超薄二维多孔纳米片在水处理中的研究进展

doi:10.16085/j.issn.1000-6613.2021-0092

化工进展 ›› 2021, Vol. 40 ›› Issue (12): 6859-6875.DOI: 10.16085/j.issn.1000-6613.2021-0092

超薄二维多孔纳米片在水处理中的研究进展

黄从新¹^,²(), 王顺藤¹^,², 范宇莹²^,³, 简美鹏⁴^,⁵(), 唐朝春¹, 刘锐平²^,⁶()

^1.华东交通大学土木建筑学院，江西南昌 330013
^2.中国科学院生态环境研究中心，中国科学院饮用水科学与技术重点实验室，北京 100085
^3.东北师范大学环境工程系，吉林长春 130117
^4.广东工业大学材料与能源学院，广东广州 510006
^5.蒙纳士大学化学工程系，澳大利亚维多利亚州 3800
^6.清华大学环境学院，清华大学水质与水生态研究中心，北京 100084

收稿日期:2021-01-14 修回日期:2021-03-07 出版日期:2021-12-05 发布日期:2021-12-21
通讯作者: 简美鹏,刘锐平
作者简介:黄从新（1997—），男，硕士研究生，研究方向为水处理理论与技术。E-mail：huangcongxin_13@163.com。
基金资助:
港澳及海外青年学者合作研究基金(51729801);中国博士后科学基金(2020M672532)

Advance of ultrathin 2D porous nanosheets in water treatment

HUANG Congxin¹^,²(), WANG Shunteng¹^,², FAN Yuying²^,³, JIAN Meipeng⁴^,⁵(), TANG Chaochun¹, LIU Ruiping²^,⁶()

^1.School of Civil Engineering and Architecture, East China Jiaotong University, Nanchang 330013, Jiangxi, China
^2.State Key Laboratory of Environmental Aquatic Chemistry, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China
^3.School of Environment, Northeast Normal University, Changchun 130117, Jilin, China
^4.School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006 Guangdong, China
^5.Department of Chemical Engineering, Monash University, Victoria 3800, Australia
^6.Center for Water and Ecology, State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China

Received:2021-01-14 Revised:2021-03-07 Online:2021-12-05 Published:2021-12-21
Contact: JIAN Meipeng,LIU Ruiping

摘要/Abstract

摘要：

二维（2D）纳米片是一类非常具有前瞻性的多孔材料。作为新型的高性能吸附剂，与传统吸附材料相比，超薄2D多孔纳米片具有高比表面积、原子级厚度和几乎完全裸露的活性位点等优点，可快速有效地捕获水体中的（有机或无机）污染物质。本综述总结了两类代表性的超薄2D多孔纳米片[金属有机骨架材料（MOFs）和共价有机骨架材料（COFs）]作为优良吸附剂去除水环境中有机染料、有毒重金属和放射性元素的最新进展。介绍了该类化合物的结构特性和物理化学性质，总结了四种常用合成方法，重点分析了四种方法的优缺点以及面临的挑战，并对不同的合成方法进行了特点比较。阐述了超薄2D多孔纳米片在水中对各种污染物的吸附条件和吸附性能，对相关吸附机理做了系统总结和对比。论述了材料的再生性能，总结分析了再生过程中可能遇到的问题。最后对当前超薄2D多孔纳米片存在的不足、合成条件复杂等问题，提出了材料的合成优化、绿色无毒或低毒新技术的开发、重复使用效率的提高将会是未来的发展方向。

关键词: 二维多孔纳米片, 吸附, 有机染料, 重金属, 放射性元素

Abstract:

