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光热协同催化去除挥发性有机化合物和CO的研究进展 被引量:13
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作者 魏龙福 余长林 +2 位作者 杨凯 樊启哲 纪红兵 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第7期1078-1095,共18页
随着社会和经济的快速发展,环境污染和能源短缺等问题,尤其是空气污染,已经影响了人类的可持续发展.挥发性有机化合物(VOCs),如苯、甲苯、甲醛和丙酮是主要的空气污染物,它们主要来源于油漆、有机化学品、石油化工产品、药物和工业生产... 随着社会和经济的快速发展,环境污染和能源短缺等问题,尤其是空气污染,已经影响了人类的可持续发展.挥发性有机化合物(VOCs),如苯、甲苯、甲醛和丙酮是主要的空气污染物,它们主要来源于油漆、有机化学品、石油化工产品、药物和工业生产过程.大多VOCs具有特殊的气味,而且具有一定的毒性、致畸性和致癌作用,尤其是苯、甲苯和甲醛等,会对人类的身体健康产生巨大的负面作用.因此,研发新型高效VOCs处理技术迫在眉睫.除VOCs外,CO也是非常常见的空气污染物,在室温条件下,它无色无味,没有刺激性且易燃易爆.CO主要来源于煤和石油等含碳材料的不完全燃烧.在日常生活中很容易被排放到大气中.在室温下,CO分子是非常稳定的,很难与其它气体分子发生化学反应.因此,CO的活化和转化是一项具有挑战性的工作.催化氧化技术是在催化剂存在的条件下进行的氧化反应,可以将VOCs直接氧化成为无毒无害的CO_(2)和H_(2)O,也可将CO氧化成CO_(2).光催化技术是一种新型的环境友好型技术,可在常温常压下进行,反应条件温和、能耗小、操作简单,成本低,氧化产物为无毒无害物质,以及不存在二次污染等优点.但光催化反应效率较低,主要通过入射光的能量驱动化学反应.热催化则通过升温的方法来驱动化学反应.目前,热催化剂主要为贵金属型催化剂,其具有催化活性较高,选择性较好且不存在二次污染等优点.但高能耗影响产物的稳定性和选择性,此外,贵金属的使用导致成本增加.光热协同催化可以整合光催化和热催化的优势,并弥补各自的不足,形成一种协同效应,是一种新颖的催化反应.目前,关于光催化或热催化高效去除VOCs和CO的综述较多,但很少有关于光热协同催化高效去除VOCs和CO的综述.本综述重点讨论光热协同催化高效去除VOCs和CO的最新研究进展.首先,介绍了光热协同催化的概况,如设计光热催化材料和催化反应器等.其次,重点介绍苯、甲苯、乙醇、甲醛、乙醛和丙酮等几种典型VOCs的光热协同催化的最新研究进展.再次,总结了光热协同催化CO加氢和氧化的最新研究进展.此外,还探讨了光热协同催化去除VOCs和CO的可能反应机理.最后,对光热协同催化的应用前景进行了展望. 展开更多
关键词 挥发性有机化合物 CO 光催化 热催化 光热协同催化
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溶剂热合成可调控氧空位的Bi_(2)MoO_(6)纳米晶及其光催化氧化制喹啉和抗生素降解 被引量:2
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作者 刘珍 田坚 +2 位作者 余长林 樊启哲 刘兴强 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第2期472-484,共13页
近年来,半导体光催化在环境净化和有机合成领域的研究引起了广泛的重视.其中,在有机合成领域中,光催化技术已经应用在醇类、环己烷以及芳香族化合物的选择性氧化研究.而另一类具有特殊结构的有机物——N-杂环芳烃,在药物化学和材料科学... 近年来,半导体光催化在环境净化和有机合成领域的研究引起了广泛的重视.其中,在有机合成领域中,光催化技术已经应用在醇类、环己烷以及芳香族化合物的选择性氧化研究.而另一类具有特殊结构的有机物——N-杂环芳烃,在药物化学和材料科学中具有重要意义.而传统用于合成N-杂化芳烃的脱氢催化氧化反应通常需要高温高压的苛刻环境,传统方法通常还需要使用贵金属催化剂,这也增加了N-杂化芳烃的合成成本;另外,如果合成是均相催化过程,则催化剂难以实现回收利用.因此,开发室温常压条件下的非贵金属多相光催化技术具有巨大的应用前景.本文以能够被可见光驱动的钼酸铋半导体为催化剂,利用氧缺陷策略来提升钼酸铋的光催化氧化性能.不同于传统氧缺陷制备方法(氢气还原热处理、离子掺杂等),本文采用一种低成本的乙二醛辅助溶剂热的方法合成具有可调控的含氧空位Bi_(2)MoO_(6)催化剂(OVBMO).通过X射线粉末衍射(XRD)、扫描电镜、透射电镜、紫外可见漫反射吸收光谱、氮气物理吸附脱附、X射线光电子能谱(XPS)、电子自旋共振光谱、光致发光光谱及电化学测试等技术对制备的OVBMO材料进行了物理化学性质及能带研究.XPS,XRD,Raman和FT-IR结果表明,氧空位存在于[Bi_(2)O_(2)]^(2+)和MoO_(6)八面体的层间.紫外可见漫反射结果表明,随着氧空位的引入,Bi_(2)MoO_(6)的光吸收范围扩大,带隙变窄.结合莫特肖特基和VBXPS分析获得OVBMO的能带位置,发现氧空位的存在不仅会导致禁带中出现缺陷带能级,还会导致价带顶位置上移,促进光生空穴的迁移.PL和电化学结果表明,氧空位的存在使得载流子浓度、载流子的分离能力与界面电荷迁移能力都有较大提升,这是因为氧空位引入的缺陷能级可以浅势捕获电子,抑制光催化剂中的电子与空穴的复合,改变化学反应的速率.同时,氧空位有助于捕获分子氧,分子氧与捕获的光生电子发生反应,产生更多的超氧自由基(·O_(2))和空穴(h^(+)),从而极大地提升光催化剂的氧化性能.因此,OVBMO在1,2,3,4-四氢喹啉脱氢氧化产生喹啉及系列抗生素(环丙沙星、四环素、盐酸土霉素)的降解反应中,表现出较好的光催化氧化性能.结合多种表征分析,本文还进一步阐明了OVBMO催化剂将1,2,3,4-四氢喹啉脱氢氧化为喹啉的自由基参与的多相催化反应机理. 展开更多
关键词 Bi_(2)MoO_(6)纳米晶体 氧空位 光催化氧化性能 喹啉生产 抗生素降解
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Novel Ni/CeO_2-Al_2O_3 composite catalysts synthesized by one-step citric acid complex and their performance in catalytic partial oxidation of methane 被引量:1
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作者 Changlin Yu Jiubiao Hu +1 位作者 Wanqin Zhou qizhe fan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2014年第2期235-243,共9页
