无机材料学报 ›› 2026, Vol. 41 ›› Issue (1): 12-26.DOI: 10.15541/jim20250019 CSTR: 32189.14.10.15541/jim20250019
范雨竹1(
), 王媛1, 王林燕1, 向美玲1, 鄢雨婷1, 黎本慧1, 李敏1, 文志东2,3, 王海超2,4, 陈永福5, 邱会东1, 赵波6, 周成裕1()
收稿日期:2025-01-14
修回日期:2025-04-14
出版日期:2026-01-20
网络出版日期:2025-05-09
通讯作者:
范雨竹, 副教授. E-mail: fanyuzhu1010@foxmail.com;作者简介:范雨竹(1990-), 女, 副教授. E-mail: fanyuzhu1010@foxmail.com
基金资助:
FAN Yuzhu1(), WANG Yuan1, WANG Linyan1, XIANG Meiling1, YAN Yuting1, LI Benhui1, LI Min1, WEN Zhidong2,3, WANG Haichao2,4, CHEN Yongfu5, QIU Huidong1, ZHAO Bo6, ZHOU Chengyu1()
Received:2025-01-14
Revised:2025-04-14
Published:2026-01-20
Online:2025-05-09
Contact:
FAN Yuzhu, associate professor. E-mail: fanyuzhu1010@foxmail.com;About author:FAN Yuzhu (1990-), female, associate professor. E-mail: fanyuzhu1010@foxmail.com
Supported by:摘要：
水体Pb(II)污染严重危害生态环境与人类健康, 而吸附法可以简单、环保地处理Pb(II)。氧化石墨烯(GO)是一种潜在的理想吸附材料, 但其表面官能团种类有限、吸附选择性差、吸附后难分离等缺点制约了其实际应用。发展各种改性策略提高GO吸附性能, 已成为目前研究热点。本文针对如何提高GO对水中Pb(II)的吸附效率, 重点总结了N/S官能团改性、形貌改性、磁化改性三类改性策略; 综述了GO基吸附剂的吸附性能, 涵盖吸附容量、吸附选择性、再生性以及其他性能; 详细讨论了Pb(II)吸附的四种机理, 包括物理吸附、静电吸引、离子交换和表面络合; 最后对GO基吸附剂去除Pb(II)进行了展望, 以期为GO改性材料在Pb(II)处理方面的研究和应用提供参考依据。
中图分类号:
范雨竹, 王媛, 王林燕, 向美玲, 鄢雨婷, 黎本慧, 李敏, 文志东, 王海超, 陈永福, 邱会东, 赵波, 周成裕. 氧化石墨烯基吸附材料去除水体中Pb(II): 制备、性能及机理[J]. 无机材料学报, 2026, 41(1): 12-26.
FAN Yuzhu, WANG Yuan, WANG Linyan, XIANG Meiling, YAN Yuting, LI Benhui, LI Min, WEN Zhidong, WANG Haichao, CHEN Yongfu, QIU Huidong, ZHAO Bo, ZHOU Chengyu. Graphene Oxide-based Adsorbents for Pb(II) Removing in Water: Progresses on Synthesis, Performance and Mechanism[J]. Journal of Inorganic Materials, 2026, 41(1): 12-26.
