高孔隙率生物炭研制及其处理废水中磷酸盐

李佳璇; 王平; 万斯; 陈润华

高孔隙率生物炭研制及其处理废水中磷酸盐

李佳璇¹,
王平^1,,
万斯²,
陈润华^1, ,

1.
中南林业科技大学环境科学与工程学院，长沙 410007
2.
湖南有色金属研究院有限责任公司，长沙 410100

基金项目: 湖南省自然科学基金重大项目(2021JC0001)；湖南省自然科学基金面上项目(2022JJ31014)；湖南省科技创新引领计划项目(2021GK4059，2020SK2006)；湖南省环保厅环保科研项目(HBKT-2022010)；湖南省教育厅科学研究项目(22A0193)

详细信息

作者简介:
王平，博士，教授，博士生导师，研究方向为水土污染控制　E-mail：csfuwp@163.com

通讯作者:
陈润华，博士，副教授，硕士生导师，研究方向为功能材料的研发与应用　E-mail：chen12@csuft.edu.cn

中图分类号: X703
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- 被引次数: 0
出版历程
- 收稿日期: 2022-11-30
- 修回日期: 2023-01-04
- 录用日期: 2023-01-08
- 网络出版日期: 2023-02-06

High porosity biochar and its treatment of phosphate in wastewater

Jiaxuan LI¹,
Ping WANG^1
,,
Si WAN²,
Runhua CHEN^{1
, ,}

1.
College of Environmental Science and Engineering, Central South University of Forestry and Technology, Changsha 410007, China
2.
Hunan Research Institute for Nonferrous Metals Co., Ltd., Changsha 410100, China

Funds: Major program Natural Science Foundation of Hunan Province of China (2021JC0001); the Natural Science Foundation of Hunan Province (2022JJ31014); the Hunan Provincial Key Research Plan Program of China (2021GK4059, 2020SK2006); Environmental Research Project of Hunan Environmental Protection Department (HBKT-2022010); Hunan Provincial Education Department Scientific Research Project (22A0193)

摘要

摘要: 生物炭是缺氧状态下生物质热解的产物；然而，常见的生物炭却表面积小、孔隙结构不发达、表面活性基团少，去除效果差。本文以高粱(GC)和柚子皮(YC)为原料，利用四种物质进行表面处理制备得到生物炭，其中制备的高粱/KOH(GC-KH)和柚子皮/KOH(YC-K)粉末表面孔状明显，证实了该工艺的可行性。GC-KH比表面积为2,096.05 m²/g，平均孔径4.12 nm，在其表面含有丰富的含氧官能团，为吸附提供了良好的结构空间和活性位点。通过批量实验，探讨了投加量、初始pH、接触时间、初始浓度等对磷酸盐吸附的影响，评估了离子强度。等温线结果表明，Langmuir模型可以很好地描述平衡数据，在pH值为7时GC-KH对磷酸盐最大吸附能力为74.73 mg/g，具有反应迅速等显著优势，为废水中磷酸盐的高效去除提供了创新路径。
- 生物炭 /
- 比表面积 /
- 磷酸盐 /
- 改性材料 /
- 吸附
Abstract: Biochar is a product of pyrolysis of biomass under anoxic conditions, but the common biochar has a small specific surface area, underdeveloped pore structure, few surface active groups and poor removal effect. In this paper, biochar was prepared from sorghum (GC) and grapefruit peel (YC) by surface treatment using four substances to obtain biochar, where the prepared sorghum/KOH (GC-KH) and grapefruit peel/KOH (YC-K) powders had obvious surface porosity, confirming the feasibility of the process. With a specific surface area of 2,096.05 m²/g and an average pore size of 4.12 nm, GC-KH is rich in oxygen-containing functional groups on its surface, providing a good structural space and active sites for adsorption. The effect of dosing volume, initial pH, contact time and initial concentration on phosphate adsorption was investigated in batch experiments to assess the ionic strength. The isotherm results show that the Langmuir model can describe the equilibrium data well, and the maximum adsorption capacity of GC-KH for phosphate at pH 7 is 74.73 mg/g, which has significant advantages such as rapid response and provides an innovative pathway for efficient removal of phosphate from wastewater.
- biochar /
- specific surface /
- phosphate /
- modified materials /
- adsorption

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图 1 高粱(GC)和柚子皮(YC)粉末制备生物炭的工艺流程图

Figure 1. Process flow diagram for the preparation of biochar from sorghum (GC) and grapefruit peel (YC) powder

