Catalytic decomposition of N2O over potassium-modified Cu-Co spinel oxides
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摘要: 制备了几个不同组成的Cu-Co尖晶石型复合氧化物,用于N2O分解反应,在活性较高的Cu0.8Co0.2Co2O4表面浸渍碱金属盐溶液,制备改性催化剂,考察了碱金属助剂类型、钾前驱物和钾负载量等对改性催化剂活性的影响。用BET、XRD、SEM、XPS等方法表征了催化剂结构。结果表明,几种碱金属碳酸盐改性Cu0.8Co0.2Co2O4的催化活性发生了显著变化,其中,K改性催化剂的活性有明显提高,而Cs的表面改性反而降低了催化剂活性;钾前驱物对K/Cu-Co的催化活性也有较大影响,其中,加入碳酸钾明显提高了催化剂的活性,而加入硝酸钾和醋酸钾反而降低了催化剂活性;有氧无水、有氧有水气氛中,400 SymbolpB@C下N2O在碳酸钾改性催化剂0.05K/Cu0.8Co0.2Co2O4上的转化率分别达到了100%和87.6%;该催化剂在400 SymbolpB@C下的恒温反应活性和稳定性均高于未改性催化剂。
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关键词:
- N2O催化分解 /
- Cu-Co复合氧化物 /
- 助剂钾 /
- 催化活性
Abstract: Cu-Co spinel oxides with different compositions were prepared for N2O catalytic decomposition in the presence of oxygen. The active catalyst of Cu0.8Co0.2Co2O4 was incipiently impregnated by alkali metal salt solutions to prepare the modified catalysts. These catalysts were characterized by BET, XRD, SEM and XPS techniques, and their catalytic activity for N2O decomposition was tested. The effect of alkali metal species, potassium precursors and potassium loadings on catalytic activity was investigated. It was found that the catalytic activity of Cu0.8Co0.2Co2O4 modified by K2CO3 was much higher than that of bare oxide, while Cs/Cu0.8Co0.2Co2O4 was inferior to Cu0.8Co0.2Co2O4 for N2O decomposition. In the case of K/Cu0.8Co0.2Co2O4 with different potassium precursors, the catalyst activity was largely enhanced by the addition of K2CO3, while the doping of KNO3 and CH3COOK notably depressed the catalytic activity. Over the optimal catalyst of 0.05K/Cu0.8Co0.2Co2O4, 100% and 87.6% conversion of N2O was reached at 400 SymbolpB@ C under the atmosphere of oxygen only and oxygen-steam together, respectively. In addition, K2CO3-modified catalyst in both reaction atmospheres showed higher stability than un-modified catalyst. -
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