化工进展 ›› 2022, Vol. 41 ›› Issue (8): 4213-4223.DOI: 10.16085/j.issn.1000-6613.2021-1977
张嘉琪1,2(), 林丽娜1,2, 高文桂1,2,3(), 祝星2,3
收稿日期:
2021-09-06
修回日期:
2021-11-18
出版日期:
2022-08-25
发布日期:
2022-08-22
通讯作者:
高文桂
作者简介:
张嘉琪(1997—),女,硕士研究生,研究方向为能源催化。E-mail:基金资助:
ZHANG Jiaqi1,2(), LIN Lina1,2, GAO Wengui1,2,3(), ZHU Xing2,3
Received:
2021-09-06
Revised:
2021-11-18
Online:
2022-08-25
Published:
2022-08-22
Contact:
GAO Wengui
摘要:
采用水热法制备CeO2纳米颗粒(W-CeO2)、CeO2纳米片(S-CeO2)、CeO2纳米棒(B-CeO2)及CeO2纳米八面体(O-CeO2),用浸渍法负载相同质量分数的铜形成CuO/CeO2催化剂。通过扫描电镜(SEM)、高分辨透射电子显微镜(TEM)、X射线衍射(XRD)、拉曼光谱(Raman)、自动吸附分析仪(BET)、H2程序升温还原(H2-TPR)、N2O滴定等表征技术对催化剂进行表征,并在可控温控压的固定床石英管反应器中对催化剂的催化性能进行评价。研究了不同形貌CuO/CeO2催化剂对CO2加氢制备甲醇的影响;结果表明,CuO/CeO2催化剂的催化活性存在明显的形貌依赖性,催化剂的暴露晶面、比表面积、表面碱性位点、表面氧缺陷的差异均会对CO2转化率、甲醇选择性和产率产生影响。其中,不同形貌CeO2优先暴露晶面的活性顺序为S-CeO2({100}+{110})>W-CeO2{100}>B-CeO2{111}≈O-CeO2{111},暴露晶面活性越高,催化剂表面氧缺陷越多,CuO-CeO2间相互作用越强,则催化活性越好。当为CuO/S-CeO2时,催化剂表面中碱性位点最多,催化剂比表面积为88.8m2/g,铜分散度为19.2%,CO2转化率为6.56%,甲醇选择性和收率为96.3%和0.063g/(gcat·h),催化活性最好,由活性评价试验得转化率由高到低依次为S-CeO2>B-CeO2>W-CeO2>O-CeO2,可知CeO2形貌差异会决定CuO/CeO2催化剂的物化性能和催化活性,从而提升对不同形貌CuO/CeO2催化剂催化CO2加氢制甲醇的基础认识。
中图分类号:
张嘉琪, 林丽娜, 高文桂, 祝星. CeO2的形貌对CuO/CeO2催化剂CO2加氢制甲醇性能的影响[J]. 化工进展, 2022, 41(8): 4213-4223.
ZHANG Jiaqi, LIN Lina, GAO Wengui, ZHU Xing. Effect of CeO2 morphology on the performance of CuO/CeO2 catalyst for CO2 hydrogenation to methanol[J]. Chemical Industry and Engineering Progress, 2022, 41(8): 4213-4223.