A series of novel Ni/CeO2-Al2O3composite catalysts were synthesized by one-step citric acid complex method. The as-synthesized catalysts were characterized by N2physical adsorption/desorption, X-ray diffraction(XRD), ... A series of novel Ni/CeO2-Al2O3composite catalysts were synthesized by one-step citric acid complex method. The as-synthesized catalysts were characterized by N2physical adsorption/desorption, X-ray diffraction(XRD), Fourier transform infrared(FT-IR) spectroscopy, hydrogen temperature-programmed reduction(H2-TPR), X-ray photoelectron spectroscopy(XPS) and thermogravimetry analysis(TGA). The effects of nickel content, calcination and reaction temperatures, gas hourly space velocity(GHSV) and inert gas dilution of N2on their performance of catalytic partial oxidation of methane(CPOM) were investigated. Catalytic activity test results show that the highest methane conversion(>85%), the best selectivities to carbon monoxide(>87%) and to hydrogen(>95%), the excellent stability and perfect H2/CO ratio(2.0) can be obtained over Ni/CeO2-Al2O3with 8 wt% Ni content calcined at 700 ℃ under the reaction condition of 750 ℃, CH4/O2ratio of 2 : 1 and gas hourly space velocity of 12000 mL h-1 g-1. Characterization results show that the good catalytic performance of this composite catalyst can be contributed to its large specific surface area(~108 m2 g-1), small crystallite size, easy reducibility and low coking rate. 展开更多
关键词 复合催化剂 氧化性能 络合物 柠檬酸 一步法 合成 甲烷 X射线光电子能谱
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La/Ce-codoped Bi_2O_3 composite photocatalysts with high photocatalytic performance in removal of high concentration dye 被引量:7
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作者 Shuangshuang Xue Hongbo He +5 位作者 qizhe fan Changlin Yu Kai Yang Weiya Huang Yang Zhou Yu Xie 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2017年第10期70-77,共8页
A series of La/Ce-codoped Bi_2O_3 composite photocatalysts were fabricated via hydrothermal–calcination process. The as-prepared products were intensively characterized by some physicochemical characterizations like ... A series of La/Ce-codoped Bi_2O_3 composite photocatalysts were fabricated via hydrothermal–calcination process. The as-prepared products were intensively characterized by some physicochemical characterizations like N_2 physical adsorption, X-ray powder diffraction(XRD), scanning electron microscope(SEM), transmission electron microscope(TEM), UV–Vis diffuse reflectance(UV–Vis DRS), Fourier transform infrared spectroscopy(FT-IR),photoelectrochemical measurements, and photoluminescence(PL) spectroscopy. The characterization results indicated that La and Ce doping induced obvious crystal phase transformation in Bi_2O_3, from monoclinic to tetragonal phase. La and Ce codoping also gave rise to the obvious synergetic effects, e.g., the lattice contraction of Bi_2O_3, the decrease of crystal size and the increase of surface area. The photocatalytic performance