图1 GO改性策略及Pb(II)在GO基吸附剂上的吸附机理
Fig. 1 Modification strategies of GO and adsorption mechanisms of Pb(II) on GO-based absorbents
图2 氮化改性策略[22-23,26]
Fig. 2 N modification strategies[22-23,26] (a) Schematic diagram of synthesis of phen-GO[22]; (b, c) Adsorption processes of Pb(II) on (b) PPDG[23] and (c) GOPU[26]
图3 硫化改性策略[30-31]
Fig. 3 S modification strategies[30-31] (a, b) Adsorption processes of Pb(II) on (a) SH-graphene bio-sponges[30] and (b) MGO@LaS nanocomposites[31]
| Type | Adsorbent | Adsorption condition | Adsorption capacity/ (mg·g-1) | Removal efficiency/% | Removal efficiency after desorption (desorption agent, cycle number) | Adsorption mechanism | Isotherm/ kinetic model | |
|---|---|---|---|---|---|---|---|---|
| pH, time/min | Dosage/ (g·L−1) | |||||||
| N | GO-NH2[ | 4-6, 10 | 1 | 71.89 | − | − | SC, EA, IE | L/PSO |
| IAT-GO[ | 5, 30 | 1 | 124 | 92.3 | >97% (0.4 mol/L HNO3, 5) | SC | L/PSO | |
| IOGO[ | 5, 360 | 0.4 | 798.87 | 87 | − (10% HCl, 5) | SC | L/PSO | |
| GOCAS[ | 5.2, 45 | 0.5 | 138.7 | 93 | >50% (HCl, 4) | − | F/PSO | |
| MGO-EDTA[ | 6.8, 120 | 0.5 | 211.3 | 82.83 | − | SC | F/PSO | |
| phen-GO[ | 6.0, 30 | 1 | 548 | 95 | − | SC | L/PSO | |
| PPDG[ | 4-6, 40 | 0.35 | 800 | − | 30% (0.5 mol/L NaOH, 3) | SC | L/PSO | |
| GO-IIP[ | 6.5, 30 | 0.5 | 40.02 | − | − (2 mol/L HCl, 5) | SC | L/PSO | |
| S | GO/ZnO/CS[ | 5, 120 | 0.5 | 110.88 | 92.4 | − | − | −/PSO |
| GO-SOxR[ | 6.5, 190 | − | 285 | − | − | EA, HB | R/PSO | |
| GOCS[ | 5.5, 30 | 3 | 383.4 | − | 74.26% (0.1 mol/L HNO3, 5) | EA, SC | L/PSO | |
| SH-graphene bio-sponge[ | 5.3, 300 | 1 | 101.01 | 90 | >90% (0.1 mol/L HCl, 5) | EA, SC | L/PSO | |
| MGO@LaS[ | 5, 40 | 0.5 | 123.46 | 95 | − | EA, SC | L/PSO | |
| Fe3S4/rGO[ | 6, − | 2 | 285.71 | 29.59 | 76.88% (0.03 mol/L HNO3, 5) | SC | L/PSO | |
| PVA/GO-SH[ | 6, 60 | 1 | 218.62 | 94.7 | >75% (0.2 mol/L HCl, 5) | SC | L/PSO | |
表1
Table 1 Adsorption characteristics of N/S functional group-modified GO-based adsorbents for Pb(II)[22-23,25,28 -31,33 -40]
| Type | Adsorbent | Adsorption condition | Adsorption capacity/ (mg·g-1) | Removal efficiency/% | Removal efficiency after desorption (desorption agent, cycle number) | Adsorption mechanism | Isotherm/ kinetic model | |
|---|---|---|---|---|---|---|---|---|
| pH, time/min | Dosage/ (g·L−1) | |||||||
| N | GO-NH2[ | 4-6, 10 | 1 | 71.89 | − | − | SC, EA, IE | L/PSO |
| IAT-GO[ | 5, 30 | 1 | 124 | 92.3 | >97% (0.4 mol/L HNO3, 5) | SC | L/PSO | |
| IOGO[ | 5, 360 | 0.4 | 798.87 | 87 | − (10% HCl, 5) | SC | L/PSO | |
| GOCAS[ | 5.2, 45 | 0.5 | 138.7 | 93 | >50% (HCl, 4) | − | F/PSO | |
| MGO-EDTA[ | 6.8, 120 | 0.5 | 211.3 | 82.83 | − | SC | F/PSO | |
