Highly selective catalytic reduction of NO via SO2/H2O-tolerant spinel catalysts at low temperature.
Selective catalytic reduction of NO X by hydrogen (H2-SCR) in the presence of oxygen has been investigated over the NiCo2O4 and Pd-doped NiCo2O4 catalysts under varying conditions. The catalysts were prepared by a sol-gel method in the presence of oxygen within 50-350 °C and were characterized using XRD, BET, EDS, XPS, Raman, H2-TPR, and NH3-TPD analysis. The results demonstrated that the doped Pd could improve the catalyst reducibility and change the surface acidity and redox properties, resulting in a higher catalytic performance. The performance of NiCo1.95Pd0.05O4 was consistently better than that of NiCo2O4 within the 150-350 °C range at a gas hourly space velocity (GHSV) of 4800 mL g(-1) h(-1), with a feed stream containing 1070 ppm NO, 10,700 ppm H2, 2 % O2, and N2 as balance gas. The effects of GHSV, NO/H2 ratios, and O2 feed concentration on the NO conversion over the NiCo2O4 and NiCo1.95Pd0.05O4 catalysts were also investigated. The two samples similarly showed that an increase in GHSV from 4800 to 9600 mL h(-1) g(-1), the NO/H2 ratio from 1:10 to 1:1, and the O2 content from 0 to 6 % would result in a decrease in NO conversion. In addition, 2 %, 5 %, and 8 % H2O into the feed gas had a slightly negative influence on SCR activity over the two catalysts. The effect of SO2 on the SCR activity indicated that the NiCo1.95Pd0.05O4 possesses better SO2 tolerance than NiCo2O4 catalyst does. Graphical abstract The NiCo1.95Pd0.05O4 catalyst achieved over 90 % NO conversion with N2 selectivity of 100 % in the 200∼250 °C range than the maximum 40.5 % NO conversion over NiCo2O4 with N2 selectivity of approximately 80 % in 350 °C.
School of Resources and Environmental Engineering, State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai, 200237, China.
Xuanxuan
X
Cai
School of Resources and Environmental Engineering, State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai, 200237, China.
Wei
W
Sun
School of Resources and Environmental Engineering, State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai, 200237, China.
Chaochao
C
Xu
School of Resources and Environmental Engineering, State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai, 200237, China.
Limei
L
Cao
School of Resources and Environmental Engineering, State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai, 200237, China. yangji@ecust.edu.cn.
Ji
J
Yang
D000537:Aluminum Oxide / Q000737:chemistry*; D000641:Ammonia; D002384:Catalysis; D003080:Cold Temperature; D005740:Gases; D006859:Hydrogen; D008277:Magnesium Oxide / Q000737:chemistry*; D008956:Models, Chemical; D009589:Nitrogen Oxides / Q000737:chemistry*; D010084:Oxidation-Reduction; D010100:Oxygen; D013458:Sulfur Dioxide / Q000737:chemistry*; D013696:Temperature; D014867:Water / Q000737:chemistry*
D005740:Gases; D009589:Nitrogen Oxides; C111130:spinell; D014867:Water; D013458:Sulfur Dioxide; D008277:Magnesium Oxide; D000641:Ammonia; D006859:Hydrogen; D000537:Aluminum Oxide; D010100:Oxygen
Flue gas; Gas treatment; Hydrogen; NO X; SCR; SO2/H2O-tolerant