基于響應曲面法制備鋼渣–花生殼基生態活性炭及其吸附性能研究

杜曉燕; 韓偉勝; 孟子涵; 于先坤; 楊曉軍; 張浩

doi:10.13374/j.issn2095-9389.2022.07.18.005

基于響應曲面法制備鋼渣–花生殼基生態活性炭及其吸附性能研究

doi: 10.13374/j.issn2095-9389.2022.07.18.005

杜曉燕^{1, 2},
韓偉勝¹,
孟子涵¹,
于先坤^{3, 4},
楊曉軍^{3, 4},
張浩^{1, 2, ,}

1.
安徽工業大學建筑工程學院，馬鞍山 243032
2.
冶金減排與資源綜合利用教育部重點實驗室（安徽工業大學），馬鞍山 243002
3.
金屬礦山安全與健康國家重點實驗室，馬鞍山 243000
4.
中鋼集團馬鞍山礦山研究院股份有限公司，馬鞍山 243000

基金項目: 中國博士后科學基金資助項目（2017M612051）；金屬礦山安全與健康國家重點實驗室開發基金資助項目（2020-JSKSSYS-01）；安徽省博士后研究人員科研活動經費資助項目（2019B336）；冶金工程與資源綜合利用安徽省重點實驗室（安徽工業大學）開放基金資助項目（SKF21-03）；馬鞍山市博士后研究人員科研活動經費資助項目（2020A11）

詳細信息

通訊作者:
E-mail: fengxu19821018@163.com

中圖分類號: X753
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出版歷程
- 收稿日期: 2022-07-18
- 網絡出版日期: 2022-09-14
- 刊出日期: 2023-05-31

Preparation of steel slag–peanut shell-based ecological activated carbon based on response surface method and its adsorption performance

DU Xiao-yan^{1, 2},
HAN Wei-sheng¹,
MENG Zi-han¹,
YU Xian-kun^{3, 4},
YANG Xiao-jun^{3, 4},
ZHANG Hao^{1, 2
, ,}

1.
School of Civil Engineering and Architecture, Anhui University of Technology, Ma’anshan 243032, China
2.
Key Laboratory of Metallurgical Emission Reduction & Resources Recycling (Anhui University of Technology), Ministry of Education, Ma’anshan 243002, China
3.
State Key Laboratory of Metal Mine Safety and Health, Ma’anshan 243000, China
4.
Sinosteel Ma’anshan Mining Research Institute Co., Ltd., Ma’anshan 243000, China

