离子液体二维结构制备及其特性研究进展

doi:10.6023/A20100475

化学学报 ›› 2021, Vol. 79 ›› Issue (4): 443-458.DOI: 10.6023/A20100475 上一篇下一篇

综述

离子液体二维结构制备及其特性研究进展

吕玉苗^a, 陈伟^a^,^b, 王艳磊^a, 霍锋^a, 董依慧^a, 魏莉^b^,^*(), 何宏艳^a^,^*()

a 中国科学院过程工程研究所离子液体清洁过程北京市重点实验室绿色过程与工程重点实验室北京 100190
b 大连工业大学轻工与化学工程学院大连 116034

投稿日期:2020-10-15 发布日期:2020-11-24
通讯作者: 魏莉, 何宏艳

作者简介:

吕玉苗, 女, 助理研究员, 主要从事离子液体表界面结构、性质及应用研究. 2017年获得中国科学院物理研究所和香港城市大学博士学位, 同年加入中国科学院过程工程研究所从事助研工作, 发表SCI论文11篇, 主持国家自然科学基金青年科学基金1项, 参与国家自然科学基金委重大项目1项.

陈伟, 男, 大连工业大学轻工与化学工程学院在读硕士研究生, 中国科学院过程工程研究所联合培养硕士, 研究方向为离子液体二维结构在固体表界面的结构及性质.

魏莉, 女, 副教授, 硕士生导师. 2004年获得大连理工大学应用化学专业博士学位. 主要从事以离子液体为基质的有机催化、生物基材料合成, 离子液体电池等研究. 主持辽宁省教育厅项目1项, 辽宁省科技厅项目1项, 参加国家“973”子课题项目1项, 国家自然科学基金项目1项, 教育部重点项目1项, 省级项目4项, 市级3项, 发表论文20余篇.

何宏艳, 女, 研究员, 博士生导师, 国家自然科学基金优秀青年基金获得者. 主要从事界面离子液体结构与功能、离子液体特殊氢键与反应性能、离子液体催化木质素/CO₂转化等方向的研究工作. 相关研究成果在Chem、Small、Chem. Eng. Sci.、Green Chem.、PCCP等期刊发表SCI论文80余篇, 申请发明专利17项, 获授权6项. 主持国家自然科学基金项目、北京市基金和中科院基金等多项. 获侯德榜化工技术青年奖、中国化工学会离子液体专委会青年创新奖、中科院科技促进发展奖及中国石油和化学工业协会科学技术奖等多项. 2017年入选中科院青年创新促进会.

† These authors contributed equally to this work

基金资助:
国家自然科学基金(21922813); 国家自然科学基金(21908221); 国家自然科学基金(21776278); 国家自然科学基金(21808220); 中国科学院青年创新促进会(2017066); 多相复杂系统国家重点实验室自主部署课题(MPCS-2019-A-08)

Research Progress on the Preparation and Properties of Two Dimensional Structure of Ionic Liquids

Yumiao Lu^a, Wei Chen^a^,^b, Yanlei Wang^a, Feng Huo^a, Yihui Dong^a, Li Wei^b^,^*(), Hongyan He^a^,^*()

a CAS Key Laboratory of Green Process and Engineering, Beijing Key Laboratory of Ionic Liquids Clean Process, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China
b College of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian 116034, China

Received:2020-10-15 Published:2020-11-24
Contact: Li Wei, Hongyan He
About author:
* E-mail: weili@dlpu.edu.cn;
E-mail: hyhe@ipe.ac.cn; Tel.: 0086-010-82627080
Supported by:
National Natural Science Foundation of China(21922813); National Natural Science Foundation of China(21908221); National Natural Science Foundation of China(21776278); National Natural Science Foundation of China(21808220); Youth Innovation Promotion Association, CAS(2017066); State Key Laboratory of Multiphase Complex Systems(MPCS-2019-A-08)

文章分享

摘要/Abstract

由于阴阳离子间特殊的静电、氢键作用, 具有二维结构的离子液体呈现出独特的结构特征及热力学、动力学特性, 在化学化工和材料领域都有着巨大的应用前景, 已成为离子液体领域重要的研究方向之一. 本综述重点介绍了离子液体二维结构常用的制备方法, 包括自组装法、Langmuir-Blodgett法以及物理气相沉积法, 并总结了这些制备方法相应的优缺点. 随后归纳了离子液体二维结构的相变特征及在力学和电学方面的特性, 并综述了其在摩擦润滑领域的应用. 最后展望了离子液体二维结构的发展方向及应用前景.