| phen-GO[ | 6.0, 30 | 1 | 548 | 95 | − | SC | L/PSO | |
| PPDG[ | 4-6, 40 | 0.35 | 800 | − | 30% (0.5 mol/L NaOH, 3) | SC | L/PSO | |
| GO-IIP[ | 6.5, 30 | 0.5 | 40.02 | − | − (2 mol/L HCl, 5) | SC | L/PSO | |
| S | GO/ZnO/CS[ | 5, 120 | 0.5 | 110.88 | 92.4 | − | − | −/PSO |
| GO-SOxR[ | 6.5, 190 | − | 285 | − | − | EA, HB | R/PSO | |
| GOCS[ | 5.5, 30 | 3 | 383.4 | − | 74.26% (0.1 mol/L HNO3, 5) | EA, SC | L/PSO | |
| SH-graphene bio-sponge[ | 5.3, 300 | 1 | 101.01 | 90 | >90% (0.1 mol/L HCl, 5) | EA, SC | L/PSO | |
| MGO@LaS[ | 5, 40 | 0.5 | 123.46 | 95 | − | EA, SC | L/PSO | |
| Fe3S4/rGO[ | 6, − | 2 | 285.71 | 29.59 | 76.88% (0.03 mol/L HNO3, 5) | SC | L/PSO | |
| PVA/GO-SH[ | 6, 60 | 1 | 218.62 | 94.7 | >75% (0.2 mol/L HCl, 5) | SC | L/PSO | |
图4 不同方法制备的PGO的TEM照片[41-42,44,46]
Fig. 4 TEM images of PGO obtained by different preparation methods[41-42,44,46] (a) Hydrothermal method[41]; (b) Template method[42]; (c) Oxidation etching method[46]; (d) High-energy electron irradiation method[44]
| Adsorbent | Adsorption condition | Adsorption capacity/ (mg·g-1) | Removal efficiency/% | Removal efficiency after desorption (desorption agent, cycle number) | Adsorption mechanism | Isotherm/ kinetic model | |
|---|---|---|---|---|---|---|---|
| pH, time/min | Dosage/ (g·L−1) | ||||||
| GO-Si[ | − | 1 | 347.2 | − | − | EA | L/PSO |
| GOCB[ | 5, 120 | 2 | − | − | 48% (0.1 mol/L Na2EDTA, 3) >93% (0.1 mol/L HCl, 3) | PA | −/PFO |
| PGOC[ | − | − | 99 | − | 81% (−, 5) | SC | − |
| NT-CGG[ | 6, <30 | 0.1 | 470 | 99.9998 | 88% (0.05 mol/L EDTA, 5) | SC | L/PSO |
| BC/GO[ | 5, 90 | 0.4 | 224.5 | − | − | SC, EA | F/PSO |
表2 形貌改性GO基吸附剂对Pb(II)的吸附特性[49-53]
Table 2 Adsorption characteristics of morphology-modified GO-based adsorbents for Pb(II)[49-53]
| Adsorbent | Adsorption condition | Adsorption capacity/ (mg·g-1) | Removal efficiency/% | Removal efficiency after desorption (desorption agent, cycle number) | Adsorption mechanism | Isotherm/ kinetic model | |
|---|---|---|---|---|---|---|---|
| pH, time/min | Dosage/ (g·L−1) | ||||||
| GO-Si[ | − | 1 | 347.2 | − | − | EA | L/PSO |
| GOCB[ | 5, 120 | 2 | − | − | 48% (0.1 mol/L Na2EDTA, 3) >93% (0.1 mol/L HCl, 3) | PA | −/PFO |
| PGOC[ | − | − | 99 | − | 81% (−, 5) | SC | − |
| NT-CGG[ | 6, <30 | 0.1 | 470 | 99.9998 | 88% (0.05 mol/L EDTA, 5) | SC | L/PSO |
| BC/GO[ | 5, 90 | 0.4 | 224.5 | − | − | SC, EA | F/PSO |
| Adsorbent | Adsorption condition | Adsorption capacity/ (mg·g−1) | Removal efficiency/% | Removal efficiency after desorption (desorption agent, cycle number) | Adsorption mechanism | Isotherm /kinetic model | |
|---|---|---|---|---|---|---|---|
| pH, time/min | Dosage/ (g·L−1) | ||||||
