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化石燃料的使用,导致大量CO2温室气体排放,由此引起了一系列环境和气候问题。主要温室气体CO2和CH4的处理和利用已迫在眉睫。CH4-CO2干重整(DRM)将CO2和CH4转化为工业原料气合成气,可以实现2种温室气体的利用。贵金属催化剂对DRM反应表现出优异的催化活性和抗积碳性能,但由于资源有限、价格高,限制了其应用。非贵金属Ni基催化剂的催化活性不仅可以与贵金属相媲美,且来源丰富、价格低,是最有可能被产业化的催化剂之一。但Ni基催化剂存在易烧结和积碳的问题。研究者对Ni基催化剂进行了大量改性工作以提高其催化活性、抗烧结能力和抗积碳能力。为更全面深入认识DRM反应及其Ni基催化剂,首先综述了CH4-CO2重整反应的热力学、反应机理和动力学。热力学研究表明,高温低压有利于DRM反应进行;但至今没有适合于所有催化剂统一的反应机理,不同催化剂的反应机理和速控步骤不同。进一步对影响Ni基催化剂性能的... 相似文献
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以等离子体还原制备的Ni/Al2O3和Ni/MgO-Al2O3为催化剂,用氙灯模拟太阳光聚光系统进行CH4-CO2重整反应,并考察其催化性能及能量转化效率,实验结果表明,以等离子体还原并加入MgO助剂制备的Ni/MgO-Al2O3催化剂具有较好的低温催化活性,在温度为740℃时,CH4和CO2的最高转化率分别为83.6 25%.1和%,能量转化效率为41.5%,大大高于光伏法制氢效率的10.85%;XRD表征表明,等离子体还原使催化剂活性组分Ni具有良好的分散性和更小的纳米团簇结构,有利于甲烷的转化;MgO助剂的加入增强了催化剂表面的碱性,促进了CO2的吸附和解离。 相似文献
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太阳能驱动的CO2与CH4转化为合成气是一种非常有前景的生产可再生燃料的技术,然而太阳能驱动的CH4重整催化剂存在转化效率低、光生电子与空穴复合速率快及催化剂稳定性差等问题。本文简述了光催化CO2与CH4重整的可能机理,包括CO2和CH4的吸附、光生电子与空穴的迁移及产物的脱附过程。重点介绍了光催化CO2和CH4重整过程中贵金属催化剂、非贵金属催化剂及碳氮化合物等催化剂的研究进展,并总结归纳了各类催化剂的优点与不足。最后,本文探讨了光催化转化CO2与CH4制合成气研究领域未来可能的发展方向:开发设计高效的光催化剂提高反应效率;通过密度泛函理论计算及高端表征技术探究催化机理。 相似文献
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以Al2O3为载体,采用浸渍法制备了Cu、Co、Ni、Pt/Al2O3四种单一组分催化剂(M/Al2O3)。研究了M/Al2O3催化剂对丙三醇水蒸气重整制氢反应的适用性及反应行为;考察了制备条件及还原条件,通过活性、稳定性及抗积炭性进行了催化剂的活性评价,并对催化剂进行了TPR、XRD表征。研究发现M/Al2O3催化剂用于丙三醇水蒸气重整制氢均表现出一定活性;其中Cu/Al2O3催化剂具有一定的抗积炭性;Pt/Al2O3催化剂表现出较好的抗积炭性、高温活性,但稳定性较差;Co/Al2O3催化剂表现出较好的稳定性;Ni/Al2O3催化剂表现出较好的低温活性。 相似文献
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随着人类社会工业化进程的加快,温室气体排放量随之增加,导致温室效应加剧。在所有温室气体中,CO2占比最多、贡献最大,被认为是引起全球变暖的主要因素。人为排放的CO2主要来自工业生产过程中化石燃料的燃烧,为实现碳中和目标,除了推广清洁能源、提高能源利用效率和增加植物碳汇等措施外,对工业排放的CO2进行捕集封存必不可少。目前限制CO2捕集和分离工艺应用的主要因素是成本过高,为解决该问题,开发第2代低能耗固体CO2吸附材料对推动工业源CO2减排具有重要意义。Li4SiO4凭借较高的吸附容量、较低的再生能耗和成本在高温CO2捕集领域具有良好的应用前景。为推进Li4SiO4材料在碳捕集、利用和封存(CCUS)工艺中的应用,综述了Li4SiO4基吸附材料的研究进展,介绍了不同合成方法及合成条件对Li4 相似文献
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吸附强化蒸汽重整(SESR)制氢技术是集重整反应(H2生产)和选择性分离(CO2吸附)于一体的新型技术。该技术的特点为采用固体吸附剂在高温下对CO2进行原位脱除,以改变反应的正常平衡极限,提高烃类转化率,提高H2产量,减少CO2排放。在整个SESR制氢技术中,吸附剂的选择与反应条件至关重要。本文探讨了CaO、水滑石、Li2ZrO3、Li2SiO3以及双功能吸附剂在SESR制氢过程中的性能,总结了提高这些吸附剂吸附性能的不同方法。确定了固体吸附剂的反应条件,如温度、压力、水蒸气量等因素的影响及相关的反应机理。分析表明,CaO基吸附剂由于其低廉的价格及较高的吸附能力,被认为是最具潜力的吸附剂,然而在SESR制氢过程中,CaO基吸附剂面临着多次循环再生后吸附能力衰减的挑战。集吸附与催化双重功能的吸附催化材料由于可以克服SESR制氢中不同固体催化剂和吸附剂的匹配问题、降低所用固体材料的成本,从而使其在吸附强化蒸汽重整制氢方面具有巨大优势,并成为该领域未来研究的一个重要方向。 相似文献
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吸附强化的甲烷水蒸汽重整制氢反应特性 总被引:1,自引:0,他引:1
在实验室固定床反应器上研究了采用复合催化剂的吸附强化甲烷水蒸汽重整制氢反应,对吸附强化制氢反应条件进行了考查,得到了实验室条件下的最佳反应条件为温度600~640 ℃,压力0.2 MPa,水碳比4~5.在600 ℃,0.2 MPa,水碳比5的条件下,吸附强化段H2含量高达95.39%,吸附强化段CH4转化率达到81.37%,相对于理论平衡值的吸附强化因子达到26.76%. 相似文献
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采用生物质模板(茶花粉)掺杂制备SAPO-34分子筛,研究了SAPO-34分子筛对CO2和CH4的静态吸附性能,同时考察了水热晶化时间、硅铝摩尔比(SiO2/Al2O3摩尔比)和有机模板剂对茶花粉掺杂合成SAPO-34分子筛的影响。结果表明,茶花粉的加入可以制备性能良好的SAPO-34分子筛并降低其尺寸在1~2μm之间;晶化时间(24~36 h)的延长有利于分子筛结晶;当硅铝比为0.6、有机模板剂摩尔比为2时,SAPO-34分子筛的晶化效果最佳。茶花粉清液合成的SAPO-34分子筛在静态吸附实验压力为100 kPa时,CO2和CH4的总吸附量分别为2.92 mmol/g和0.58 mmol/g, CO2/CH4的理想分离系数为5.05。 相似文献
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随着世界经济的快速发展,能源短缺和环境污染已成为关注焦点,化石燃料的快速消耗使得温室效应持续增强,对全球环境和气候造成了严重影响。利用丰富和清洁的太阳能驱动的方式可以快速靶向供热,在温和条件下将2种主要温室气体(CH4/CO2)转化为有价值的合成气,可以大幅降低传统热催化过程所产生的能耗及碳排放。然而,当前太阳能直接驱动干重整制合成气技术距离工业应用仍有一些距离,存在反应分子转化速率低、光能-化学能转化效率低、催化剂易烧结及积碳造成的催化剂失活等问题。针对干重整反应的固有特性以及当前光热研究领域普遍存在的问题,围绕该反应涉及的催化剂制备、载体构筑、反应器及系统搭建与优化,详细介绍了光热干重整反应的研究进展,最后展望了太阳能直接驱动光热催化干重整体系的前景和挑战。 相似文献
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Surface-phase ZrO2 on SiO2 (SZrOs) and surface-phase La2O3 on Al2O3 (SLaOs) were prepared with various loadings of ZrO2 and La2O3, characterized and used as supports for preparing Pt/SZrOs and Pt/SLaOs catalysts. CH4/CO2 reforming over the Pt/SZrOs and Pt/SLaOs catalysts was examined and compared with Pt/Al2O3 and Pt/SiO2 catalysts. CO2 or CH4 pulse reaction/adsorption analysis was employed to elucidate the effects of these surface-phase oxides.