关键词: 离子液体, 二维结构, 制备方法, 相变, 力学/电学特性

As green alternatives to non-environmental reagents, ionic liquids (ILs) have brought about a revolution in green chemical engineering. Very recently, attention to interfacial ILs has arisen. As a new structural type of ionic liquid, the ionic liquid (IL) with two-dimensional structure is endowed with unique structural features, thermodynamic and dynamic characteristics due to its special electrostatic and hydrogen bonds. It shows excellent application prospects in the field of chemistry and materials and has become one of the important research directions in the field of ILs. The standard preparation methods of two-dimensional structure ILs, including self-assembly, Langmuir-Blodgett and physical vapor deposition (PVD) methods are introduced in this review. The advantages and disadvantages of each method are also summarized. Self-assembly is the easiest and most widely used method to prepare two-dimensional ILs and the obtained structure is stable at room temperature. Meanwhile, the two-dimensional structure can be regulated by choosing different polar solvents and solutions with different concentrations. Langmuir-Blodgett method is suitable for polyionic liquids and amphiphilic ILs, because it requires monolayer IL to be formed on the water surface. PVD is mainly for ILs with high stability in the heating process under vacuum conditions, through which precise regulation of two-dimensional ILs structure can be achieved at ion level. However, the structure is sensitive to temperature, and temperatures higher than 100 K will destroy it. Then we review the phase transition feature, mechanical and electrical characteristics of two-dimensional structure ILs, including the lubrication applications. The enhanced surface effect results in the liquid-solid transition of ILs and the tendency of solidification is stronger when approaching the solid surface. On one hand, the conductivity decreases drastically with decreasing the thickness of two-dimensional ILs structure due to solidification. On the other hand, the solidification contributes to better lubrication performance with stronger resistance to friction and wear. Finally, the future development and broad application of two-dimensional structure ILs are envisioned.

Key words: ionic liquid, two-dimensional structure, preparation method, phase transition, mechanical/electrical property

引用此文

吕玉苗, 陈伟, 王艳磊, 霍锋, 董依慧, 魏莉, 何宏艳. 离子液体二维结构制备及其特性研究进展[J]. 化学学报, 2021, 79(4): 443-458.

Yumiao Lu, Wei Chen, Yanlei Wang, Feng Huo, Yihui Dong, Li Wei, Hongyan He. Research Progress on the Preparation and Properties of Two Dimensional Structure of Ionic Liquids[J]. Acta Chimica Sinica, 2021, 79(4): 443-458.

