辽宁科技大学化学工程学院,辽宁 鞍山 114051
李艳鹰(1994—),女,硕士研究生,liyanying1994@163.com
李先春(1972—),男,教授,askd1972@163.com
收稿:2018-08-20,
修回:2018-11-20,
网络首发:2026-07-24,
纸质出版:2019-03-05
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李艳鹰, 李先春. 生物质活性炭负载零价铁纳米晶簇直接催化还原NO[J]. 化工学报, 2019, 70(3): 1111-1119
LI Yanying, LI Xianchun. Biomass activated carbon loaded with zero-valent iron nanocrystal clusters for direct catalytic reduction of NO[J]. CIESC Journal, 2019, 70(3): 1111-1119
李艳鹰, 李先春. 生物质活性炭负载零价铁纳米晶簇直接催化还原NO[J]. 化工学报, 2019, 70(3): 1111-1119 DOI: 10.11949/j.issn.0438-1157.20180947.
LI Yanying, LI Xianchun. Biomass activated carbon loaded with zero-valent iron nanocrystal clusters for direct catalytic reduction of NO[J]. CIESC Journal, 2019, 70(3): 1111-1119 DOI: 10.11949/j.issn.0438-1157.20180947.
采用等体积浸渍法
制备以生物质活性炭为载体的纳米铁基催化剂,利用TG、SEM、XPS、Raman等分析仪器对催化剂进行表征,探讨了活性炭负载零价铁和铁氧化物在无氧条件下脱硝的机理。结果表明:在750℃热还原条件下制得的铁基催化剂具备较高的活性,其活性中心是分散均匀的零价铁纳米晶簇。在280℃无氧条件下对NO的脱除效率达100%,且避免了活性炭载体的损耗。研究发现,催化剂快速失活是由于零价Fe被氧化为Fe
3
O
4
,因而降低了脱硝剂的活性。直接对失活催化剂进行热还原可以完全恢复活性,但这种方法会消耗炭载体;利用CO作为还原剂进行制备与再生,可以有效提高纳米晶簇的分散性,延长脱硝寿命并减少炭载体的损失,为零价Fe催化剂在实际应用中提供了可能性。
The nano-iron-based catalysts with biomass activated carbon as carrier were prepared by equal volume impregnation method. The catalysts were characterized by TG
SEM
XPS
Raman and other analytical instruments. The activated carbon was loaded with zero-valent iron and iron oxide under anaerobic conditions. Actively developing a cheap catalyst suitable for coke oven flue gas denitrification at low temperature and no oxygen so that its flue gas emissions meet the national environmental protection standards is one of the research hotspots at the present stage. The mechanism of denitrification of zero-valent iron and iron oxides supported on activated carbon under anaerobic conditions is discussed. The results prove that the Fe-based catalyst prepared by thermal reduction at 750℃ has high activity
and its active center is the homogeneously dispersed zero-valent iron nanocrystalline cluster. The removal efficiency of NO at 280℃ is 100% and the loss of activated carbon carrier was avoided. The fast deactivation of the catalyst is due to the oxidation of zero-valent iron to Fe
3
O
4
thus reducing the activity of the denitrifying agent. The catalyst activity can be completely restored by heat treatment at 750℃ nitrogen atmosphere
but the carbon carrier will be consumed by regeneration method without adding reducing gas. The preparation and regeneration of CO as reducing agent can effectively improve the dispersion of nanocrystalline clusters
prolong the denitrification life and reduce the loss of carbon support
which provides the possibility for the application of zero valent Fe catalyst in pra
ctical application.
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