化工学报 ›› 2020, Vol. 71 ›› Issue (4): 1646-1656.DOI: 10.11949/0438-1157.20191050
焦昭杰1(),陈立功1,柳云骐2,张贤明1,龚海峰1,高旭3()
收稿日期:
2019-09-23
修回日期:
2019-12-09
出版日期:
2020-04-05
发布日期:
2020-04-05
通讯作者:
高旭
作者简介:
焦昭杰(1981—),男,博士,助理研究员,基金资助:
Zhaojie JIAO1(),Ligong CHEN1,Yunqi LIU2,Xianming ZHANG1,Haifeng GONG1,Xu GAO3()
Received:
2019-09-23
Revised:
2019-12-09
Online:
2020-04-05
Published:
2020-04-05
Contact:
Xu GAO
摘要:
为解决Fenton法存在活性组分流失及通常在pH 2~3条件下运行的局限性,采用柠檬酸络合法制备了CuCe氧化物催化剂,建立了双酚A非均相催化湿式过氧化氢氧化(CWPO)反应体系。考察了焙烧温度、Cu/Ce摩尔比、H2O2用量、双酚A初始浓度和pH对催化剂物化结构和CWPO性能的影响。并分析了可能的降解路径。结果表明:催化剂具有良好的高温稳定性和pH适应性,在pH 1.6~7.9范围内对双酚A都具有较高的降解性能,不需要调节pH。在焙烧温度450℃、Cu/Ce摩尔比1.0、催化剂用量1 g·L-1、H2O2用量196 mmol·L-1、BPA浓度152 mg·L-1、pH 6.6、反应温度75℃、反应95 min后,BPA和TOC去除率分别为91.8%和84.5%,Cu2+析出浓度为19.3 mg·L-1。推测了双酚A可能的降解路径。
中图分类号:
焦昭杰, 陈立功, 柳云骐, 张贤明, 龚海峰, 高旭. CuCe氧化物催化剂的制备及CWPO降解双酚A废水研究[J]. 化工学报, 2020, 71(4): 1646-1656.
Zhaojie JIAO, Ligong CHEN, Yunqi LIU, Xianming ZHANG, Haifeng GONG, Xu GAO. Preparation of CuCe oxide catalyst for CWPO degradation of bisphenol A[J]. CIESC Journal, 2020, 71(4): 1646-1656.
CuCe 催化剂 | 结晶度①/% | 平均晶粒尺寸/nm | 晶胞参数 | ||
---|---|---|---|---|---|
a (α=90°)/? | b (β=90°)/? | c (γ=90°)/? | |||
CC450 | 42.55 | 8.0 | 5.4045 | 5.4001 | 5.3241 |
CC550 | 45.43 | 9.6 | 5.4054 | 5.4219 | 5.4065 |
CC650 | 62.17 | 17.9 | 5.4032 | 5.4111 | 5.4071 |
CC750 | 63.14 | 32.5 | 5.4095 | 5.4096 | 5.4096 |
Cu2Ce1 | 63.81 | 20.7 | 5.3988 | 5.4100 | 5.4003 |
Cu1Ce2 | 56.57 | 15.8 | 5.4031 | 5.4167 | 5.4085 |
Cu1Ce3 | 52.58 | 12.5 | 5.4097 | 5.4133 | 5.4081 |
表1 制得的CuCe氧化物催化剂参数
Table 1 Parameters of CuCe oxide catalysts
CuCe 催化剂 | 结晶度①/% | 平均晶粒尺寸/nm | 晶胞参数 | ||
---|---|---|---|---|---|
a (α=90°)/? | b (β=90°)/? | c (γ=90°)/? | |||
CC450 | 42.55 | 8.0 | 5.4045 | 5.4001 | 5.3241 |
CC550 | 45.43 | 9.6 | 5.4054 | 5.4219 | 5.4065 |
CC650 | 62.17 | 17.9 | 5.4032 | 5.4111 | 5.4071 |
CC750 | 63.14 | 32.5 | 5.4095 | 5.4096 | 5.4096 |
Cu2Ce1 | 63.81 | 20.7 | 5.3988 | 5.4100 | 5.4003 |
Cu1Ce2 | 56.57 | 15.8 | 5.4031 | 5.4167 | 5.4085 |
Cu1Ce3 | 52.58 | 12.5 | 5.4097 | 5.4133 | 5.4081 |