CeO2载体 | SBET/m2·g-1 | ID/IF2g | CuO/CeO2催化剂 | SBET/m2·g-1 | ID/IF2g |
---|---|---|---|---|---|
W-CeO2 | 66.9 | 0.035 | CuO/W-CeO2 | 76.4 | 0.126 |
S-CeO2 | 79.2 | 0.056 | CuO/S-CeO2 | 88.8 | 0.284 |
B-CeO2 | 114.1 | 0.048 | CuO/B-CeO2 | 122.2 | 0.154 |
O-CeO2 | 35.8 | 0.026 | CuO/O-CeO2 | 43.5 | 0.067 |
表1 载体及催化剂的比表面积、氧空位浓度比
CeO2载体 | SBET/m2·g-1 | ID/IF2g | CuO/CeO2催化剂 | SBET/m2·g-1 | ID/IF2g |
---|---|---|---|---|---|
W-CeO2 | 66.9 | 0.035 | CuO/W-CeO2 | 76.4 | 0.126 |
S-CeO2 | 79.2 | 0.056 | CuO/S-CeO2 | 88.8 | 0.284 |
B-CeO2 | 114.1 | 0.048 | CuO/B-CeO2 | 122.2 | 0.154 |
O-CeO2 | 35.8 | 0.026 | CuO/O-CeO2 | 43.5 | 0.067 |
催化剂 | α | β | ||||
---|---|---|---|---|---|---|
面积/mV·℃ | Tmax/℃ | 面积/mV·℃ | Tmax/℃ | |||
CuO/W-CeO2 | 5200 | 323 | 16820 | 390 | 0.236 | |
CuO/S-CeO2 | 3200 | 311 | 10256 | 358 | 0.238 | |
CuO/B-CeO2 | 5395 | 428 | 18202 | 470 | 0.229 | |
CuO/O-CeO2 | 3143 | 312 | 11824 | 372 | 0.210 |
表2 不同温度下催化剂H2-TPR还原峰数据
催化剂 | α | β | ||||
---|---|---|---|---|---|---|
面积/mV·℃ | Tmax/℃ | 面积/mV·℃ | Tmax/℃ | |||
CuO/W-CeO2 | 5200 | 323 | 16820 | 390 | 0.236 | |
CuO/S-CeO2 | 3200 | 311 | 10256 | 358 | 0.238 | |
CuO/B-CeO2 | 5395 | 428 | 18202 | 470 | 0.229 | |
CuO/O-CeO2 | 3143 | 312 | 11824 | 372 | 0.210 |
催化剂 | 弱碱性位点 | 中碱性位点 | 强碱性位点 | 总位点 |
---|---|---|---|---|
CuO/W-CeO2 | 1220 | 902 | 30 | 2152 |
CuO/S-CeO2 | 1126 | 1835 | 35 | 2996 |
CuO/B-CeO2 | 250 | 986 | 11 | 1247 |
CuO/O-CeO2 | 55 | 579 | 24 | 658 |
表3 不同形貌CuO/CeO2催化剂碱性位点分布表
催化剂 | 弱碱性位点 | 中碱性位点 | 强碱性位点 | 总位点 |
---|---|---|---|---|
CuO/W-CeO2 | 1220 | 902 | 30 | 2152 |
CuO/S-CeO2 | 1126 | 1835 | 35 | 2996 |
CuO/B-CeO2 | 250 | 986 | 11 | 1247 |
CuO/O-CeO2 | 55 | 579 | 24 | 658 |
催化剂 | SCO/% | DCu/% | |||
---|---|---|---|---|---|
CuO/W-CeO2 | 5.47 | 99.04 | 0.96 | 5.42 | 15.8 |
CuO/S-CeO2 | 8.56 | 96.30 | 3.70 | 8.24 | 19.2 |
CuO/B-CeO2 | 6.01 | 98.09 | 1.91 | 5.90 | 17.4 |
CuO/O-CeO2 | 3.97 | 99.99 | 0.01 | 3.97 | 11.9 |
表4 不同形貌CuO/CeO2催化剂的CO2催化评价表
催化剂 | SCO/% | DCu/% | |||
---|---|---|---|---|---|
CuO/W-CeO2 | 5.47 | 99.04 | 0.96 | 5.42 | 15.8 |
CuO/S-CeO2 | 8.56 | 96.30 | 3.70 | 8.24 | 19.2 |
CuO/B-CeO2 | 6.01 | 98.09 | 1.91 | 5.90 | 17.4 |
CuO/O-CeO2 | 3.97 | 99.99 | 0.01 | 3.97 | 11.9 |
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