磷化处理催化剂 CeSnOx 在 NH3-SCR 脱氮氧化物反应中具有优异的低温活性和抗 K 中毒性能

Ziting Wang, Mihang Yao, Xiaoyu Niu, Yujun Zhu
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摘要

抗碱金属中毒仍然是铈基脱硝(脱氮)催化剂面临的一项挑战。本文通过对 CeSnO 进行磷酸化处理,提高了其低温性能和抗 K 中毒能力。活性测试表明,即使在 K 中毒后,磷酸化 CeSnO(3 wt%P/CeSn)在 190-450 ℃ 时的 NO 转化率超过 90%,在 240-400 ℃ 时的 NO 转化率大于 90%。通过多种表征和 DFT 计算研究了磷酸化处理 K 中毒的机理。结果表明,磷化处理促进了 Ce 和 Sn 之间的相互作用,而 K 更倾向于与 PO 物种相互作用。这防止了 K 破坏 Ce-O-Sn 结构,形成 Ce-O-K 结构,从而保持了催化剂的氧化还原特性。此外,与 CeSnO 相比,磷化处理补充了 3 wt%P/CeSn 的酸性。这有效缓解了 K 导致的酸度降低,确保了催化剂表面对 NH 的吸附和活化。
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Excellent low-temperature activity and resistance to K-poisoning in NH3-SCR de-NOx reaction over CeSnOx with phosphorylation treatment catalyst
Resistance to alkali metal poisoning remains a challenge for Ce-based denitration (de-NO) catalysts. In this paper, improved low-temperature performance and resistance to K poisoning were achieved by phosphorylating CeSnO. The activity tests revealed that the phosphorylated CeSnO (3 wt%P/CeSn) exhibited over 90 % NO conversion at 190–450 °C and >90 % NO conversion at 240–400 °C even after K poisoning. The mechanism of phosphorylation treatment against K poisoning was investigated by many characterizations and DFT calculation. The results showed that the phosphorylation treatment facilitated the interaction between Ce and Sn, and K interacts more preferentially with PO species. This prevents K from destroying the Ce-O-Sn structure to form a Ce-O-K structure, which in turn maintained the catalyst’s redox properties. Moreover, the phosphorylation treatment supplemented the acidity of 3 wt%P/CeSn compared with CeSnO. This effectively mitigated the reduction of acidity caused by K and ensured the adsorption and activation of NH on the catalyst surface.
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