CuCe催化剂 | 晶格氧/% | 吸附氧/% | 羟基氧/% | Ce/%(质量分数) | Cu/%(质量分数) | O/%(质量分数) |
---|---|---|---|---|---|---|
Cu1Ce3 | 62.71 | 28.04 | 9.25 | 23.68 | 8.92 | 67.39 |
Cu1Ce2 | 69.16 | 18.07 | 12.77 | 25.22 | 8.49 | 66.30 |
Cu2Ce1 | 64.10 | 22.75 | 13.14 | 2.44 | 18.90 | 78.67 |
CC450 | 68.32 | 20.00 | 11.69 | 23.54 | 12.02 | 64.44 |
CC550 | 66.44 | 20.56 | 13.00 | 21.62 | 12.83 | 65.55 |
CC650 | 65.49 | 20.38 | 14.13 | 19.75 | 13.95 | 66.31 |
CC750 | 68.73 | 18.47 | 12.80 | 19.78 | 14.14 | 66.08 |
表2 制备的CuCe氧化物催化剂XPS参数
Table 2 XPS parameters of CuCe oxide catalysts
CuCe催化剂 | 晶格氧/% | 吸附氧/% | 羟基氧/% | Ce/%(质量分数) | Cu/%(质量分数) | O/%(质量分数) |
---|---|---|---|---|---|---|
Cu1Ce3 | 62.71 | 28.04 | 9.25 | 23.68 | 8.92 | 67.39 |
Cu1Ce2 | 69.16 | 18.07 | 12.77 | 25.22 | 8.49 | 66.30 |
Cu2Ce1 | 64.10 | 22.75 | 13.14 | 2.44 | 18.90 | 78.67 |
CC450 | 68.32 | 20.00 | 11.69 | 23.54 | 12.02 | 64.44 |
CC550 | 66.44 | 20.56 | 13.00 | 21.62 | 12.83 | 65.55 |
CC650 | 65.49 | 20.38 | 14.13 | 19.75 | 13.95 | 66.31 |
CC750 | 68.73 | 18.47 | 12.80 | 19.78 | 14.14 | 66.08 |
图5 制备条件对CWPO性能的影响
Fig.5 Effects of preparations on heterogeneous CWPO performance of bisphenol A (催化剂=1 g·L-1, BPA=152 mg·L-1, H2O2=196 mmol·L-1, pH=6.6, t=95 min, T=75℃)
Compound | Molecular weight | Tentative structure |
---|---|---|
benzaldehyde, 4-ethyl- | 134 | |
p-benzoquinone | 108 | |
phenol | 94 | |
styrene | 104 | |
p-isopropenylphenol | 134 | |
p-xylene | 106 | |
p-hydroxytoluene | 108 | |
o-cresol | 108 | |
phenol,-2,4-bis(1,1-dimethylethyl)- | 206 | |
phenol, 2,5-bis(1,1-dimethylethyl)- | 206 |
表3 BPA降解过程中可能的主要中间产物
Table 3 Possible major intermediates in BPA degradation process
Compound | Molecular weight | Tentative structure |
---|---|---|
benzaldehyde, 4-ethyl- | 134 | |
p-benzoquinone | 108 | |
phenol | 94 | |
styrene | 104 | |
p-isopropenylphenol | 134 | |
p-xylene | 106 | |
p-hydroxytoluene | 108 | |
o-cresol | 108 | |
phenol,-2,4-bis(1,1-dimethylethyl)- | 206 | |
phenol, 2,5-bis(1,1-dimethylethyl)- | 206 |
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