The zirconia can be homogeneously dispersed on SiO2 to form a stable surface-phase oxide. The lanthana cannot be spread well on Al2O3, but it forms a stable amorphous oxide with Al2O3. The Pt/SZrOs and Pt/SLaOs catalysts showed higher steady activity than did Pt/SiO2 and Pt/Al2O3 by a factor of three to four. The Pt/SZrOs and Pt/SLaOs catalysts were also much more stable than the Pt/SiO2 and Pt/Al2O3 catalysts for long stream time and for reforming temperatures above 700 °C. These findings were attributed to the activation of CO2 adsorbed on the basic sites of SZrOs and SLaOs. 相似文献
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Photocatalytic reduction of CO2 with H2O on Ti-MCM-41 and Ti-MCM-48 mesoporous zeolite catalysts 总被引:1,自引:0,他引:1
Masakazu Anpo Hiromi Yamashita Keita Ikeue Yo Fujii Shu Guo Zhang Yuichi Ichihashi Dal Ryung Park Yasuo Suzuki Keiko Koyano Takashi Tatsumi 《Catalysis Today》1998,44(1-4):327-332
Titanium oxide species included within the framework of mesoporous zeolites (Ti-MCM-41 and Ti-MCM-48) prepared by a hydrothermal synthesis exhibited high and unique photocatalytic reactivity for the reduction of CO2 with H2O at 328 K to produce CH4 and CH3OH in the gas phase. In situ photoluminescence, diffuse reflectance absorption, ESR and XAFS investigations indicated that the titanium oxide species are highly dispersed within the zeolite framework and exist in tetrahedral coordination. The charge transfer excited state of the highly dispersed titanium oxide species played a significant role in the reduction of CO2 with H2O exhibiting a high selectivity for the formation of CH3OH. 相似文献
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Zheng Xu Yumin Li Jiyan Zhang Liu Chang Rongqi Zhou Zhanting Duan 《Applied Catalysis A: General》2001,210(1-2):45-53
The effects of nickel loading, calcination temperature, support, and basic additives on Ni-based catalyst structure and reactivity for CH4 reforming with CO2 were investigated. The results show that the structure of the nickel active phase strongly depends on the interactions of the metal and the support, which are related to the support properties, the additives and the preparation conditions. “Free” Ni species can be formed when the interaction is weak and their mobility makes them easily deactivated by coking and sintering. The effect of strong metal-support interaction (SMSI effect) is different for various supports. The formation of solid solution of Ni–Mg–O2 and the blocking of TiOx by the partially reduced TiO2 can both decrease the availability of Ni active sites in Ni/MgO and Ni/TiO2. The spinel NiAl2O4 formed in Ni/γ-Al2O3 might be responsible for its high activity and resistance to coking and sintering because it can produce a highly dispersed active phase and a large active surface area as bound-state Ni species when the catalyst is prepared at high calcined temperatures or with low nickel loading. The addition of La2O3 or MgO as alumina modifiers can also be beneficial for the performance of the Ni/γ-Al2O3 catalyst. 相似文献
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Conversion of NOx with reducing agents H2, CO and CH4, with and without O2, H2O, and CO2 were studied with catalysts based on MOR zeolite loaded with palladium and cerium. The catalysts reached high NOx to N2 conversion with H2 and CO (>90% conversion and N2 selectivity) range under lean conditions. The formation of N2O is absent in the presence of both H2 and CO together with oxygen in the feed, which will be the case in lean engine exhaust. PdMOR shows synergic co-operation between H2 and CO at 450–500 K. The positive effect of cerium is significant in the case of H2 and CH4 reducing agent but is less obvious with H2/CO mixture and under lean conditions. Cerium lowers the reducibility of Pd species in the zeolite micropores. The catalysts showed excellent stability at temperatures up to 673 K in a feed with 2500 ppm CH4, 500 ppm NO, 5% O2, 10% H2O (0–1% H2), N2 balance but deactivation is noticed at higher temperatures. Combining results of the present study with those of previous studies it shows that the PdMOR-based catalysts are good catalysts for NOx reduction with H2, CO, hydrocarbons, alcohols and aldehydes under lean conditions at temperatures up to 673 K. 相似文献
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Esther Ochoa-Fernndez Hans Kristian Rusten Hugo Atle Jakobsen Magnus Rnning Anders Holmen De Chen 《Catalysis Today》2005,106(1-4):41-46
