铜物种对Cu/Fe<sub>2</sub>O<sub>3</sub>水煤气变换反应催化剂性能的影响

引用本文: 林性贻, 马俊涛, 陈崇启, 詹瑛瑛, 郑起. 铜物种对Cu/Fe₂O₃水煤气变换反应催化剂性能的影响[J]. 物理化学学报, 2014, 30(1): 157-163. doi: 10.3866/PKU.WHXB201311271 shu

Citation: LIN Xing-Yi, MA Jun-Tao, CHEN Chong-Qi, ZHAN Ying-Ying, ZHENG Qi. Influence of Copper Species on Performance of Cu/Fe₂O₃ Catalysts for Water Gas Shift Reaction[J]. Acta Physico-Chimica Sinica, 2014, 30(1): 157-163. doi: 10.3866/PKU.WHXB201311271 shu

铜物种对Cu/Fe₂O₃水煤气变换反应催化剂性能的影响

基金项目:
福建省教育厅A类科技项目(JA08021) (JA08021)

摘要:

采用共沉淀法制备了系列铜负载量不同的Cu/Fe₂O₃水煤气变换(WGS)催化剂，并考察了铜负载量对催化剂结构和水煤气变换反应性能的影响. 结果表明，Cu/Fe₂O₃催化剂呈现出良好的水煤气反应性能，当CuO质量分数为20%时，催化剂的WGS性能最优，250 ℃时CO转化率高达97.2%，同时热稳定性也最好. 运用X射线粉末衍射(XRD)、N₂物理吸脱附和H₂程序升温还原(H₂-TPR)等手段对Cu/Fe₂O₃催化剂的物相、织构特征及还原性能进行了表征，结果表明，CuFe₂O₄物种的存在极大地改善了催化剂的还原性能和WGS反应活性. 这是由于CuFe₂O₄特殊的尖晶石结构有利于Cu微晶的稳定；同时，CuFe₂O₄在低温下即被还原为单质铜，有利于促进催化剂体系中电子的转移. 此外，通过(NH₄)₂CO₃溶液处理，研究了独立相CuO对Cu/Fe₂O₃催化剂WGS反应性能的影响，结果发现，独立相CuO的存在，有利于H原子在各组分传递，从而促进催化剂的CuFe₂O₄的还原，改善Cu/Fe₂O₃催化剂的WGS反应性能.

关键词:

English

Influence of Copper Species on Performance of Cu/Fe₂O₃ Catalysts for Water Gas Shift Reaction

1.
National Engineering Research Center of Chemical Fertilizer Catalyst, Fuzhou University, Fuzhou 350002, P. R. China
Received Date: 02 September 2013
Available Online: 01 January 2014
Fund Project:
福建省教育厅A类科技项目(JA08021)

Abstract:

A series of Cu/Fe₂O₃ catalysts with different Cu loadings were prepared using a co-precipitation method, and the relationship between their structures and catalytic activities for the water gas shift (WGS) reaction was carefully examined. It was found that the as-prepared Cu/Fe₂O₃ catalysts exhibit excellent WGS performances, in particular, the one containing 20% (w) CuO (CF-20) shows the best catalytic activity, with CO conversion of 97.2% at 250 ℃. Its catalytic stability is also outstanding during the temperature range of 250-400 ℃. X-ray diffraction (XRD), N₂ physisorption, and H₂ temperature program reduction (H₂-TPR) techniques were used to characterize the crystal phases, textures, and reduction properties of the Cu/Fe₂O₃ catalysts. The results show that the generation of CuFe₂O₄, which has a spinel structure in stabilizing Cu microcrystals and is easier to be reduced at low temperature, resulting in enhancing their reduction properties and facilitating electrons transfer between Cu and Fe₂O₃, thus greatly improving the catalytic performance. Furthermore, (NH₄)₂CO₃ solution treatment of the as-prepared catalysts was performed to study the effect of bulk CuO existed in the Cu/Fe₂O₃ catalysts. The result suggests that the bulk CuO is favor for H atom transfer between Cu and Fe₂O₃, thus promoting the reduction of CuFe₂O₄, finally improving the catalytic performance.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

铜物种对Cu/Fe₂O₃水煤气变换反应催化剂性能的影响

English

Influence of Copper Species on Performance of Cu/Fe₂O₃ Catalysts for Water Gas Shift Reaction

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

铜物种对Cu/Fe2O3水煤气变换反应催化剂性能的影响

English

Influence of Copper Species on Performance of Cu/Fe2O3 Catalysts for Water Gas Shift Reaction

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

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CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

铜物种对Cu/Fe₂O₃水煤气变换反应催化剂性能的影响

Influence of Copper Species on Performance of Cu/Fe₂O₃ Catalysts for Water Gas Shift Reaction

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs