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CO2和CH4均是温室气体的重要成员并且数量可观,其资源化利用对于应对气候变化和能源危机具有重要意义。甲烷干重整是经典转化方式之一,将CO2"供氧"还原反应和CH4"需氧"氧化反应结合起来并相互转化,其产物合成气(H2和CO)可用于费-托合成碳氢化合物液态燃料。近年来,干重整已经成为能源环境领域热点之一,在重整新工艺和催化剂设计策略方面取得了重要进展,推动了高活性和高稳定性催化剂和新工艺研发。详细综述了甲烷干重整工艺和催化剂的研究成果,重点介绍了干重整工艺新发展和催化剂功能设计,结合Ni-载体相互作用、双金属协同效应、界面效应、单原子催化等新策略对干重整工艺中的基础科学问题进行了探讨,并对干重整技术现有难点和未来发展方向进行了展望。 相似文献
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通过共沉淀法制备了Pr0.7Zr0.3O2-δ复合氧化物氧载体,考察了制备温度、老化时间、pH以及母液浓度对Pr-Zr固溶体形成的影响,借助XRD、H2-TPR、O2-TPD和甲烷气-固反应等手段,进行了Pr-Zr固溶体制备最优路径的探索与其氧化性能的研究。结果表明:以Pr(NO3)3·6H2O和Zr(NO3)4为前驱盐,沉淀温度20℃、pH=12、800℃焙烧可制得Pr0.7Zr0.3O2-δ完美固溶体,固溶体的形成可增强材料晶格氧的移动性,从而提高其与甲烷的反应活性。 相似文献
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Chemical interaction of Ce-Fe mixed oxides was investigated in methane selective oxidation via methane temperature programmed reduction and methane isothermal reaction tests over Ce-Fe oxygen carriers. In methane temperature programmed reduction test, Ce-Fe oxide behaved complete oxidation at the lower temperature and selective oxidation at higher temperatures. Ce-Fe mixed oxides with the Fe content in the range of 0.1–0.5 was able to produce syngas with high selectivity in high-temperature range(800–900 °C), and a higher Fe amount over 0.5 seemed to depress the CO formation. In isothermal reaction, complete oxidation occurred at beginning following with selective oxidation later. Ce1–xFexO2–δ oxygen carriers(x≤0.5) were proved to be suitable for the selective oxidation of methane. Ce-Fe mixed oxides had the well-pleasing reducibility with high oxygen releasing rate and CO selectivity due to the interaction between Ce and Fe species. Strong chemical interaction of Ce-Fe mixed oxides originated from both Fe*activated CeO2 and Ce3+ activated iron oxides(FeOm), and those chemical interaction greatly enhanced the oxygen mobility and selectivity. 相似文献
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以共沉淀法制备的Pr0.7Zr0.3O2-δ固溶体作为氧载体,研究其在选择性氧化甲烷制取合成气工艺(CH4/空气氧化还原循环)中的服役性能。结合X射线衍射(XRD)、H2-程序升温还原(H2-TPR)、O2-程序升温脱附(O2-TPD)、比表面测试(BET)、X射线光电子能谱(XPS)表征手段描述氧载体在氧化还原循环反应过程中物化特性演变。结果表明,Pr0.7Zr0.3O2-δ固溶体在氧化还原反应中保持较高的甲烷反应活性与CO选择性,且能够保持反应性能稳定(CO选择性为83.5%~83.1%)。随着循环反应的进行,Pr-Zr固溶体保持了较高的热稳定性,但是表面氧的消失导致其还原性能下降。然而,表面氧的消失促进了氧空位的增加从而在一定程度上增强了氧移动能力,使足够的晶格氧参与到甲烷选择性氧化反应中,保证了较高的反应活性。通过比较新鲜、循环与老化后材料结构与还原性能,认为甲烷选择性氧化制取合成气工艺中的热点问题可以避免。 相似文献
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祝星家 《Canadian Metallurgical Quarterly》2011,28(8)
本文以新型氨法脱硫技术(SAAS)在重庆建峰工业集团有限公司自备热电厂2×80+2×130t/h锅炉烟气脱硫中的应用为例,对新型氨法脱硫技术(SAAS)的技术原理、工艺流程、运行效果、技术特点、参数影响、存在问题等进行了阐述。新型氨法脱硫技术在建峰热电厂的应用实践证明,该技术具有脱硫效率高,兼有一定除尘脱销功能,基本没有二次污染,对原煤硫含量适应性广,可以实现变废为宝产出符合国家标准的农用肥料等的技术特点,具有明显的环境效益和社会效益。 相似文献
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A series of Ce-Fe-Zr-O(x)/MgO(x denotes the mass fraction of Ce-Fe-Zr-O,x=10%,15%,20%,25%,30%) complex oxide oxygen carriers for selective oxidation of methane to synthesis gas were prepared by the co-precipitation method.The catalysts were characterized by means of X-ray diffraction and H2-TPR.The XRD measurements showed that MgFeO4 particles were formed and Fe2O3 particles well dispersed on the oxygen carriers.The reactions between methane diluted by argon(10% CH4) and oxygen carriers were investigated.Suitable content of CeO2/Fe2O3/ZrO2 mixed oxides could promote the reaction between methane and oxygen carriers.There are mainly two kinds of oxygen of carriers:surface lattice oxygen which had higher activity but lower selectivity,and bulk lattice oxygen which had lower activity but higher selectivity.Among all the catalysts,Ce-Fe-Zr-O(20%)/MgO exhibited the best catalytic performance.The conversion of the methane was above 56%,and the selectivity of the H2 and CO were both above 93%,the ratio of H2/CO was stable and approached to 2 for a long time. 相似文献
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采用真空电弧熔炼技术结合水冷铜模快速凝固工艺制备出在一定温度范围内具有负热膨胀行为的系列成分富Ti含量Ti_(100-x)Ni_x(x=38~50,摩尔分数,%)熔铸态与吸铸态合金。结果表明:合金的负热膨胀行为主要源于升温过程中B19′→B2逆马氏体相变所引起的体积变化。富Ti含量Ti-Ni合金在室温下的主要物相为B19′-NiTi相和Ti_2Ni相,通过热膨胀实验数据和混合定则(ROM)计算所得的B19′相、Ti_2Ni相和B2相的热膨胀系数值与文献报道实验结果非常接近。所制备合金的显微组织具有明显择优取向生长特征,导致合金的负热膨胀行为呈现显著的各向异性。当合金中Ni含量增加时,样品的负热膨胀系数沿最大冷却速率方向增大,而在垂直于最大冷却速率方向上先增大后减小。 相似文献