SiO2-CTAB复合材料的制备及其对PNP的吸附性能

doi:10.16085/j.issn.1000-6613.2022-2370

摘要/Abstract

摘要：

以黄磷炉渣为硅源，十六烷基三甲基溴化铵（CTAB）为负载剂，制备二氧化硅基复合吸附剂（SiO₂-CTAB）并研究其对废水中对硝基苯酚（PNP）的吸附性能。考察吸附过程中吸附温度、溶液pH、吸附剂投入量、PNP初始浓度和吸附时间对吸附效果的影响；探究吸附过程动力学、热力学及吸附剂再生性能并采用扫描电子显微镜、能量色散光谱仪、X射线光电子能谱、傅里叶变换红外光谱仪等手段对相关物质进行表征。结果表明：在实验研究范围内，最佳吸附条件为温度20℃、pH=6、吸附剂投入量1.5g/L。该条件下，对PNP最大吸附容量为157.2mg/g；对50mg/L的PNP模拟废水去除率可达96.95%。该吸附剂对PNP的吸附过程符合拟二级动力学模型，Langmuir吸附等温线模型能很好地描述该吸附行为。

关键词: 二氧化硅, 十六烷基三甲基溴化铵, 吸附材料, 对硝基苯酚, 黄磷炉渣

Abstract:

Using yellow phosphorus slag as silicon source and cetyltrimethyl ammonium bromide (CTAB) as a supporting agent, the SiO₂-based composite adsorbent (SiO₂-CTAB) was prepared and its adsorption performance for p-nitrophenol (PNP) in wastewater was studied. Effects of adsorption temperature, solution pH, adsorbent input, initial concentration of PNP and adsorption time on the adsorption performance were investigated. The adsorption kinetics, thermodynamics and adsorbent regeneration properties were analyzed, and the related substances were characterized by SEM, EDS, XPS, FTIR and other means. The results showed that the optimum adsorption conditions were temperature 20℃, pH=6 and the amount of adsorbent 1.5g/L. Under these conditions, the removal rate of 50mg/L PNP simulated wastewater can reach 96.95% and the maximum adsorption capacity of PNP was 157.2mg/g. The adsorption process of PNP by this adsorbent conformed to the pseudo-second-order kinetic model, and the Langmuir adsorption isotherm model can well describe the adsorption process.

Key words: silica, cetyltrimethyl ammonium bromide, adsorption material, p-nitrophenol, yellow phosphorus slag

中图分类号:

TQ424

田月, 董晓涵, 苏毅. SiO₂-CTAB复合材料的制备及其对PNP的吸附性能[J]. 化工进展, 2023, 42(11): 6064-6075.

TIAN Yue, DONG Xiaohan, SU Yi. Preparation of the SiO₂-CTAB composite material and its adsorption properties for PNP[J]. Chemical Industry and Engineering Progress, 2023, 42(11): 6064-6075.

图/表 23

参考文献 27

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项目	SiO₂	CaO	MgO	P₂O₅	Al₂O₃	Fe₂O₃	氟化物
黄磷炉渣	38.33	44.21	3.93	2.68	1.92	0.65	2.57
SiO₂基体	89.90	0.18	0.16	0.69	0.50	0.36	0.26

项目	SiO₂	CaO	MgO	P₂O₅	Al₂O₃	Fe₂O₃	氟化物
黄磷炉渣	38.33	44.21	3.93	2.68	1.92	0.65	2.57
SiO₂基体	89.90	0.18	0.16	0.69	0.50	0.36	0.26

模型	C₀/mg·L^-1	q_e,exp/mg·g^-1	q_e,cal/mg·g^-1	k₁/min^-1	R²
拟一级动力学	40	25.53	6.496	7.144×10^-2	0.8576
	60	37.86	11.69	6.134×10^-2	0.8338
	80	49.93	10.97	5.706×10^-2	0.8453

模型	C₀/mg·L^-1	q_e,exp/mg·g^-1	q_e,cal/mg·g^-1	k₁/min^-1	R²
拟一级动力学	40	25.53	6.496	7.144×10^-2	0.8576
	60	37.86	11.69	6.134×10^-2	0.8338
	80	49.93	10.97	5.706×10^-2	0.8453

模型	C₀/mg·L^-1	q_e,exp/mg·g^-1	q_e,cal/mg·g^-1	k₂/g·mg^-1·min^-1	R²
拟二级动力学	40	25.53	25.68	1.363×10^-1	0.9999
	60	37.86	38.17	5.872×10^-2	0.9999
	80	49.93	50.20	6.505×10^-2	0.9999

SiO₂-CTAB复合材料的制备及其对PNP的吸附性能

Preparation of the SiO₂-CTAB composite material and its adsorption properties for PNP

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模型	C₀/mg·L^-1	阶段	K_id/mg·g^-1·min^-0.5	N/mg·g^-1	R²
颗粒内扩散	40	1	9.484	9.938	0.9810
		2	2.984×10^-1	23.80	0.8565
	60	1	17.40	8.286	0.9901
		2	6.246×10^-1	34.18	0.8976
	80	1	18.07	19.10	0.9715
		2	4.974×10^-1	46.80	0.7797

T/℃	拟合方程	q_m/mg·g^-1	K_L/L·mg^-1	R_L	R²
20	y=0.0061x+0.1717	164.0	0.0355	0.0340~0.3602	0.9967
40	y=0.0071x+0.2158	140.9	0.0329	0.0366~0.3781	0.9997
80	y=0.0298x+1.6559	33.56	0.0180	0.0649~0.5264	0.9961

T/℃	拟合方程	K_F	1/a	R²
20	y=0.2792x+3.4273	30.80	0.2792	0.9520
40	y=0.3198x+3.0461	21.03	0.3198	0.8846
80	y=0.3176x+1.4819	4.401	0.3176	0.8535

T/K	K_T	ΔG^θ/J·mol^-1	ΔH^θ/J·mol^-1	ΔS^θ/J·mol^-1·K^-1
293	4.942×10³	-20.72×10³	-10.16×10³	36.63
313	4.577×10³	-21.93×10³
353	2.503×10³	-22.97×10³

样品	比表面积/m²·g^-1	V_t/cm³·g^-1	D_a/nm
SiO₂基体	519.2	0.7603	5.051
黄磷炉渣	1.307	6.683×10^-3	34.35

项目	C 1s		Si 2p	O 1s
项目	C—(C,H)	C—O—C	Si—O	O—Si
结合能/eV	284.74	286.26	103.39	532.84
质量分数/%	10.39	3.20	28.41	58.00

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项目	C 1s		Si 2p	O 1s		N 1s
项目	C—(C,H)	C—O—C	Si—O	O—Si	O—C	N—SiO₂	N—C
结合能/eV	284.74	286.36	102.76	532.11	530.59	402.46	399.24
质量分数/%	45.40	11.10	11.44	22.21	6.68	2.21	0.95

项目	C 1s		Si 2p	O 1s		N 1s
项目	C—(C,H)	C—O—C	Si—O	O—Si	O—C	N—SiO₂	N—C
结合能/eV	284.74	286.36	102.76	532.11	530.59	402.46	399.24
质量分数/%	45.40	11.10	11.44	22.21	6.68	2.21	0.95