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硼基材料催化低碳烷烃氧化脱氢制烯烃研究进展 被引量:4
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作者 盛健 陆文多 +4 位作者 闫冰 邱彬 周禹希 王东琪 陆安慧 《化工进展》 EI CAS CSCD 北大核心 2021年第4期1883-1892,共10页
以氮化硼为代表的硼基材料在低碳烷烃氧化脱氢反应中显示出高的催化活性和优异的烯烃选择性,已在国际上形成新的研究热点。本文主要综述了近年来硼基材料催化低碳烷烃氧化脱氢的研究进展,阐述了不同硼基催化剂(h-BN、SiB_(6)、BC_(4)、... 以氮化硼为代表的硼基材料在低碳烷烃氧化脱氢反应中显示出高的催化活性和优异的烯烃选择性,已在国际上形成新的研究热点。本文主要综述了近年来硼基材料催化低碳烷烃氧化脱氢的研究进展,阐述了不同硼基催化剂(h-BN、SiB_(6)、BC_(4)、硼单质等)对氧化脱氢烯烃选择性的影响,结合多种谱学(IR、XPS、NMR、SVUVPIMS等)、动力学(分压、同位素效应、同位素标记等)证据和理论计算,探讨了硼基催化剂表面三配位的硼氧物种(B—OH/B—O)是引发烷烃氧化脱氢生成烯烃的活性位,主要遵循表面和气相自由基反应机理。总结了硼基催化材料氧化脱氢中存在的机遇和挑战,提升烯烃选择性是材料设计合成的主要方向,并提出后续硼基催化材料理性设计和实际应用的一些参考建议。 展开更多
关键词 硼基材料 催化 烷烃 氧化脱氢 烯烃
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纤维状BPO_(4)/SiO_(2)催化剂的制备及其丙烷氧化脱氢性能 被引量:1
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作者 丁鼎 陆文多 +1 位作者 侯璐 陆安慧 《化工学报》 EI CAS CSCD 北大核心 2021年第11期5590-5597,共8页
通过静电纺丝法制备了一种高温焙烧后具有纤维状结构的磷酸硼/二氧化硅(BPO4/SiO2)催化剂,并考察了BPO4负载量和焙烧温度对该催化剂的结构和催化丙烷氧化脱氢性能的影响。研究发现焙烧过程使纤维直径减小。随着BPO4负载量的增加,丙烷氧... 通过静电纺丝法制备了一种高温焙烧后具有纤维状结构的磷酸硼/二氧化硅(BPO4/SiO2)催化剂,并考察了BPO4负载量和焙烧温度对该催化剂的结构和催化丙烷氧化脱氢性能的影响。研究发现焙烧过程使纤维直径减小。随着BPO4负载量的增加,丙烷氧化脱氢活性增高。当BPO4负载量为7%(质量分数),焙烧温度为600℃时,BPO4/SiO2催化剂具有最佳的催化性能;在反应温度为480℃下,丙烷转化率和丙烯产率分别达到17.0%和13.0%,且催化剂稳定性良好。当焙烧温度较低时(550℃),催化剂中的有机物分子未被除尽,导致烯烃的选择性偏低;当焙烧温度较高时(700℃),SiO2结构收缩紧密,抑制了活性相的暴露。由于纤维结构可暴露更多活性位点,该催化剂较相同条件下粉末状BPO4催化剂有着更高的催化活性。 展开更多
关键词 烷烃 氧化脱氢 纤维 纳米结构 静电纺丝 催化剂 磷酸硼
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Rod-shaped porous alumina-supported Cr_2O_3 catalyst with low acidity for propane dehydrogenation 被引量:17
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作者 Xin-Qian Gao Wen-Duo Lu +2 位作者 Shou-Zhao Hu Wen-Cui Li An-Hui Lu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第2期184-191,共8页
Direct catalytic propane dehydrogenation(PDH)to obtain propylene is a more economical and environmentally friendly route for propylene production.In particular,alumina-supported Cr2O3 catalysts can have better potenti... Direct catalytic propane dehydrogenation(PDH)to obtain propylene is a more economical and environmentally friendly route for propylene production.In particular,alumina-supported Cr2O3 catalysts can have better potential applications if the acidic properties could be tuned.Herein,a series of rod-shaped porous alumina were prepared through a hydrothermal route,followed by calcination.It was found that the acidity of the synthesized alumina was generally lower than that of the commercial alumina and could be adjusted well by varying the calcination temperature.Such alumina materials were used as supports for active Cr2O3,and the obtained catalysts could enhance the resistance to coke formation associated with similar activity in PDH reaction compared to the commercial alumina.The amount of coke deposited on a self-made catalyst(Cr-Al-800)was 3.6%,which was much lower than that deposited on the reference catalyst(15.7%).The lower acidity of the catalyst inhibited the side reactions and coke formation during the PDH process,which was beneficial for its high activity and superior anti-coking properties. 展开更多
关键词 ALUMINA ACIDITY CALCINATION CHROMIUM ANTI-COKING
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Ordered macroporous boron phosphate crystals as metal-free catalysts for the oxidative dehydrogenation of propane 被引量:8
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作者 Wen-Duo Lu Xin-Qian Gao +4 位作者 Quan-Gao Wang Wen-Cui Li Zhen-Chao Zhao Dong-Qi Wang An-Hui Lu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2020年第12期1837-1845,共9页