| MZIF-8/GO2[ | 4−6, 10 | 0.4 | 625 | 99 | − | − | L/PSO |
| PPy-FG[ | 5, 180 | 0.4 | 93.2 | 85.7 | 85.7% (0.2 mol/L HNO3, 5) | − | L/PSO |
| Fe3O4@C-GO-MOF[ | 6, 60 | 1 | 344.83 | 87 | >85% (5% (in volume) HNO3, 5) | SC | L/PSO |
| MnFe2O4@SiO2-NH2@GO[ | 6.5, 30 | 0.5 | 42.48 | 99.8 | − (0.3 mol/L HCl, 5) | SC | L/PSO |
| MCGO[ | 8, 44 | 0.5 | 372.24 | 93.06 | 68.9% (−, 5) | EA | L/PSO |
| MgFe2O4-NGO[ | 7, 120 | 1 | 930 | 99.7 | 83.6% (0.1 mol/L HCl, 6) | SC, EA, PA | L/PSO |
| SMGI[ | 7, 60 | 0.4 | 1666.66 | − | 75% (0.05 mol/L HCl, 5) | EA | L/F/PSO |
| NH2/β-CD/NH2/β-CD MGO[ | 6.5, 75 | − | 296.16 | − | − (0.1 mol/L HCl, 5) | SC | F/PSO |
表3
Table 3 Adsorption characteristics of magnetization-modified GO-based adsorbents for Pb(II)[54-61]
| Adsorbent | Adsorption condition | Adsorption capacity/ (mg·g−1) | Removal efficiency/% | Removal efficiency after desorption (desorption agent, cycle number) | Adsorption mechanism | Isotherm /kinetic model | |
|---|---|---|---|---|---|---|---|
| pH, time/min | Dosage/ (g·L−1) | ||||||
| MZIF-8/GO2[ | 4−6, 10 | 0.4 | 625 | 99 | − | − | L/PSO |
| PPy-FG[ | 5, 180 | 0.4 | 93.2 | 85.7 | 85.7% (0.2 mol/L HNO3, 5) | − | L/PSO |
| Fe3O4@C-GO-MOF[ | 6, 60 | 1 | 344.83 | 87 | >85% (5% (in volume) HNO3, 5) | SC | L/PSO |
| MnFe2O4@SiO2-NH2@GO[ | 6.5, 30 | 0.5 | 42.48 | 99.8 | − (0.3 mol/L HCl, 5) | SC | L/PSO |
| MCGO[ | 8, 44 | 0.5 | 372.24 | 93.06 | 68.9% (−, 5) | EA | L/PSO |
| MgFe2O4-NGO[ | 7, 120 | 1 | 930 | 99.7 | 83.6% (0.1 mol/L HCl, 6) | SC, EA, PA | L/PSO |
| SMGI[ | 7, 60 | 0.4 | 1666.66 | − | 75% (0.05 mol/L HCl, 5) | EA | L/F/PSO |
| NH2/β-CD/NH2/β-CD MGO[ | 6.5, 75 | − | 296.16 | − | − (0.1 mol/L HCl, 5) | SC | F/PSO |
图5 不同MGO纳米复合材料的合成路线示意图[67,69]
Fig. 5 Schematic diagrams of synthesis routes of different MGO nanocomposites[67,69] (a) pFe3O4-GO[67]; (b) CMC/SA/GO@Fe3O4 (including its adsorption process for Pb(II))[69]
图6 不同GO基吸附剂的吸附性能[29-30,54,71 -72,83 -84,87]
Fig. 6 Adsorption performance of different GO-based adsorbents[29-30,54,71 -72,83 -84,87] (a) Effects of contact time and initial concentration on lead adsorption by GO and GOCS[29]; (b) Effect of Pb(II) initial concentration on adsorption capacity of 3D CA/GO for Pb(II)[71]; (c) Effect of Pb(II) initial concentration on adsorption efficiency of MCGO for Pb(II)[54]; (d) Competitive adsorption of Cu(II), Pb(II), Zn(II), and Cd(II) ions on GO/P(AA-co-AM)[83]; (e) Selectivity of multiple metal ions for SH-graphene bio-sponge in comparison with activated carbon and alginate sponge[30]; (f-h) Recyclability of (f) GOLA[72], (g) GO-MBT[87] and (h) GFC nanosorbent[84] for Pb(II) removal