The kinetics of CO2 sorption on a solid adsorbent, namely lithium zirconate, have been studied in an oscillating microbalance. The solid sorbent has been prepared by a novel route resulting in a high capacity, good stability and much improved sorption rates, making it suitable for its application in sorption enhanced hydrogen production by steam methane reforming. A kinetic equation for the sorption kinetics as a function of CO2 partial pressure and temperature has been developed. The hydrogen production by sorption enhanced reaction process has been simulated by a dynamic one-dimensional pseudo-homogenous model of a fixed-bed reactor, where a hydrotalcite-derived Ni catalyst has been used as steam reforming catalysts. Simulation results show that hydrogen purer than 95% with a concentration of carbon monoxide lower than 0.2 mol% can be produced in a single step. 相似文献
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Roles of CO2 and H2O as oxidants are discussed based on the data on the substrate conversions and the product distributions in the nonthermal plasma reforming of aliphatic hydrocarbons such as methane, propane, and neopentane from 303 K to 433 K. Only small effects of initial concentrations of hydrocarbons and types of oxidants are observed on hydrocarbon conversions, and the initial chemical interaction between hydrocarbons and the oxidants unlikely occurs. CO2 and H2O have shown the comparable oxidation powers in the hydrocarbon reforming. Two molar excess of CO2 or H2O to methane is required to oxidize methane carbon atoms to CO and CO2, and larger amounts of CO2 or H2O for propane and neopentane. The different natures of CO2 and H2O are reflected in the synthesis gas composition as in the ordinary catalytic reforming processes at higher temperatures: higher H2 yields and higher H2 to CO ratios on addition of H2O. 相似文献
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CH4/CO2 reforming over La2NiO4 and 10%NiO/CeO2–La2O3 catalysts under the condition of supersonic jet expansion was studied via direct monitoring of the reactants and products using the sensitive technique of cavity ring-down spectroscopy. Vibration–rotational absorption lines of CH4, H2O, CO2 and CO molecules were recorded in the near infrared spectral region. Our results indicated that La2NiO4 is superior to 10%NiO/CeO2–La2O3 in performance. In addition, we observed enhanced reverse-water-gas-shift reaction at augmented reaction temperature. The formation of reaction intermediates was also investigated by means of time-of-flight mass spectrometry and there was the detection of CHx+, OH+ and H+ species. 相似文献
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M. Rezaei S.M. Alavi S. Sahebdelfar Peng Bai Xinmei Liu Zi-Feng Yan 《Applied catalysis. B, Environmental》2008,77(3-4):346-354
Mesoporous nanocrystalline zirconia with high-surface area and pure tetragonal crystalline phase has been prepared by the surfactant-assisted route, using Pluronic P123 block copolymer surfactant. The synthesized zirconia showed a surface area of 174 m2 g−1 after calcination at 700 °C for 4 h. The prepared zirconia was employed as a support for nickel catalysts in dry reforming reaction. It was found that these catalysts possessed a mesoporous structure and even high-surface area. The activity results indicated that the nickel catalyst showed stable activity for syngas production with a decrease of about 4% in methane conversion after 50 h of reaction. Addition of promoters (CeO2, La2O3 and K2O) to the catalyst improved both the activity and stability of the nickel catalyst, without any decrease in methane conversion after 50 h of reaction. 相似文献
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Pt/MgO catalysts were prepared by wet impregnation. At 800 °C and atmospheric pressure, Pt/MgO catalysts exhibited a high stability at high gas hourly space velocity of 36,000 ml/g h with a CH4/CO2 ratio of 1.0. During 72 h time on stream, the conversion of CH4 and CO2 remained almost constant, at about 88% and 90%, respectively. There was no loss of Pt. After reaction, the XRD peaks of MgO became broader, indicating amorphization of MgO, which was supported by TEM results. XPS indicated that the reforming reaction had little influence on Pt. CO2-TPSR results showed that some carbon deposition occurred under stoichiometric feed of CH4 and CO2, but it did not result in the deactivation of the catalyst. The deposited carbon came mainly from the decomposition of methane. 相似文献
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介绍CO2汽提法尿素装置合成系统的NH3/CO2的控制方法,合成系统NH3/CO2异常的症状,判断方法,偏离正常时的处理和防范措施。 相似文献