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图 2 (a，b)为不同倍数下高粱粉末的扫描电镜图像；(c，d)为不同倍数下高GC-H的扫描电镜图像；(e，f)为不同倍数下GC-S的扫描电镜图像

Figure 2. (a, b) Scanning electron microscopy images of sorghum powder at different magnifications; (c, d) Scanning electron microscopy images of high GC-H at different magnifications; (e, f) Scanning electron microscopy images of GC-S at different magnifications

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图 3 (a，b，c)分别为高粱粉末、GC-H和GC-S的孔径分布图；(e，f，g)分别为高粱粉末、GC-H和GC-S的N₂吸附脱附等温线

Figure 3. (a, b, c) Pore size distribution of sorghum powder, GC-H and GC-S, respectively; (e, f, g) N₂ adsorption and desorption isotherms of sorghum powder, GC-H and GC-S, respectively

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图 4 (a, b)为不同倍数下GC-Na高粱粉末的扫描电镜图像；(c, d)为不同倍数下高GC-KC的扫描电镜图像；(e, f)为不同倍数下GC-KO的扫描电镜图像；(g, h)为不同倍数下GC-KH高粱粉末的扫描电镜图像

Figure 4. (a, b) Scanning electron microscopy images of GC-Na sorghum powder at different magnifications; (c, d) Scanning electron microscopy images of high GC-KC at different magnifications; (e, f) Scanning electron microscopy images of GC-KO at different magnifications; (g, h) Scanning electron microscopy images of GC-KH sorghum powder at different magnifications

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图 5 (a, b, c, d)分别为GC-Na、GC-KC、GC-KO和GC-KH的孔径分布图；(e, f, g, h)分别为GC-Na、GC-KC、GC-KO和GC-KH的N₂吸附脱附等温线

Figure 5. (a, b, c, d) Pore size distribution of GC-Na, GC-KC, GC-KO and GC-KH respectively; (e, f, g, h) N₂ adsorption and desorption isotherms of GC-Na, GC-KC, GC-KO and GC-KH respectively

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图 6 高粱粉末、GC-S和GC-KH的傅里叶变换红外光谱图像

Figure 6. FTIR images of sorghum powder, GC-S and GC-KH

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图 7 (a, b)为不同倍数下柚子皮粉末的扫描电镜图像；(c, d)为不同倍数下高YC的扫描电镜图像；(e, f)为不同倍数下YC-K的扫描电镜图像

Figure 7. (a, b) Scanning electron microscope images of grapefruit peel powder at different magnifications; (c, d) Scanning electron microscope images of high YC at different magnifications; (e, f) Scanning electron microscope images of YC-K at different magnifications

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图 8 (a, b, c)分别为柚子皮粉末、YC和YC-K的孔径分布图；(e, f, g)分别为柚子皮粉末、YC和YC-K的N₂吸附脱附等温线

Figure 8. (a, b, c) Pore size distribution of grapefruit peel powder, YC and YC-K, respectively; (e, f, g) N₂ adsorption and desorption isotherms of grapefruit peel powder, YC and YC-K, respectively

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图 9 (a) GC-KH投加量对吸附磷酸盐效果的影响；(b) pH对GC-KH吸附磷酸盐效果的影响；(c) 共存离子对GC-KH吸附磷酸盐效果的影响；(d)不同温度下反应时间对GC-KH吸附磷酸盐效果的影响；(e)不同温度下初始浓度对GC-KH吸附磷酸盐效果的影响；

Figure 9. (a) Effect of GC-KH dosage on the effect of phosphate adsorption; (b) Effect of pH on the effect of phosphate adsorption by GC-KH; (c) Effect of coexisting ions on the effect of phosphate adsorption by GC-KH; (d) Effect of reaction time at different temperatures on the effect of phosphate adsorption by GC-KH; (e) Effect of initial concentration at different temperatures on the effect of phosphate adsorption by GC-KH.

q_t is the amount adsorbed at time t; q_e is the amount adsorbed when adsorption equilibrium is reached; C_e is the concentration of pollutant in the solution after removal

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图 10 (a) GC-KH吸附磷酸盐的伪一阶动力学模型；(b) GC-KH吸附磷酸盐的伪二阶动力学模型；(c) 不同温度下GC-KH吸附磷酸盐的Langmuir模型和Freundlich模型；(d) 不同温度下GC-KH吸附磷酸盐的D-R模型；(f) 不同温度下GC-KH吸附磷酸盐的热力学；