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图/表 17

离子液体	基底	溶剂^a	方法	参考文献
[Emim][NTFI]	云母	—	润湿法	^[40-41]
[Emim][FAP]	氢化的类金刚石膜/Si	Vertrel XF (2,3-二氢十氟戊烷)	浸涂法	^[42]
[Pmim]Br	羟基化Si(100)	C₂H₅OH	浸涂法	^[43]
[Pmim]CO₃	羟基化Si(100)	C₂H₅OH	浸涂法	^[43]
[Pmim]Cl	羟基化Si(100)	C₂H₅OH	浸涂法	^[43]
[Pmim] SO₃	羟基化Si(100)	C₂H₅OH	浸涂法	^[43]
[Bmim][FAP]	氢化的类金刚石膜/Si	Vertrel XF	浸涂法	^[42,44]
[Bmim][PF₆]	云母	CH₃OH	滴涂法	^[36]
	氧化Si(100)	(CH₃)₂CHOH	浸涂法	^[32]
	Si(100)	(CH₃)₂CHOH	浸涂法	^[33]
	羟基化/氨基化Si(100)	CH₃COCH₃	浸涂法	^[34]
	HOPG	CH₃OH	旋涂法	^[45]
	Si(100)	CH₃COCH₃	浸涂法	^[46]
	羟基化Si(100)	CH₃COCH₃	浸涂法	^[47]
[Bmim][NTFI]	SiO₂/Si(110)/云母/HOPG	CH₃OH	滴涂法	^[37]
	Si/SiO₂/MgO/ 云母/TiO₂/NaCl	CH₃OH/C₂H₅OH/CHCl₃	滴涂法	^[38]
	云母	—	润湿法	^[40-41]
	氧化Si(110)/SiO₂	CH₃OH	滴涂法	^[48]
	羟基化SiO₂	CH₃OH	旋涂法	^[49]
	羟基化SiO₂	CH₃OH	旋涂法	^[50]
[Bmim][BF₄]	羟基化/氨基化Si(100)	CH₃COCH₃	浸涂法	^[34]
	Si(100)	CH₃COCH₃	浸涂法	^[51]
	Si(100)	CH₃COCH₃	浸涂法	^[46]
[Bmim][OctSO₄]	氧化Si(100)	(CH₃)₂CHOH	浸涂法	^[32]
[Bmim][Apc]	羟基化/氨基化Si(100)	CH₃COCH₃	浸涂法	^[34]
[Bmim][ClO₄]	Si(100)	CH₃COCH₃	浸涂法	^[46]
[Bmim][NO₃]	Si(100)	CH₃COCH₃	浸涂法	^[46]
[Hmim][NTFI]	云母	—	润湿法	^[40-41]
[Hmim][NTFI]	羟基化SiO₂	CH₃OH	旋涂法	^[50]
[Hmim][FAP]	氢化的类金刚石膜/Si	Vertrel XF	浸涂法	^[42]
[Omim][BF₄]	Al	C₂H₅OH	旋涂法	^[52]
[Dmim][NTFI]	羟基化SiO₂	CH₃OH	旋涂法	^[50]
[Dmim][PF₆]	羟基化Si(100)	CH₃COCH₃	浸涂法	^[47]
[BPtmSiIm][BMdB]	羟基化Si	CH₃COCH₃	旋涂法	^[53]
硫醇端基IL	Au	C₂H₅OH	浸入法	^[54]
巯基IL	Au	C₂H₅OH	浸入法	^[55]
咪唑IL-COOH	氨基化Si(100)	CH₃COCH₃	浸涂法	^[56]
咪唑磷酸盐IL	羟基化Si(100)	CH₃COCH₃	浸涂法	^[57]
羟乙基IL	Si(100)	CH₃COCH₃	浸涂法	^[58]
双阳离子IL	Si(100)	(CH₃)₂CHOH	浸涂法	^[33]
[AEImi]Cl	羟基化Si(100)	C₂H₅OH	浸涂法	^[59]
[MOEDEA][FAP]	氢化的类金刚石膜/Si	Vertrel XF	浸涂法	^[42,44]
[AHIm][PF₆]	羟基/乙烯基/氢化/甲基化Si	CH₂Cl₂	旋涂法	^[60]
[HEHIm][PF₆]	羟基/乙烯基/氢化/甲基化Si	CH₂Cl₂	旋涂法	^[60]
[P₄₄₄₆][BF₄]	Si(100)	CH₃COCH₃	浸涂法	^[51]
[BPy][BF₄]	Si(100)	CH₃COCH₃	浸涂法	^[51]