of the prepared catalysts was evaluated by removal of dye acid orange II with high concentration under visible light irradiation. Results showed that La/Ce-codoped Bi_2O_3 displayed much higher photocatalytic performance than that of bare Bi_2O_3, single La or Ce doped Bi_2O_3 samples. The superior photocatalytic activity was mainly attributed to the improved texture and surface properties and the synergistic effects of La and Ce codoping on suppressing the recombination of photo-generated electrons(e^-) and holes(h^+). 展开更多
关键词 复合光催化剂 BI2O3 光催化性能 酸性染料 铈掺杂 浓度 扫描电子显微镜 去除率
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High value-added fluorescence upconversion agents-assisted nanosemiconductors for efficient wide spectral response photocatalysis:Exerting energy transfer effect and applications 被引量:1
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作者 Kailian Zhang Man Zhou +7 位作者 Changlin Yu Xiaoxiao Li Kai Yang Shi Yang Wenxin Dai Weiya Huang qizhe fan Lihua Zhu 《Journal of Rare Earths》 SCIE EI CAS CSCD 2021年第3期243-260,I0001,共19页
The design of the photocatalytic materials has made a great of remarkable progress in the area of the enhancement photocatalytic activity,but there are still lots of problems such as wide band gap,low utilization of s... The design of the photocatalytic materials has made a great of remarkable progress in the area of the enhancement photocatalytic activity,but there are still lots of problems such as wide band gap,low utilization of sunlight,low quantum efficiency and poor stability,which further limit the extensive practical applications.Thus,it is a hot research topic and key scientific problem to be solved that how to design and prepare the catalysts,which can respond to visible and near-infrared light in sunlight.Inspired by efficient nonlinear optical upconversion materials,upconversion-based nanocomposites can indirectly broaden the absorption ranges of semiconductors by co nverting the captured long-band visible and near-infrared incident light into high-energy short-band visible or ultraviolet light,which can be adopted as the promising candidate in wide-spectral-light-activating photocatalytic materials coupling with conventional semiconductors.According to our recent works and literature reports,recent review summarizes the research progress of photocatalytic materials with upconversion effect on photolysis of water for hydrogen production,degradation of organic and inorganic pollutants,reduction of CO_(2) and photodynamic therapy.The prepared nanocomposites can suppress the recombination of electrons and holes,and greatly improve the photocatalytic efficiency by the synergistic effect.It maybe stimulates a great interest in rational design and preparation of efficient full-spectrum photocatalytic systems and their wide application in solar energy conversion. 展开更多
关键词 Fluorescence upconversion Hydrogen production PHOTOCATALYSIS Treatment of pollutants Photodynamic therapy Rare earths
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