Figure 10. (a) Pseudo-first-order kinetic model for phosphate adsorption by GC-KH; (b) Pseudo-second-order kinetic model for phosphate adsorption by GC-KH; (c) Langmuir and Freundlich models for phosphate adsorption by GC-KH at different temperatures; (d) D-R model for phosphate adsorption by GC-KH at different temperatures; (f) Thermodynamics of phosphate adsorption by GC-KH at different temperatures

θ is the isotherm constant; T is the absolute temperature; Kd is the thermodynamic equilibrium constant

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表 1 生物炭BET表征结果

Table 1. BET characterization results

Sample	Surface aera^a /(m²·g⁻¹)	Pore volume^b /(cm³·g ⁻¹)	Pore diameter^c /nm
Sorghum powder	11.8903	15.6159	0.023938
GC-H	65.1037	10.8345	0.048291
GC-S	189.3184	5.7914	0.115718
GC-Na	437.8670	7.6935	0.35028
GC-KC	737.9431	3.2892	0.353356
GC-KO	565.2083	3.8595	0.307675
GC-KH	2,096.0475	4.1166	1.000354
Grapefruit peel powder	8.7806	5.9119	0.010157
YC	144.5847	2.7633	0.070626
YC-K	1059.8472	2.5587	0.51121
Notes: a is BET multi-point method specific surface; b is BJH method desorption (cylindrical pore model, 2.0 nm−49.6 nm) pore volume; c is BJH method desorption (cylindrical hole model) average hole diameter.

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表 2 GC-KH吸附磷酸盐的伪一阶和二阶动力学参数

Table 2. Pseudo-first- and second-order kinetic parameters for phosphate adsorption by GC-KH

Sample	Pseudo-first-order model			Pseudo-second-order model
Sample	q_cal /(mg·g⁻¹)	k₁/(min⁻¹)	R²	q_cal /(mg·g⁻¹)	k₂ /(g·mg⁻¹·min⁻¹)	R²
GC-KH (15℃)	7.6071	0.0275	0.9649	12.3916	0.0807	0.9948
GC-KH (25℃)	15.1653	0.0310	0.9689	17.3974	0.0575	0.9939
GC-KH (35℃)	17.9383	0.0288	0.9712	21.8818	0.0457	0.9971
Notes: qcal is the adsorption capacity at equilibrium time; k1 and k2 are reaction rate constants of pseudo-first-order and pseudo-second-order equations, respectively; R² is the correlation coefficient.

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表 3 GC-KH吸附磷酸盐的Langmuir、Freundlich和DR等温线参数

Table 3. Langmuir, Freundlich and DR isotherm parameters for phosphate adsorption by GC-KH

Sample	Langmuir			Freundlich			D-R
Sample	q_m/(mg·g^-1)	KL /(L·mg^-1)	R²	KF /(mg·g^-1)	n	R²	q_m/(mol·g^-1)	E/(kJ·mol^-1)	R²
GC-KH (15℃)	44.79	0.0879	0.9829	8.45	2.72	0.9121	3.3532	5.64	0.8702
GC-KH (25℃)	49.92	0.1250	0.9738	12.21	3.12	0.9419	4.0295	7.68	0.8997
GC-KH (35℃)	74.73	0.1694	0.9445	22.87	3.59	0.9104	5.9133	11.57	0.8876
Notes: qm represents the maximum adsorption capacity of Langmuir; KL is Langmuir adsorption constant; KF is the Freundlich adsorption constant, and n is the constant related to the adsorption strength.

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表 4 GC-KH吸附磷酸盐的热力学参数

Table 4. Thermodynamic parameters of phosphate adsorption by GC-KH

C/(mg L⁻¹)	ΔH/(kJ·mol⁻¹)	ΔS/(J·mol⁻¹·K⁻¹)	ΔG/(kJ·mol⁻¹)
C/(mg L⁻¹)	ΔH/(kJ·mol⁻¹)	ΔS/(J·mol⁻¹·K⁻¹)	15℃	25℃	35℃
20	86.5333	311.6134	−89.6581	−92.7743	−95.8904
30	72.9616	257.7752	−74.1663	−76.7441	−79.3218
40	30.8975=	113.1529	−32.5572	−33.6887	−34.8202
50	36.3046	128.6047	−37.0018	−38.2879	−39.5739
60	39.3341	137.6547	−39.6052	−40.9818	−42.3583
80	34.9713	120.6423	−34.71	−35.9164	−37.1229
100	32.4302	109.8654	−31.6088	−32.7075	−33.8061
Notes: ΔG is Gibbs free energy change; ΔH is enthalpy change; ΔS is entropy change.

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