离子液体	基底	溶剂^a	方法	参考文献
[Emim][NTFI]	云母	—	润湿法	^[40-41]
[Emim][FAP]	氢化的类金刚石膜/Si	Vertrel XF (2,3-二氢十氟戊烷)	浸涂法	^[42]
[Pmim]Br	羟基化Si(100)	C₂H₅OH	浸涂法	^[43]
[Pmim]CO₃	羟基化Si(100)	C₂H₅OH	浸涂法	^[43]
[Pmim]Cl	羟基化Si(100)	C₂H₅OH	浸涂法	^[43]
[Pmim] SO₃	羟基化Si(100)	C₂H₅OH	浸涂法	^[43]
[Bmim][FAP]	氢化的类金刚石膜/Si	Vertrel XF	浸涂法	^[42,44]
[Bmim][PF₆]	云母	CH₃OH	滴涂法	^[36]
	氧化Si(100)	(CH₃)₂CHOH	浸涂法	^[32]
	Si(100)	(CH₃)₂CHOH	浸涂法	^[33]
	羟基化/氨基化Si(100)	CH₃COCH₃	浸涂法	^[34]
	HOPG	CH₃OH	旋涂法	^[45]
	Si(100)	CH₃COCH₃	浸涂法	^[46]
	羟基化Si(100)	CH₃COCH₃	浸涂法	^[47]
[Bmim][NTFI]	SiO₂/Si(110)/云母/HOPG	CH₃OH	滴涂法	^[37]
	Si/SiO₂/MgO/ 云母/TiO₂/NaCl	CH₃OH/C₂H₅OH/CHCl₃	滴涂法	^[38]
	云母	—	润湿法	^[40-41]
	氧化Si(110)/SiO₂	CH₃OH	滴涂法	^[48]
	羟基化SiO₂	CH₃OH	旋涂法	^[49]
	羟基化SiO₂	CH₃OH	旋涂法	^[50]
[Bmim][BF₄]	羟基化/氨基化Si(100)	CH₃COCH₃	浸涂法	^[34]
	Si(100)	CH₃COCH₃	浸涂法	^[51]
	Si(100)	CH₃COCH₃	浸涂法	^[46]
[Bmim][OctSO₄]	氧化Si(100)	(CH₃)₂CHOH	浸涂法	^[32]
[Bmim][Apc]	羟基化/氨基化Si(100)	CH₃COCH₃	浸涂法	^[34]
[Bmim][ClO₄]	Si(100)	CH₃COCH₃	浸涂法	^[46]
[Bmim][NO₃]	Si(100)	CH₃COCH₃	浸涂法	^[46]
[Hmim][NTFI]	云母	—	润湿法	^[40-41]
[Hmim][NTFI]	羟基化SiO₂	CH₃OH	旋涂法	^[50]
[Hmim][FAP]	氢化的类金刚石膜/Si	Vertrel XF	浸涂法	^[42]
[Omim][BF₄]	Al	C₂H₅OH	旋涂法	^[52]
[Dmim][NTFI]	羟基化SiO₂	CH₃OH	旋涂法	^[50]
[Dmim][PF₆]	羟基化Si(100)	CH₃COCH₃	浸涂法	^[47]
[BPtmSiIm][BMdB]	羟基化Si	CH₃COCH₃	旋涂法	^[53]
硫醇端基IL	Au	C₂H₅OH	浸入法	^[54]
巯基IL	Au	C₂H₅OH	浸入法	^[55]
咪唑IL-COOH	氨基化Si(100)	CH₃COCH₃	浸涂法	^[56]
咪唑磷酸盐IL	羟基化Si(100)	CH₃COCH₃	浸涂法	^[57]
羟乙基IL	Si(100)	CH₃COCH₃	浸涂法	^[58]
双阳离子IL	Si(100)	(CH₃)₂CHOH	浸涂法	^[33]
[AEImi]Cl	羟基化Si(100)	C₂H₅OH	浸涂法	^[59]
[MOEDEA][FAP]	氢化的类金刚石膜/Si	Vertrel XF	浸涂法	^[42,44]
[AHIm][PF₆]	羟基/乙烯基/氢化/甲基化Si	CH₂Cl₂	旋涂法	^[60]
[HEHIm][PF₆]	羟基/乙烯基/氢化/甲基化Si	CH₂Cl₂	旋涂法	^[60]
[P₄₄₄₆][BF₄]	Si(100)	CH₃COCH₃	浸涂法	^[51]
[BPy][BF₄]	Si(100)	CH₃COCH₃	浸涂法	^[51]

表1. 自组装法制备离子液体二维结构中相关参数列表

Table 1. List of preparation parameters for two-dimensional ionic liquids via self-assembly method

表1. 自组装法制备离子液体二维结构中相关参数列表

Table 1. List of preparation parameters for two-dimensional ionic liquids via self-assembly method

图1. (a) [Bmim][PF6]在云母表面的层状结构AFM图像, (b) 基底云母的原子像, (c) 层状结构和液滴共存的AFM图像[36]

Figure 1. (a) AFM image of layered structure of [Bmim][PF6] on mica surface, (b) atomic image of basal mica, (c) AFM image of coexistence of layered structure and droplets [36]

图2. 自组装单层膜(SAMs)的生长机理和前驱膜随时间生长示意图: 分子或离子液体在固体表面上的重排过程[40]

Figure 2. Schematic diagram of growth mechanism of self-assembled monolayer (SAM) and precursor membrane growth over time: the rearrangement of molecules or ionic liquids at solid surface[40]

