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MgO/h-BN复合载体对Ba-Ru/MgO/h-BN氨合成催化剂性能的影响(英文)
  • ISSN号:0253-9837
  • 期刊名称:《催化学报》
  • 时间:0
  • 分类:O643[理学—物理化学;理学—化学]
  • 作者机构:[1]中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室,甘肃兰州730000, [2]中国科学院研究生院,北京100049
  • 相关基金:国家自然科学基金(20576025); 国家杰出青年科学基金(20625308)
中文摘要:

采用浸渍法制备了系列不同质量比的MgO/h-BN复合载体负载的Ru基氨合成催化剂,采用X射线衍射、N2低温物理吸附、X射线荧光、扫描电镜、透射电镜、程序升温分析等手段对催化剂进行了详细的表征,并在固定床反应器上考察了它们在氨合成反应中的催化性能.结果表明,MgO/h-BN复合载体中h-BN含量对催化剂活性的影响较大,Ba-Ru[1:1](摩尔比)/MgO/h-BN[8:2](质量比),Ba-Ru[1:1]/MgO/h-BN[6:4]和Ba-Ru[1:1]/MgO/h-BN[5:5]催化剂上氨合成活性均高于Ba-Ru/MgO催化剂.在425°C,5.0MPa,N2/H2=1/3和5000h?1条件下,Ba-Ru[1:1]/MgO/h-BN[8:2]表现出最优催化活性,达506.9ml/(gcat·h).这可归因于MgO/h-BN复合载体上存在较高数量的碱性位,特别是弱碱性位和中等强度碱性位,而这些碱性位可能是由MgO和h-BN之间的相互作用造成.

英文摘要:

A series of MgO/hexagonal boron nitride (h-BN) composite with different mass ratio were synthesized by impregnation method and used as supports for ruthenium catalysts in ammonia synthesis reaction. The catalysts were characterized by X-ray diffraction, N2 physical adsorption, X-ray fluorescent spectrometer, scanning electron microscope, transmission electron microscope, temperature programmed reduction of H2, and temperature programmed desorption of CO2 (CO2-TPD). The activity measurements of ammonia synthesis were carried out in a fixed-bed flow reactor with a mixture of N2 and H2 atomsphere under steady-state conditions (5.0 MPa, 350–500 °C, 5000 h–1). The results showed that the rate of ammonia formation was strongly influenced by the h-BN content used in the catalysts preparation process. The Ba-Ru[1:1] (molar ratio of Ba to Ru = 1:1)/MgO/h-BN[8:2] (weight ratio of MgO to h-BN = 8:2), Ba-Ru[1:1]/MgO/h-BN[6:4] and Ba-Ru[1:1]/MgO/h-BN[5:5] catalysts exhibited higher activity than Ba-promoted Ru/MgO catalyst. At 425 °C, 5.0 MPa, flow rate of 5000 h–1, and a N2/H2 = 1/3 atmosphere, the optimum activity of 506.9 ml/(gcat·h) was achieved when MgO/h-BN[8:2] was used as the catalytic support. The execllent activity was mainly attributed to the basicity of the MgO/h-BN combination-type support, especially "weak" and "medium" basic sites. Large numbers of basic sites were observed from CO2-TPD characterization due to the interaction between MgO and the h-BN material

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期刊信息
  • 《催化学报》
  • 北大核心期刊(2011版)
  • 主管单位:中国科学院
  • 主办单位:中国化学会 中国科学院大连化学物理研究所
  • 主编:李灿 张涛
  • 地址:大连市沙河口区中山路457号
  • 邮编:116023
  • 邮箱:chxb@dicp.ac.cn
  • 电话:0411-84379240
  • 国际标准刊号:ISSN:0253-9837
  • 国内统一刊号:ISSN:21-1195/O6
  • 邮发代号:8-93
  • 获奖情况:
  • 第三届国家期刊奖提名奖,中国科协精品科技期刊示范项目
  • 国内外数据库收录:
  • 俄罗斯文摘杂志,美国化学文摘(网络版),荷兰文摘与引文数据库,美国工程索引,美国剑桥科学文摘,美国科学引文索引(扩展库),日本日本科学技术振兴机构数据库,中国中国科技核心期刊,中国北大核心期刊(2004版),中国北大核心期刊(2008版),中国北大核心期刊(2011版),中国北大核心期刊(2014版),英国英国皇家化学学会文摘,中国北大核心期刊(2000版)
  • 被引量:19199