不同助剂对Ru/CeO_(2)-NR的氨合成性能研究  

Influences of different promoters on performance of Ru/CeO_(2)-NR in ammonia synthesis

作　　者：张江涛 王鹏[1,2] 王爽[1,2] ZHANG Jiang-tao;WANG Peng;WANG Shuang(College of Environmental Science and Engineering,Taiyuan University of Technology,Jinzhong 030600,China;Shanxi Key Laboratory of Gas Energy Efficient and Clean Utilization,Taiyuan University of Technology,Taiyuan 030024,China)

机构地区：[1]太原理工大学环境科学与工程学院,山西晋中030600 [2]太原理工大学,气体能源高效清洁利用山西省重点实验室,山西太原030024

出　　处：《现代化工》2023年第1期98-103,109,共7页Modern Chemical Industry

基　　金：国家自然科学基金(22078215);山西省自然科学基金(201901D211117);山西省省筹留学归国人员基金(2021-055)。

摘　　要：以2.5%Ru/CeO_(2)-NR为母体,通过浸渍法制备不同助剂负载的钌基催化剂X-2.5%Ru/CeO_(2)-NR(X分别为4%K、4%Ba、4%Cs、2%K 2%Ba、2%K 2%Cs、2%Ba 2%Cs),并在温和条件下对其进行了氨合成性能测试。结果表明,不同的助剂组成对催化剂的促进作用大小顺序为:电子(4%Cs)≥电子+结构(2%Ba 2%Cs)>电子+电子(2%K 2%Cs)>结构(4%Ba);其中,4%Cs-2.5%Ru/CeO_(2)-NR展示了最佳的氨合成性能,在1 MPa、400℃、H_(2)/N_(2)体积比为1的条件下氨产率可达16500μmol/(g·h),该产率与1 MPa、450℃、H_(2)/N_(2)体积比为3条件下的氨产率相当。测试结果表明,适宜的反应参数、Ru0质量分数及Ce^(3+)/Ce^(4+)比是钌基氨合成催化剂具有较高催化性能的关键。Using 2.5%Ru/CeO_(2)-NR as matrix,ruthenium-based catalysts X-2.5%Ru/CeO_(2)-NR loaded with different promoters are prepared via the impregnation method(X=4%K,4%Ba,4%Cs,2%K+2%Ba,2%K+2%Cs,and 2%Ba+2%Cs,respectively).Their performance in ammonia synthesis is tested under mild conditions.Experimental results show that the promoting effects of different promoters on the catalysts are in the following order:electron(4%Cs)≥electron+structure(2%Ba+2%Cs)>electron+electron(2%K+2%Cs)>structure(4%Ba).Among them,4%Cs-2.5%Ru/CeO_(2)-NR displays the best performance in ammonia synthesis,over which the yield of ammonia can reach 16500μmol·g-1·h-1under the conditions of 1 MPa,400℃and v(H_(2))/v(N_(2))=1.The yield is equal to that under the conditions of 1 MPa,450℃and v(H_(2))/v(N_(2))=3.The test results exhibit that the suitable reaction parameters,the content of Ru~0 and the ratio of Ce^(3+)/Ce^(4+)are the keys to the high catalytic performance of ruthenium-based catalysts in ammonia synthesis.

关 键 词：合成氨 二氧化铈载体 钌基催化剂 助剂 

分 类 号：X703.1[环境科学与工程—环境工程]