图3. [Bmim][NTFI]薄膜的制备过程示意图. 第一步用类似[Bmim][NTFI]结构的离子单层对SiO2表面进行功能化. 第二步将溶解在甲醇中的[Bmim][NTFI]旋涂在功能化的表面[49]

Figure 3. Schematic diagram of the preparation process of [Bmim][NTFI] thin film. The first step is to functionalize the SiO2 surface with ion monolayer similar to [Bmim][NTFI] structure. A second step is to spin coating the [Bmim][NTFI] dissolved in methanol onto the functionalized surface[49]

图4. [Bmim][NTFI]滴涂在不同基底表面的AFM形貌图: (A)氧化硅(甲醇溶液), (B)氧化硅(乙醇溶液), (C)氧化硅(氯仿溶液), (D)单晶抛光MgO(甲醇溶液), (E)单晶抛光TiO2金红石(甲醇溶液)和(F)单晶NaCl(甲醇溶液)[38]

Figure 4. Surface morphology of drop-casted [Bmim][NTFI] on different substrate surfaces: (A) oxidized silicon (methanol solution), (B) oxidized silicon (ethanol solution), (C) oxidized silicon (chloroform solution), (D) single crystal polished MgO (methanol solution), (E) single crystal polished TiO2 rutile (methanol solution) and (F) single crystal NaCl (methanol solution)[38]

离子液体	基底	除气温度^a T/K	除气时间^b t/h	压强 p/Pa	蒸发温度 T/K	蒸发时间^c t/min	基底温度 T/K	结构稳定温度T/K	参考文献
[BMP][FAP]	Au(111)	438~463	N	4×10^–8	450	10 s	298	210	^[69]
[BMP][NTFI]	Ag(111)	—	24	1×10^–8	373	3	—	100~180	^[71]
	TiO₂(110)	350	24	2×10^–8	453	5	—	80~380	^[72]
	Au(111)	360	N	5×10^–8	375	3	—	111~170	^[26]
	Ag(111)	360	N	5×10^–8	375	3	—	134~180	^[26]
	Au(111)	—	24	5×10^–8	375	3	—	100~225	^[73]
	Cu(111)	400	N	2×10^–8	450	—	200	80~200	^[74,76]
	HOPG(0001)	400	N	2×10^–8	450	—	—	100	^[75]
[Mmim][NTFI]	Ni(111)	400	N	1×10^–8	440	—	220±20	220	^[77]
	Au(111)	380~410	N	1×10^–7	410~440	—	290~320	—	^[78]
	Ag(111)	—	—	2×10^–7	380~430	—	295~320	300	^[79]
[Emim][NTFI]	Au(111)	350	24	1×10^–8	350~390	—	—	107~113	^[28]
	Ag(111)	350	24	1×10^–8	350~390	—	—	108~130	^[28]
	HOPG	—	—	1×10^–6	—	—	—	180~205	^[25]
	Ni(111)	353	12	1×10^–6	—	—	150	150~200	^[80]
	玻璃	—	—	6×10^–7	320	30	—	—	^[81]
	Au(110)	—	—	5×10^–8	423~523	—	128	311~323	^[82]
[Emim][OTF]	Pd(111)	—	—	2×10^–8	220	—	220	220	^[83]
	Au(111)	—	—	1×10^–7	440	—	298	—	^[84]
	Pd(111)	—	—	2×10^–8	300	—	298	300~380	^[85]
[Bmim][NTFI]	Al₂O₃/NiAl(110)	—	—	2×10^–8	425~475	N	—	298~323	^[86]
[Hmim][NTFI]	CeO₂(111)/CeO_2–_x	—	N	1×10^–8	385	—	160	—	^[87]
[Omim][NTFI]	Au(111)	380~410	N	1×10^–7	410~440	—	290~320	—	^[78]
	Ag(111)	—	—	2×10^–7	380~430	—	295~320	300	^[79]
	Au(111)	300	24	1×10^–8	300~330	—	—	102~150	^[28]
	Ag(111)	300	24	1×10^–8	300~330	—	—	110~150	^[28]
	Li/Cu(111)	375	—	5×10^–7	413	10	—	—	^[88]
	HOPG	—	—	5×10^–7	400	—	—	100	^[89]
	Cu(100)	—	—	5×10^–8	423~503	—	—	—	^[90]
	Au(111)	—	—	5×10^–8	423~503	—	—	—	^[90]
[Omim][BF₄]	Cu(111)	423/523	N	5×10^–8	423~523	—	120	120	^[91]
[Omim]NTFI] [Omim][PF₆]	Ag(111)	370~430	24	8×10^–8/3×10^–7	403~413/ 428~443	—	—	90	^[92]
[Omim][PF₆] [PFBmim][PF₆]	Ag(111)	370~460	24	2×10^–7/5×10^–7	423~443/ 443~463	—	—	82	^[93]

