-defect graphite carbon (GC) and oxidized activated carbon (oAC). At the same time, the presence of carbon vacancies can significantly increase the selectivity of ethylene in the product. After the introduction of carbon vacancies, the yield of ethylene is 325.1 times that of vinyl chloride, which is 14 times and 1.7 times higher than that of oAC and GC, respectively. The carbon vacancy modification significantly improves the electrocatalytic activity of carbon materials, and the topology defect engineering broadens the way to further improve the environmental purification and energy conversion performance of carbon materials.

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