Two-dimensional (2D) nanosheets are a kind of appealing porous materials. As a new type of highperformance adsorbent, the ultrathin 2D porous nanosheets have the advantages of high specific surface area, atomic thickness and abundant exposed active sites (organic or inorganic) in comparison with traditional adsorption materials. The pollutants can be selectively captured from aqueous solution quickly and effectively. This paper reviewed the latest progress of three representative 2D porous nanosheets [metal organic frameworks (MOFs) and covalent organic frameworks (COFs)] as excellent adsorbents for the removal of organic dyes, toxic heavy metals and radioactive elements from water environment. The structural characteristics and physicochemical properties of these compounds were introduced, and four commonly used synthetic methods were summarized. The advantages, disadvantages and challenges of the four methods were analyzed, and the characteristics of different synthesis methods were compared. The adsorption conditions and performance of ultra-thin 2D porous nanosheets for various pollutants in water were described, and the relevant adsorption mechanisms were systematically summarized and compared. The regeneration properties of materials were discussed, and the problems that may be encountered in the process of regeneration were introduced and analyzed. Finally, in view of the shortcomings and complex synthesis conditions of the ultra-thin 2D porous nanosheets, the optimization direction of the material synthesis, the development of green non-toxic or low-toxic new technologies and the improvement of reuse efficiency would be the development direction in the future.

Key words: two-dimensional porous nanosheets, adsorption, organic dyes, heavy metals, radioactive elements

中图分类号:

X703.1

黄从新, 王顺藤, 范宇莹, 简美鹏, 唐朝春, 刘锐平. 超薄二维多孔纳米片在水处理中的研究进展[J]. 化工进展, 2021, 40(12): 6859-6875.

HUANG Congxin, WANG Shunteng, FAN Yuying, JIAN Meipeng, TANG Chaochun, LIU Ruiping. Advance of ultrathin 2D porous nanosheets in water treatment[J]. Chemical Industry and Engineering Progress, 2021, 40(12): 6859-6875.

图/表 14

图1 超薄2D多孔纳米材料MOFs和COFs的图示、合成方法及污染物吸附应用

图2 Zn2(Bim)4分子筛纳米片（MSN）的表征和模型图[29]

图3 TPA-COF材料的合成、表征和晶体结构图[49]

图4 两种2D COFs的剥离方法

表1 几种超薄2D多孔纳米片的制备方法比较

制备方法	制备条件	特点	产品质量
微机械剥离	以层状块体为原料，借助透明胶带或研磨	缺陷少，厚度和形状难控制，适合大的层状晶体材料	尺寸小，产量极低
液基剥离	以层状粉末为原料，通过插层剂或超声的方式	成本较低，操作相对简单，可量化生产，不使用有毒有害的有机溶剂	尺寸较小，较宽的厚度，产量偏低
化学气相沉积	特定的CVD设备，高温高真空，挥发性前体在基体上沉积	衬底选择不具有任意性，不可避免地会引入残留物和缺陷，低温下合成难度大	产品纯度高，质量好，多为片状
水热合成	高温或蒸气压下，在水溶液或有机溶液中结晶	成本低，高产率，可大批量生产，控制参数多，获得单层纳米片难度大	成分可控，大型优质，纳米薄片

图5 部分染料的结构示意图

图6 铀基MOF对亚甲基蓝在不同吸附时间下的紫外光谱[81]

表2 各种超薄2D多孔纳米片吸附水中染料的差异对比

吸附剂	吸附剂带电性	染料	吸附强弱	主要吸附机理	文献来源
［（CH₃）₂NH₂］₂［（Ca₄O）L₄（H₂O）₄］·6DMF （SHU-1）	-	MG、CR、CV、RhB	MG>RhB>CR>CV	尺寸排斥、酸碱相互作用、π-π相互作用	［79］
IPM-MOF-201	+	MO、MB、IC、BTB	MO>IC>MB>BTB	—SO $3 -$ 与染料分子之间的离子交换、尺寸选择	［80］
［（CH₃）₂NH₂］［UO₂（TATAB）］·2DMF·4H₂O （U-TATAB）	-	MB、ST、茜素、MO、EY	MB>ST>茜素>MO>EY	层间不配位阳离子与阳离子染料离子交换作用、仲胺基团与染料相互作用	［81］
Cu-TCPP-MOF	-	RhB、MB、CR	MB>CR>RhB	—COO^-与染料分子相互作用、静电作用	［85］
Ni-MOF	-	MB、CR	MB>CR	静电引力、π-π相互作用、氢键相互作用	［86］
［Zn₂（tpdc）₂（H₂O）₂］（H₂O）₂（DMF）₅ （Zn-MOF）	中性	NR、BR-2、MO	NR>BR-2>MO	尺寸选择	［88］
Ttba-TPDA-COF	-	RhB	—	三嗪基和亚氨基与RhB分子的静电作用	［89］
PC-COF	+	MO、AG-25、DFBM、AR-27	AR-27>MO>DFBM>AG-25	染料与层间Cl^-交换作用	［91］

