4.6 Article

Precise regulation of acid pretreatment for red mud SCR catalyst: Targeting on optimizing the acidity and reducibility

出版社

HIGHER EDUCATION PRESS
DOI: 10.1007/s11783-021-1447-x

关键词

Air pollution control; Nitrogen oxides; Selective catalytic reduction; Red mud; Solid waste utilization

资金

  1. National Natural Science Foundation of China [21906090]
  2. National Key Research and Development Program of China [2017YFC0210200, 2017YFC0212800]
  3. Primary Research & Development Project of Shandong Province (China) [2018GSF117034, 2019JZZY020305]

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In this study, the researchers achieved directional control of the chemical state of active sites in red mud by tuning the acid pretreatment process. Dealkalization improved the acidity and reducibility of red mud, leading to high NOx conversion and SCR performance of the activated catalysts at pH values of 3 and 5.
Red mud (RM), as an alkaline waste, was recently proved to be a promising substitute for the SCR catalyst. Dealkalization could improve the acidity and reducibility of red mud, which were critical for SCR reaction. However, the dealkalization effect depended on the reaction between acid solution and red mud. In this study, we realized the directional control of the chemical state of active sites through tuning the acid pretreatment (dealkalization) process. The pretreatment endpoint was controlled at pH values of 3-5 with diluted nitric acid. When the pH values of red mud were 3 and 5 (CRM-3 and CRM-5), activated catalysts showed NOx conversion above 90% at 275 degrees C-475 degrees C. The high initial reaction rate, Ce3+/(Ce3+ + Ce4+) ratio, and surface acidity accounted for the excellent SCR performance of CRM-5 catalyst. Meanwhile, more Fe3+ on the CRM-3 surface improved the NH3 adsorption. There was a strong interaction between Al and Fe in both CRM-5 and CRM-3 catalysts. DFT results showed that the adsorption capacity of the Al-O-3-Fe for NH3 and NO is stronger than that of Fe-O-3-Fe, which enhanced the NOx conversion of the catalyst. However, the almandine was formed in CRM-4, consumed part of Fe3+ and Al3+, and the interaction between Al and Fe was weakened. Also, deposited almandine on the catalyst surface covered the active sites, thus leading to lower NH3-SCR activity. (C) Higher Education Press 2021

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