PMID- 35926302 OWN - NLM STAT- MEDLINE DCOM- 20221011 LR - 20221011 IS - 1095-7103 (Electronic) IS - 0021-9797 (Linking) VI - 628 IP - Pt A DP - 2022 Dec 15 TI - Reveal of free radicals in manganese-based catalysts and their roles during selective catalytic reduction of nitrogen oxide. PG - 193-204 LID - S0021-9797(22)01273-5 [pii] LID - 10.1016/j.jcis.2022.07.093 [doi] AB - HYPOTHESIS: Manganese-based catalysts attract extensive attentions in low-temperature selective catalytic reduction (SCR) of nitrogen oxide (NO(x)). However, seldom work focuses on the existence of free radicals and their roles in SCR. EXPERIMENTS: In this work, electron paramagnetic resonance spectrometer and density functional theory are combined to reveal surface characterizations of manganese oxide and Ce/La-doped manganese oxides. FINDINGS: As a result, superoxide radical (O(2)*) exists on manganese-oxide surface, produces nitrogen-containing free radical, and functions as electron transfer between NO(x) and NH(3) at 100  degrees C, resulting in good NO(x) conversion as well as N(2) selectivity at the same time. The O(2)* is born of accepting electrons on adsorbed oxygen through overlapped orbits of Mn-d and O-p. Additional metal doping increases the percentage of O(2)* among all oxygen species from 2.9 % to 6.9 % (Ce doping) and 5.1 % (La doping). The order of O(2)* percentage is consistent with the NO(x)-conversion order at 100  degrees C, i.e., Ce doping (91.6 %) > La doping (55.7 %) > catalyst without doping (27.5 %). Above result helps to understand interface behaviors of manganese-based catalyst in SCR. This work is also in favor of developing more effective low-temperature catalysts. CI - Copyright (c) 2022 Elsevier Inc. All rights reserved. FAU - Hou, Luman AU - Hou L AD - Materials Genome Institute, Shanghai University, 333 Nanchen Road, Shanghai 200444, China. FAU - Wen, Yuling AU - Wen Y AD - SHU Center of Green Urban Mining & Industry Ecology, School of Environmental and Chemical Engineering, Shanghai University, No. 381 Nanchen Road, Shanghai 200444, China. FAU - Wu, Jianzhong AU - Wu J AD - Materials Genome Institute, Shanghai University, 333 Nanchen Road, Shanghai 200444, China. FAU - Yue, Yang AU - Yue Y AD - Materials Genome Institute, Shanghai University, 333 Nanchen Road, Shanghai 200444, China. FAU - Zhang, Jia AU - Zhang J AD - SHU Center of Green Urban Mining & Industry Ecology, School of Environmental and Chemical Engineering, Shanghai University, No. 381 Nanchen Road, Shanghai 200444, China. Electronic address: irujam@t.shu.edu.cn. FAU - Zhang, Jincang AU - Zhang J AD - Materials Genome Institute, Shanghai University, 333 Nanchen Road, Shanghai 200444, China. Electronic address: jczhang@shu.edu.cn. FAU - Qian, Guangren AU - Qian G AD - Materials Genome Institute, Shanghai University, 333 Nanchen Road, Shanghai 200444, China. LA - eng PT - Journal Article DEP - 20220718 PL - United States TA - J Colloid Interface Sci JT - Journal of colloid and interface science JID - 0043125 RN - 0 (Ions) RN - 0 (Manganese Compounds) RN - 0 (Nitrogen Oxides) RN - 0 (Oxides) RN - 11062-77-4 (Superoxides) RN - 31C4KY9ESH (Nitric Oxide) RN - 42Z2K6ZL8P (Manganese) RN - 64J2OA7MH3 (manganese oxide) RN - 7664-41-7 (Ammonia) RN - N762921K75 (Nitrogen) RN - S88TT14065 (Oxygen) SB - IM MH - Ammonia MH - Catalysis MH - Ions MH - *Manganese MH - Manganese Compounds MH - Nitric Oxide MH - Nitrogen MH - Nitrogen Oxides MH - Oxidation-Reduction MH - Oxides MH - Oxygen MH - *Superoxides MH - Temperature OTO - NOTNLM OT - Manganese oxide OT - Nitrogen oxide OT - Nitrogen-containing free radical OT - Selective catalytic reduction OT - Superoxide radical COIS- Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. EDAT- 2022/08/05 06:00 MHDA- 2022/10/12 06:00 CRDT- 2022/08/04 18:19 PHST- 2022/04/23 00:00 [received] PHST- 2022/06/07 00:00 [revised] PHST- 2022/07/15 00:00 [accepted] PHST- 2022/08/05 06:00 [pubmed] PHST- 2022/10/12 06:00 [medline] PHST- 2022/08/04 18:19 [entrez] AID - S0021-9797(22)01273-5 [pii] AID - 10.1016/j.jcis.2022.07.093 [doi] PST - ppublish SO - J Colloid Interface Sci. 2022 Dec 15;628(Pt A):193-204. doi: 10.1016/j.jcis.2022.07.093. Epub 2022 Jul 18.