表2 各种超薄2D多孔纳米片吸附水中染料的差异对比

吸附剂	吸附剂带电性	染料	吸附强弱	主要吸附机理	文献来源
［（CH₃）₂NH₂］₂［（Ca₄O）L₄（H₂O）₄］·6DMF （SHU-1）	-	MG、CR、CV、RhB	MG>RhB>CR>CV	尺寸排斥、酸碱相互作用、π-π相互作用	［79］
IPM-MOF-201	+	MO、MB、IC、BTB	MO>IC>MB>BTB	—SO $3 -$ 与染料分子之间的离子交换、尺寸选择	［80］
［（CH₃）₂NH₂］［UO₂（TATAB）］·2DMF·4H₂O （U-TATAB）	-	MB、ST、茜素、MO、EY	MB>ST>茜素>MO>EY	层间不配位阳离子与阳离子染料离子交换作用、仲胺基团与染料相互作用	［81］
Cu-TCPP-MOF	-	RhB、MB、CR	MB>CR>RhB	—COO^-与染料分子相互作用、静电作用	［85］
Ni-MOF	-	MB、CR	MB>CR	静电引力、π-π相互作用、氢键相互作用	［86］
［Zn₂（tpdc）₂（H₂O）₂］（H₂O）₂（DMF）₅ （Zn-MOF）	中性	NR、BR-2、MO	NR>BR-2>MO	尺寸选择	［88］
Ttba-TPDA-COF	-	RhB	—	三嗪基和亚氨基与RhB分子的静电作用	［89］
PC-COF	+	MO、AG-25、DFBM、AR-27	AR-27>MO>DFBM>AG-25	染料与层间Cl^-交换作用	［91］

图7 2D-NCS捕获氯化汞形成2D-NCS@Hg和2D-NCS的再生示意图[97]

图8 Zn(Bim)(OAc)-NS上可能形成的Pb2+和Cu2+配合物的示意图[100]

图9 MPCOF的制备以及对铀的吸附模型[103]

表3 各种超薄2D多孔纳米片用于水中重金属离子吸附的差异对比

金属离子	吸附剂	吸附强弱	主要吸附机理	文献来源
Hg²⁺	｛［Co（NCS）₂（pyz）₂］｝_n （2D-NCS）	高亲和力（K_d=2.26×10⁶mL/g）	2D-NCS的吡嗪环之间的阳离子-π相互作用，硫氰酸根与Hg²⁺的螯合作用	［97］
Hg²⁺、Pb²⁺、Cu²⁺、Zn²⁺	COF-S-SH	Hg²⁺>Pb²⁺>Cu²⁺>Zn²⁺	含硫基团与Hg²⁺的螯合作用	［98］
Pb²⁺、Cu²⁺、Fe³⁺、Cd²⁺、Mn²⁺、Cr⁶⁺	COF-SH	Pb²⁺>Cu²⁺>Fe³⁺>Cd²⁺>Mn²⁺>Cr⁶⁺	Pb²⁺与巯基之间的静电吸引或螯合作用	［99］
Pb²⁺、Cu²⁺、Ni²⁺、Co²⁺、Cd²⁺	Zn（Bim）（OAc）-NS	Pb²⁺>Cu²⁺>Ni²⁺>Co²⁺>Cd²⁺	—NH₂、—OH与重金属离子的络合作用	［100］
Pb²⁺、Ni²⁺、Zn²⁺、Cu²⁺、Cd²⁺	［Ca（H₄L）（DMA）₂］·2DMA （Ca-MOF）	Pb²⁺>Cd²⁺>Ni²⁺>Cu²⁺>Zn²⁺	Ca²⁺与重金属离子之间的离子交换作用	［101］
Cu²⁺、Hg²⁺、Pb²⁺、Cd²⁺、Cr²⁺	TpODH-COF	Cu²⁺>Hg²⁺>Pb²⁺>Cr²⁺>Cd²⁺	Cu²⁺与酰胺、氨基和羰基之间的配位作用	［102］
UO $2 2 +$ 、La³⁺、Ce³⁺、Nd³⁺、Sm³⁺、Gd³⁺	MPCOF	UO $2 2 +$ >Nd³⁺>Sm³⁺>Gd³⁺>Ce³⁺>La³⁺	颗粒内扩散和阳离子筛分效应	［103］