More Information

Corresponding author: E-mail: fengxu19821018@163.com

摘要

摘要: 以鋼渣超微粉和花生殼為原料制備鋼渣–花生殼基生態活性炭，基于響應曲面法研究微波功率、浸漬比、鋼渣摻量和鋼渣細度對鋼渣–花生殼基生態活性炭對甲醛氣體吸附率的影響，并對其進行優化處理。利用X-射線紅外光譜儀、場發射掃描電鏡、比表面積及孔徑測定儀等對鋼渣–花生殼基生態活性炭進行表征分析。結果表明：鋼渣–花生殼基生態活性炭最優制備參數為微波功率530 W，鋼渣細度1160目，鋼渣摻量(質量分數)10.8%，浸漬比1.25，其對甲醛氣體的吸附率為94.14%。影響鋼渣–花生殼基生態活性炭性能的因素次序依次為：微波功率、鋼渣摻量、浸漬比、鋼渣細度，其中微波功率與浸漬比、微波功率與鋼渣摻量、鋼渣摻量與鋼渣細度均存在顯著交互作用。適量鋼渣改性活性炭有利于形成規則的孔結構、提高表面酸性官能團含量以及增強表面極性。
- 鋼渣 /
- 花生殼 /
- 生態活性炭 /
- 甲醛 /
- 響應曲面法 /
- 優化
Abstract: Steel slag–peanut shell-based activated carbon was prepared using ultrafine steel slag powder and peanut shells through microwave processing. The response surface method was used to evaluate the effects of microwave power, impregnation ratio, steel slag content, and steel slag particle size on the rate of the adsorption of formaldehyde gas by the prepared activated carbon. Subsequently, optimum parameters were calculated for the preparation of activated carbon with the maximum rate of adsorption for formaldehyde gas adsorption. Finally, the activated carbon was characterized by an X-ray infrared spectrometer, field emission scanning electron microscope, and specific surface area and pore size analyzer. Results revealed that the activated carbon prepared using 530 W of microwave power, steel slag powder corresponding to a mesh size 1160, steel slag content equal to 10.8%, and impregnation ratio of 1.25 has the highest formaldehyde adsorption rate. According to the established regression model, the theoretical adsorption rate of formaldehyde gas will be 94.96% under the above optimal preparation conditions. Thus, the prepared activated carbon had a formaldehyde adsorption rate of 94.14%, which is within a 5% error range of the adsorption rate estimated by our regression model for the same conditions. We further demonstrated that our response curve model can predict the adsorption rate of the activated carbon prepared by this process efficiently and that it is feasible to optimize the preparation of activated carbon by the response surface method. Furthermore, the regression analysis further reveals that the degree of influence of the four factors related to this method of preparing activated carbon on the rate of formaldehyde gas adsorption is in the following order, from large to small: microwave power, steel slag content, impregnation ratio, and steel slag fineness. The mutual interaction of the four influencing factors on the formaldehyde gas adsorption rate can be intuitively observed through the three-dimensional response surface graph. Pore structure analysis of the activated carbon prepared using the optimal preparation conditions revealed that it has an H3-type hysteresis loop and a flat-panel slot-like structure. The pore size distribution is uneven, with predominant micropores and small-sized mesopores. Fourier-transform infrared spectroscopy analysis showed that after adding steel slag for modification, the activated carbon had more acidic functional groups, which is beneficial to the adsorption of formaldehyde. Morphological analysis reveals that the layered structure of the activated carbon is clear and that adding a small amount of steel slag is beneficial to improve the rate of pulverization.
- steel slag /
- peanut shell /
- ecological activated carbon /
- formaldehyde /
- response surface method /
- optimization

HTML全文

圖 1 各因素交互作用對甲醛氣體吸附率的響應面與等高線圖. (a)微波功率與浸漬比；(b)微波功率與鋼渣摻量；(c)鋼渣細度與鋼渣摻量

Figure 1. Response surface and the contour map of the interaction of various factors for the formaldehyde adsorption rate: (a) microwave power and impregnation ratio; (b) microwave power and steel slag mixing amount; (c) steel slag fineness and steel slag mixing amount

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圖 2 BET測試結果．生態活性炭的吸脫附等溫線(a)和孔徑分布(b)；最優鋼渣–花生殼基生態活性炭吸脫附等溫線(c)和孔徑分布(d)

Figure 2. BET test results: adsorption–desorption isotherm (a) and aperture distribution (b) of ecological activated carbon; adsorption–desorption isotherm (c) and aperture distribution (d) of optimal steel slag–peanut shell-based ecological activated carbon

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圖 3 生態活性炭的FTIR表征

Figure 3. FTIR characterization of the activated carbon

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圖 4 SEM測試結果。（a)生態活性炭；（b）最優鋼渣–花生殼生態活性炭

Figure 4. SEM micrographs: (a) ecological activated carbon; (b) optimal steel slag–peanut shell-based ecological activated carbon

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表 1 鋼渣超微粉的化學成分(質量分數)

Table 1. Chemical composition of steel slag ultrafine powder %

CaO	Fe₂O₃	SiO₂	MgO	P₂O₅	Al₂O₃	MnO	V₂O₅	TiO₂	Other
45.24	27.61	12.24	7.49	2.17	2.06	1.67	0.613	0.453	0.434

