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用于氯乙烯废气高效催化氧化的Ce-Cu-W-O微球的新颖合成
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作者 冯晓珊 郑颖滨 +6 位作者 林代峰 吴恩惠 罗永晋 游钰锋 薛珲 钱庆荣 陈庆华 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第12期1864-1872,共9页
含氯挥发性有机物(CVOC)氯乙烯(VC)出现在工业生产聚氯乙烯(PVC)的尾气中,其具有高毒性和环境稳定性,若直接排放到大气中,会引起环境污染和威胁人类健康,因此有效的去除CVOC至关重要.在众多处理技术,催化氧化法具有反应温度低、能耗少... 含氯挥发性有机物(CVOC)氯乙烯(VC)出现在工业生产聚氯乙烯(PVC)的尾气中,其具有高毒性和环境稳定性,若直接排放到大气中,会引起环境污染和威胁人类健康,因此有效的去除CVOC至关重要.在众多处理技术,催化氧化法具有反应温度低、能耗少、避免二次污染等优点,因而备受关注.用于CVOC催化氧化的催化剂包含贵金属和非贵金属催化剂,后者因为具有较低的成本和较好的抗氯中毒能力而广受研究.CVOC氧化催化剂通常需要具备酸性位和氧化还原位,酸性位用来吸附活化CVOC分子,而氧化还原位对应深度氧化能力.过渡金属氧化物CeO2具有良好的储氧能力和氧化还原性而被作为催化材料应用于CVOC的催化氧化,但深度氧化能力不佳.研究发现,复合Cu氧化物可以提高CeO2的氧化还原性,继而提升催化剂对CVOC的氧化能力,但酸性不足仍然限制了氯乙烯低温完全氧化的能力.为此,可以尝试在Ce-Cu复合氧化物中引入氧化钨来提高催化剂的酸性,但往往削弱了催化剂的氧化还原性,且酸性位大多分布在催化剂体相中,无法充分发挥其对VC分子的吸附活化.基于此,本文利用钨酸铵随水热时间延长而逐渐溶解并扩散W离子的这一特性,通过一步水热法设计合成了表面富集W物种和高分散精细Cu物种的Ce-Cu-W-O微球,其相对于Ce-Cu-O催化剂具有同时更好的酸性和氧化还原性,从而表现出对VC优异的深度氧化能力和热稳定性.通过扫描电子显微镜,X射线能谱和X射线衍射分析,我们解析了Ce-Cu-W-O微球上不同元素组分在水热过程中的生长阶段和物相状态.NH3程序升温脱附分析验证了W物种的添加将提高Ce-Cu氧化物的酸性.H2程序升温还原分析表明,共沉淀方式引入W会降低Ce-Cu氧化物的氧化还原性,而水热一步法制备Ce-Cu-W-O微球的氧化还原性却得到了改善,归因细小晶粒尺寸CuO物种的生成.此外,拉曼光谱和XPS分析表明,HW-CeCuW催化剂具有更多的氧空位,有利于活性氧物种的迁移.因此,Ce-Cu-W-O微球表现出优异的低温氧化活性(250 oC时的反应速率为2.01×10^-7 mol/(gcat·s))和较高的HCl选择性.同时,Ce-Cu-W-O微球经三次循环测试后性能仅略微下降,且在300℃下进行72 h的耐久性实验中保持稳定的VC转化率和矿化率,表明其良好的热稳定性.本合成策略可以为高效的CVOC催化氧化的金属氧化物催化剂的设计和合成提供一些新思路. 展开更多
关键词 氯乙烯催化氧化 Ce-Cu-W-O微球 钨酸铵溶解性 丰富表面WO3 精细CuO纳米颗粒
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N-doped CoAl oxides from hydrotalcites with enhanced oxygen vacancies for excellent low-temperature propane oxidation
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作者 Enhui Wu daifeng lin +7 位作者 Yinye Chen Xiaoshan Feng Kui Niu Yongjin Luo Baoquan Huang Jianbin Qiu Qingrong Qian Qinghua Chen 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2022年第6期79-89,共11页
A series of nitrogen-doped CoAlO(N-CoAlO)were constructed by a hydrothermal route combined with a controllable NH_(3) treatment strategy.The effects of NH_(3) treatment on the physico-chemical properties and oxidation... A series of nitrogen-doped CoAlO(N-CoAlO)were constructed by a hydrothermal route combined with a controllable NH_(3) treatment strategy.The effects of NH_(3) treatment on the physico-chemical properties and oxidation activities of N-Co AlO catalysts were investigated.In comparison to CoAlO,a smallest content decrease in surface Co^(3+)(serving as active sites)while a largest increased amount of surface Co^(2+)(contributing to oxygen species)are obtained over N-Co AlO/4h among the N-CoAlO catalysts.Meanwhile,a maximum N doping is found over N-CoAlO/4h.As a result,N-CoAlO/4h(under NH_(3) treatment at 400℃ for 4 hr)with rich oxygen vacancies shows optimal catalytic activity,with a T90(the temperature required to reach a 90% conversion of propane)at 266℃.The more oxygen vacancies are caused by the co-operative effects of N doping and suitable reduction of Co^(3+) for NCoAlO/4h,leading to an enhanced oxygen mobility,which in turn promotes C_(3)H_(8) total oxidation activity dominated by Langmuir-Hinshelwood mechanism.Moreover,in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTs)analysis shows that N doping facilities the decomposition of intermediate species(propylene and formate)into CO_(2)over the catalyst surface of N-CoAlO/4h more easily.Our reported design in this work will provide a promising way to develop abundant oxygen vacancies of Co-based catalysts derived from hydrotalcites by a simple NH_(3) treatment. 展开更多
关键词 Hydrotalcite derived oxides Propane oxidation N doping Co species Oxygen vacancies
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Insights into the Low-temperature Synthesis of LaCoO3 Derived from Co(CH3COO)2 Via Electrospinning for Catalytic Propane Oxidation
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作者 Yingbin Zheng Xiaoshan Feng +6 位作者 daifeng lin Enhui Wu Yongjin Luo Yufeng You Baoquan Huang Qingrong Qian Qinghua Chen 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2020年第2期144-150,共7页
Summary of main observation and conclusion A series of electrospun LaCoO3 perovskites derived from CoX2 (X =CH3COO-,NO3-) were prepared and investigated for total propane oxidation.It is shown that pure rhombohedral p... Summary of main observation and conclusion A series of electrospun LaCoO3 perovskites derived from CoX2 (X =CH3COO-,NO3-) were prepared and investigated for total propane oxidation.It is shown that pure rhombohedral perovskite LaCoO3 from Co(CH3COO)2 can be obtained at a relatively low temperature,400 ℃,benefitting from the complexation effect of CH3COO-.On the other hand,CH3COO-can accelerate the complete decomposition of polymer.The low-temperature process can protect LaCoO3 nanoparticles from growing up. 展开更多
关键词 LACOO3 oxidation. PEROVSKITE
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