| Adsorbent | Adsorption condition | Adsorptioncapacity/ (mg·g−1) | Removal efficiency/% | Removal efficiency after desorption (desorption agent, cycle number) | Adsorption mechanism | Isotherm/ kinetic model | |
|---|---|---|---|---|---|---|---|
| pH, time/min | Dosage/ (g·L−1) | ||||||
| OSH[ | 8, 70 | 12 | 6.1 | − | 87% (0.1 mol/L HCl, 3) | EA | F/PSO |
| Zeolite[ | 6, 24 h | 1 | 14 | − | − | PA | L/PSO |
| Calcined MCM-41[ | 5, 120 | 4 | 18.8 | − | − | PA | F/PSO |
| Cu0.5Mg0.5Fe2O4[ | 7, 180 | 2 | 57.7 | 97 | ~90% (2 mol/L NaOH, 5) | − | L/PSO |
| AC/MIL-101(Al)[ | 6, 90 | 0.6 | 241 | − | 92.6% (HCl, 4) | EA, SC, IE | L/PSO |
| Ceramsite[ | 6, 750 | 12 | 46.7 | − | >80% (0.03 mol/L HCl/NaOH, 5) | IE, EA | L/PSO |
| AC from peanut shells[ | 4.5, 50 | 2 | 130.89 | 95 | 66% (NaCl, 4) | EA, IE, PA | L/PSO |
| FmB[ | 6.5, 180 | 1 | 73.68 | 95 | >41.2% (0.1 mol/L HCl, −) | EA, IE | L/PSO |
| PAANa[ | −, 170 | 10 | 173.6 | − | − | IE | F/L/PSO |
| GOLA[ | 5, 20 | 0.12 | 505.8 | − | 90.6% (HNO3, −) | SC | L/PSO |
| 3D CA/GO[ | 3, 240 | 0.4 | 490.2 | 99.8 | 91.6% (1 mol/L HCl, 8) | EA, SC, IE | F/PSO |
| Pip@MGO[ | 6, 27.5 | 0.7 | 558.2 | − | >90% (1 mol/L HNO3, 4) | SC, IE | − |
| FeGO-TiLa[ | 6, 120 | 2 | 109.89 | 93 | 71% (0.1 mol/L HCl, 10) | EA | L/PSO |
表4
Table 4 Comparsion on Pb(II) removal performance of GO-based and other adsorbents[68,71 -82]
| Adsorbent | Adsorption condition | Adsorptioncapacity/ (mg·g−1) | Removal efficiency/% | Removal efficiency after desorption (desorption agent, cycle number) | Adsorption mechanism | Isotherm/ kinetic model | |
|---|---|---|---|---|---|---|---|
| pH, time/min | Dosage/ (g·L−1) | ||||||
| OSH[ | 8, 70 | 12 | 6.1 | − | 87% (0.1 mol/L HCl, 3) | EA | F/PSO |
| Zeolite[ | 6, 24 h | 1 | 14 | − | − | PA | L/PSO |
| Calcined MCM-41[ | 5, 120 | 4 | 18.8 | − | − | PA | F/PSO |
| Cu0.5Mg0.5Fe2O4[ | 7, 180 | 2 | 57.7 | 97 | ~90% (2 mol/L NaOH, 5) | − | L/PSO |
| AC/MIL-101(Al)[ | 6, 90 | 0.6 | 241 | − | 92.6% (HCl, 4) | EA, SC, IE | L/PSO |
| Ceramsite[ | 6, 750 | 12 | 46.7 | − | >80% (0.03 mol/L HCl/NaOH, 5) | IE, EA | L/PSO |
| AC from peanut shells[ | 4.5, 50 | 2 | 130.89 | 95 | 66% (NaCl, 4) | EA, IE, PA | L/PSO |
| FmB[ | 6.5, 180 | 1 | 73.68 | 95 | >41.2% (0.1 mol/L HCl, −) | EA, IE | L/PSO |
| PAANa[ | −, 170 | 10 | 173.6 | − | − | IE | F/L/PSO |
| GOLA[ | 5, 20 | 0.12 | 505.8 | − | 90.6% (HNO3, −) | SC | L/PSO |
| 3D CA/GO[ | 3, 240 | 0.4 | 490.2 | 99.8 | 91.6% (1 mol/L HCl, 8) | EA, SC, IE | F/PSO |
| Pip@MGO[ | 6, 27.5 | 0.7 | 558.2 | − | >90% (1 mol/L HNO3, 4) | SC, IE | − |
| FeGO-TiLa[ | 6, 120 | 2 | 109.89 | 93 | 71% (0.1 mol/L HCl, 10) | EA | L/PSO |
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