In this manuscript, a series of catalyst SG n-[VVO2-PAMAM-MSA] (SG silica gel, PAMAM polyamidoamine, MSA 5-methyl salicylaldehyde, n=0, 1, 2, 3) was prepared and their structures were fully characterized by Fourier tr...In this manuscript, a series of catalyst SG n-[VVO2-PAMAM-MSA] (SG silica gel, PAMAM polyamidoamine, MSA 5-methyl salicylaldehyde, n=0, 1, 2, 3) was prepared and their structures were fully characterized by Fourier transform-infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS) and inductive coupled plasma emission spectrometer (ICP) etc. XPS revealed that the metal V and SG n-PAMAM-MSA combined more closely after the formation of Schiff base derivatives. Their catalytic activities for oxidation of dibenzothiophene were evaluated using tert-butyl hydroperoxide as oxidant. The results showed that the catalyst SG 2.0-[VVO2-PAMAM-MSA] presented good catalytic activity and recycling time. Meanwhile, the optimal condition for the catalytic oxidation of SG 2.0-[VVO2-PAMAM-MSA] was also investigated, which showed that when the oxidation temperature was 90 °C, time was 60 min, the O/S was 3:1, and the mass content of catalyst was 1%, the rate of desulfurization could reach 85.2%. Moreover, the catalyst can be recycled several times without significant decline in catalytic activity.展开更多
高效电催化析氧催化剂的理性设计与可控合成对发展新型可持续能源转换系统具有重要意义.具有混合价态的四氧化三钴纳米材料具有一定的电催化析氧活性,但性能一般且导电性较差.本文首先制备出超薄二维MXene纳米片,并在此基础上可控构建0D...高效电催化析氧催化剂的理性设计与可控合成对发展新型可持续能源转换系统具有重要意义.具有混合价态的四氧化三钴纳米材料具有一定的电催化析氧活性,但性能一般且导电性较差.本文首先制备出超薄二维MXene纳米片,并在此基础上可控构建0D Co3O4/2D MXene纳米复合材料.二维MXene丰富的表面官能团能很好地调控四氧化三钴纳米颗粒的尺寸.纳米复合催化剂在碱性介质中表现出优异的电催化析氧活性.在电流密度达到10 m A cm-2时,优先的复合催化剂所需的过电位仅为300 m V,远低于纯相MXene和Co3O4纳米颗粒,大幅提升的电催化活性归因于纳米复合材料中两组分间的界面强耦合效应和协同作用.该工作纳米复合材料制备方法简单有效,研究思路可以进一步拓展到其他类似二维MXene基纳米复合材料的设计合成及应用中.展开更多
基金Supported by the National Natural Science Foundation of China （20901063） the Natural Science Foundation of Hubei Province （2011CDB221）
文摘In this manuscript, a series of catalyst SG n-[VVO2-PAMAM-MSA] (SG silica gel, PAMAM polyamidoamine, MSA 5-methyl salicylaldehyde, n=0, 1, 2, 3) was prepared and their structures were fully characterized by Fourier transform-infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), X-ray photoelectron spectroscopy (XPS) and inductive coupled plasma emission spectrometer (ICP) etc. XPS revealed that the metal V and SG n-PAMAM-MSA combined more closely after the formation of Schiff base derivatives. Their catalytic activities for oxidation of dibenzothiophene were evaluated using tert-butyl hydroperoxide as oxidant. The results showed that the catalyst SG 2.0-[VVO2-PAMAM-MSA] presented good catalytic activity and recycling time. Meanwhile, the optimal condition for the catalytic oxidation of SG 2.0-[VVO2-PAMAM-MSA] was also investigated, which showed that when the oxidation temperature was 90 °C, time was 60 min, the O/S was 3:1, and the mass content of catalyst was 1%, the rate of desulfurization could reach 85.2%. Moreover, the catalyst can be recycled several times without significant decline in catalytic activity.
基金financial support from the National Natural Science Foundation of China (21975129, 51902164)Natural Science Foundation of Jiangsu Province (BK20180777, BK20190759)+4 种基金Natural Science Foundation of Jiangsu Higher Education Institutions of China (18KJB430018, 19KJB430003)Scientific Research Foundation for Advanced Talents (CXL2018046)Science Innovation Foundation for Young Scientists (CX2018012)supported by Student’s Platform for Innovation and Entrepreneurship Training Program in Jiangsu Province (201810298029Z)Student’s Platform for Innovation and Entrepreneurship Training Program (2018NFUSPITP602)。
文摘高效电催化析氧催化剂的理性设计与可控合成对发展新型可持续能源转换系统具有重要意义.具有混合价态的四氧化三钴纳米材料具有一定的电催化析氧活性,但性能一般且导电性较差.本文首先制备出超薄二维MXene纳米片,并在此基础上可控构建0D Co3O4/2D MXene纳米复合材料.二维MXene丰富的表面官能团能很好地调控四氧化三钴纳米颗粒的尺寸.纳米复合催化剂在碱性介质中表现出优异的电催化析氧活性.在电流密度达到10 m A cm-2时,优先的复合催化剂所需的过电位仅为300 m V,远低于纯相MXene和Co3O4纳米颗粒,大幅提升的电催化活性归因于纳米复合材料中两组分间的界面强耦合效应和协同作用.该工作纳米复合材料制备方法简单有效,研究思路可以进一步拓展到其他类似二维MXene基纳米复合材料的设计合成及应用中.