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表 2 實驗自變量因素及水平

Table 2. Factors and levels of the independent variables

No.	Factors
No.	Microwave power/W	Steel slag fineness (mesh)	Steel slag content/%	Impregnation ratio
?1	400	800	10	1.00
0	575	1000	15	1.25
1	700	1200	20	1.50

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表 3 Box–Behnken實驗設計結果

Table 3. Box–Behnken experiment design results

No.	Code				Adsorption rate of formaldehyde gas/%
No.	Microwave power/W	Steel slag fineness (mesh)	Steel slag content/%	Impregnation ratio/%	Adsorption rate of formaldehyde gas/%
1	400	1000	10	1.25	83.6
2	550	1000	10	1.00	88.4
3	400	1000	15	1.00	77.4
4	400	800	15	1.25	86.2
5	700	800	15	1.25	81.5
6	550	1000	10	1.50	86.1
7	550	1000	15	1.25	92.0
8	550	800	20	1.25	91.2
9	550	800	15	1.50	84.6
10	400	1000	15	1.50	80.4
11	550	1000	15	1.25	90.5
12	550	1200	20	1.25	82.3
13	550	1200	15	1.50	84.5
14	550	1200	10	1.25	92.5
15	400	1200	15	1.25	88.6
16	400	1000	20	1.25	81.3
17	550	1000	15	1.25	91.1
18	700	1000	15	1.50	64.2
19	550	1200	15	1.00	87.1
20	550	800	10	1.25	90.3
21	550	1000	20	1.50	78.4
22	700	1000	10	1.25	87.5
23	700	1200	15	1.25	78.5
24	550	800	15	1.00	91.9
25	550	1000	15	1.25	94.0
26	550	1000	20	1.00	85.1
27	700	1000	20	1.25	65.2
28	700	1000	15	1.00	77.3
29	550	1000	15	1.25	91.2

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表 4 方差分析表

Table 4. Analysis of variance

No.	Sum of squares	Degree of freedom	Square error	F	P
Model	1466.80	14	104.77	20.72	<0.0001
A	156.24	1	156.24	30.90	<0.0001
B	14.52	1	14.52	2.87	0.1122
C	160.60	1	160.60	31.77	<0.0001
D	70.08	1	70.08	13.86	0.0023
AB	7.29	1	7.29	1.44	0.2497
AC	100	1	100	19.78	0.0006
AD	64.80	1	64.80	12.82	0.0030
BC	36.60	1	36.60	7.24	0.0176
BD	5.52	1	5.52	1.09	0.3137
CD	4.84	1	4.84	0.96	0.3445
A²	654.72	1	654.72	129.50	<0.0001
B²	6.69	1	6.69	1.32	0.2692
C²	37.26	1	37.26	7.37	0.0168
D²	220.78	1	230.78	43.67	<0.0001
Residual	70.78	14	5.06	—	—
Lack of fit	63.37	10	6.34	3.42	0.1237
Errors	7.41	4	1.85	—	—
Deviation	1537.58	28	—	—	—

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表 5 回歸方程的R²和標準差分析

Table 5. R² and standard deviation analysis of the regression equations

Std. Dev.	Mean	C.V./%	Press	R²	Adj R²	Pred R²	Adeq precision
2.25	84.62	2.66	373.57	0.9540	0.9079	0.7551	18.634

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表 6 孔結構測試結果

Table 6. Results of the hole structure test

Sample	BET/(m²·g^–1)	S_micro/(m²·g^–1)	V_total/(cm³·g^–1)	V_micro/(cm³·g^–1)	D_aver/nm
Ecological activated carbon	1008.68	360.96	0.622	0.195	2.46
Optimal steel slag–peanut shell-based ecological activated carbon	397.96	143.98	0.331	0.074	3.33
Note: BET is surface area; S_micro is surface area of micropore; V_total is total pore volume; V_micro is pore volume of micropore; D_aver is mean pore size.

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