表3 各种超薄2D多孔纳米片用于水中重金属离子吸附的差异对比

金属离子	吸附剂	吸附强弱	主要吸附机理	文献来源
Hg²⁺	｛［Co（NCS）₂（pyz）₂］｝_n （2D-NCS）	高亲和力（K_d=2.26×10⁶mL/g）	2D-NCS的吡嗪环之间的阳离子-π相互作用，硫氰酸根与Hg²⁺的螯合作用	［97］
Hg²⁺、Pb²⁺、Cu²⁺、Zn²⁺	COF-S-SH	Hg²⁺>Pb²⁺>Cu²⁺>Zn²⁺	含硫基团与Hg²⁺的螯合作用	［98］
Pb²⁺、Cu²⁺、Fe³⁺、Cd²⁺、Mn²⁺、Cr⁶⁺	COF-SH	Pb²⁺>Cu²⁺>Fe³⁺>Cd²⁺>Mn²⁺>Cr⁶⁺	Pb²⁺与巯基之间的静电吸引或螯合作用	［99］
Pb²⁺、Cu²⁺、Ni²⁺、Co²⁺、Cd²⁺	Zn（Bim）（OAc）-NS	Pb²⁺>Cu²⁺>Ni²⁺>Co²⁺>Cd²⁺	—NH₂、—OH与重金属离子的络合作用	［100］
Pb²⁺、Ni²⁺、Zn²⁺、Cu²⁺、Cd²⁺	［Ca（H₄L）（DMA）₂］·2DMA （Ca-MOF）	Pb²⁺>Cd²⁺>Ni²⁺>Cu²⁺>Zn²⁺	Ca²⁺与重金属离子之间的离子交换作用	［101］
Cu²⁺、Hg²⁺、Pb²⁺、Cd²⁺、Cr²⁺	TpODH-COF	Cu²⁺>Hg²⁺>Pb²⁺>Cr²⁺>Cd²⁺	Cu²⁺与酰胺、氨基和羰基之间的配位作用	［102］
UO $2 2 +$ 、La³⁺、Ce³⁺、Nd³⁺、Sm³⁺、Gd³⁺	MPCOF	UO $2 2 +$ >Nd³⁺>Sm³⁺>Gd³⁺>Ce³⁺>La³⁺	颗粒内扩散和阳离子筛分效应	［103］

图10 2D MOF/2D COF对有机染料和重金属离子的吸附机理

表4 各种超薄2D多孔纳米片用于水中污染物吸附再生性能对比

污染物	吸附剂	解吸剂	再生性能	文献来源
CR、RhB、MB、MO	｛［Mn₃（L¹）₂（L²）₂（H₂O）₈］·4H₂O｝_n（Mn-MOF）	DMF	95%（5次）	［104］
CR、MO	｛［Zn₂（5-OH-BDC）₂L₂］·1.5H₂O｝_n（Zn-MOF）	—	86.79%（7次）	［105］
MB	［（1，2-DPE）Co₂Cl₂］_n（HT-1）	乙醇	＞80%（5次）	［106］
Hg²⁺、Pb²⁺、Zn²⁺、Fe³⁺	TAPB-BMTTPA-COF	6mol/L的盐酸	92%（6次）	［107］
Cu²⁺、Hg²⁺、Pb²⁺、Cd²⁺、Cr²⁺	TpODH-COF	6mmol/L的盐酸	51%（2次）	［102］
Hg²⁺	｛Zn（BDC）（L^?）｝·DMF（TMU-40）	0.5mol/L的硝酸	90%（3次）	［108］

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超薄二维多孔纳米片在水处理中的研究进展

Advance of ultrathin 2D porous nanosheets in water treatment

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