Ordered macroporous materials with rapid mass transport and enhanced active site accessibility are essential for achieving improved catalytic activity.In this study,boron phosphate crystals with a three-dimensionally ... Ordered macroporous materials with rapid mass transport and enhanced active site accessibility are essential for achieving improved catalytic activity.In this study,boron phosphate crystals with a three-dimensionally interconnected ordered macroporous structure and a robust framework were fabricated and used as stable and selective catalysts in the oxidative dehydrogenation(ODH)of propane.Due to the improved mass diffusion and higher number of exposed active sites in the ordered macroporous structure,the catalyst exhibited a remarkable olefin productivity of^16 golefin gcat^-1 h^-1,which is up to 2–100 times higher than that of ODH catalysts reported to date.The selectivity for olefins was 91.5%(propene:82.5%,ethene:9.0%)at 515℃,with a propane conversion of 14.3%.At the same time,the selectivity for the unwanted deep-oxidized CO2 product remained less than 1.0%.The tri-coordinated surface boron species were identified as the active catalytic sites for the ODH of propane.This study provides a route for preparing a new type of metal-free catalyst with stable structure against oxidation and remarkable catalytic activity,which may represent a potential candidate to promote the industrialization of the ODH process. 展开更多
关键词 Ordered macroporous material Metal-free catalyst Boron phosphate Oxidative dehydrogenation PROPANE
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Electrospinning synthesis of porous boron-doped silica nanofibers for oxidative dehydrogenation of light alkanes 被引量:4
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作者 Bing Yan Wen-Duo Lu +3 位作者 Jian Sheng Wen-Cui Li Ding Ding An-Hui Lu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2021年第10期1782-1789,共8页
The discovery of the high activity and selectivity of boron-based catalysts for oxidative dehydrogenation(ODH)of alkanes to olefins has attracted significant attention in the exploration of a new method for the synthe... The discovery of the high activity and selectivity of boron-based catalysts for oxidative dehydrogenation(ODH)of alkanes to olefins has attracted significant attention in the exploration of a new method for the synthesis of highly active and selective catalysts.Herein,we describe the synthesis of porous boron-doped silica nanofibers(PBSNs)100-150 nm in diameter by electrospinning and the study of their catalytic performance.The electrospinning synthesis of the catalyst ensures the uniform dispersion and stability of the boron species on the open silica fiber framework.The one-dimensional nanofibers with open pore structures not only prevented diffusion limitation but also guaranteed high catalytic activity at high weight hourly space velocity(WHSV)in the ODH of alkanes.Compared to other supported boron oxide catalysts,PBSN catalysts showed higher olefin selectivity and stability.The presence of Si-OH groups in silica-supported boron catalysts may cause low propylene selectivity during the ODH of propane.When the ODH conversion of ethane reached 44.3%,the selectivity and productivity of ethylene were 84%and 44.2%g_(cat)^(-1)s^(-1),respectively.In the case of propane ODH,the conversion,selectivity of olefins,and productivity of propylene are 19.2%,90%,and 76.6 jimol g_(cat)^(-1)s^(-1),respectively.No significant variations in the conversion and product selectivity occurred during 20 h of operation at a high WHSV of 84.6 h^(-1).Transient analysis and kinetic experiments indicated that the activation of O2 was influenced by alkanes during the ODH reaction. 展开更多
关键词 ELECTROSPINNING NANOFIBERS Boron-based catalyst Oxidative dehydrogenation Light alkanes
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