Promotion effect of Co addition on the activity and SO2 tolerance of CrCe catalysts for selective catalytic reduction of NOx with NH3 at middle–low temperatures

催化作用 化学 氧化还原 选择性催化还原 柠檬酸 路易斯酸 无机化学 氮氧化物 核化学 选择性 有机化学 燃烧
作者
Gai Zeng,Ninghan Wei,Xuehai Hu,Cheng Zhao,Junge Yun,Zimo Chen,Zhonghe Han,Liping Xiao,Zhihang Chen
出处
期刊:Journal of Chemical Technology & Biotechnology [Wiley]
卷期号:98 (10): 2506-2516 被引量:1
标识
DOI:10.1002/jctb.7477
摘要

Abstract Background Nitrogen oxides (NO x ) can result in a series of environmental issues (haze, photochemical smog and acid rain) that endanger human health. Currently, selective catalytic reduction (SCR) of NO x with ammonia (NH 3 ‐SCR) has been considered to be one of the most efficient techniques to eliminate NO x . Results Novel Co‐modified chromium/cerium (CrCe) catalysts were synthesized by the citric acid method to improve their insufficient SCR activity and sulfur dioxide (SO 2 ) resistance for NO x removal at middle–low temperatures. Cobalt (Co) addition could significantly increase the catalytic activity of CrCe catalysts, and the 5CoCrCe catalyst exhibited the highest catalytic activity with ≤95% NO x conversion and >80% N 2 selectivity within 180–280 °C. In addition, the 5CoCrCe catalyst exhibited outstanding SO 2 resistance as well as reversibility, with >90% NO conversion under 600 ppm SO 2 for 510 min. Conclusion It was determined by characterizations that Co addition can increase SSA, Cr 6+ concentration, electron transfer between Co and Cr by redox cycle (Cr 6+ + 4Co 2+ ↔ 4Co 3+ + Cr 2+ ) and the redox properties of the CrCe catalyst. The 5CoCrCe catalyst surface consists mainly of Lewis acid and its NH 3 ‐SCR reactions follows the Eley–Rideal (E–R) mechanism. The 5CoCrCe catalyst exhibited outstanding SO 2 resistance due to higher Cr 3+ , Ce 3+ and O α concentrations and strong redox cycles (3Ce 4+ + Cr 3+ ↔ 3Ce 3+ + Cr 6+ and Cr 6+ + 3Co 2+ ↔ 3Co 3+ + Cr 3+ ). Furthermore, in situ DRIFTS results revealed that SO 2 could induce more adsorbed NO x and NH 3 species instead of bulk sulfate, which also was responsible for good SO 2 resistance. © 2023 Society of Chemical Industry.
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