离子液体	基底	除气温度^a T/K	除气时间^b t/h	压强 p/Pa	蒸发温度 T/K	蒸发时间^c t/min	基底温度 T/K	结构稳定温度T/K	参考文献
[BMP][FAP]	Au(111)	438~463	N	4×10^–8	450	10 s	298	210	^[69]
[BMP][NTFI]	Ag(111)	—	24	1×10^–8	373	3	—	100~180	^[71]
	TiO₂(110)	350	24	2×10^–8	453	5	—	80~380	^[72]
	Au(111)	360	N	5×10^–8	375	3	—	111~170	^[26]
	Ag(111)	360	N	5×10^–8	375	3	—	134~180	^[26]
	Au(111)	—	24	5×10^–8	375	3	—	100~225	^[73]
	Cu(111)	400	N	2×10^–8	450	—	200	80~200	^[74,76]
	HOPG(0001)	400	N	2×10^–8	450	—	—	100	^[75]
[Mmim][NTFI]	Ni(111)	400	N	1×10^–8	440	—	220±20	220	^[77]
	Au(111)	380~410	N	1×10^–7	410~440	—	290~320	—	^[78]
	Ag(111)	—	—	2×10^–7	380~430	—	295~320	300	^[79]
[Emim][NTFI]	Au(111)	350	24	1×10^–8	350~390	—	—	107~113	^[28]
	Ag(111)	350	24	1×10^–8	350~390	—	—	108~130	^[28]
	HOPG	—	—	1×10^–6	—	—	—	180~205	^[25]
	Ni(111)	353	12	1×10^–6	—	—	150	150~200	^[80]
	玻璃	—	—	6×10^–7	320	30	—	—	^[81]
	Au(110)	—	—	5×10^–8	423~523	—	128	311~323	^[82]
[Emim][OTF]	Pd(111)	—	—	2×10^–8	220	—	220	220	^[83]
	Au(111)	—	—	1×10^–7	440	—	298	—	^[84]
	Pd(111)	—	—	2×10^–8	300	—	298	300~380	^[85]
[Bmim][NTFI]	Al₂O₃/NiAl(110)	—	—	2×10^–8	425~475	N	—	298~323	^[86]
[Hmim][NTFI]	CeO₂(111)/CeO_2–_x	—	N	1×10^–8	385	—	160	—	^[87]
[Omim][NTFI]	Au(111)	380~410	N	1×10^–7	410~440	—	290~320	—	^[78]
	Ag(111)	—	—	2×10^–7	380~430	—	295~320	300	^[79]
	Au(111)	300	24	1×10^–8	300~330	—	—	102~150	^[28]
	Ag(111)	300	24	1×10^–8	300~330	—	—	110~150	^[28]
	Li/Cu(111)	375	—	5×10^–7	413	10	—	—	^[88]
	HOPG	—	—	5×10^–7	400	—	—	100	^[89]
	Cu(100)	—	—	5×10^–8	423~503	—	—	—	^[90]
	Au(111)	—	—	5×10^–8	423~503	—	—	—	^[90]
[Omim][BF₄]	Cu(111)	423/523	N	5×10^–8	423~523	—	120	120	^[91]
[Omim]NTFI] [Omim][PF₆]	Ag(111)	370~430	24	8×10^–8/3×10^–7	403~413/ 428~443	—	—	90	^[92]
[Omim][PF₆] [PFBmim][PF₆]	Ag(111)	370~460	24	2×10^–7/5×10^–7	423~443/ 443~463	—	—	82	^[93]

表2. 物理气相沉积法制备离子液体二维结构相关参数列表

Table 2. Preparation parameters for two-dimensional ionic liquids by physical vapor deposition method

表2. 物理气相沉积法制备离子液体二维结构相关参数列表

Table 2. Preparation parameters for two-dimensional ionic liquids by physical vapor deposition method

图5. (a) [BMP][NTFI]在Ag(111)上的两种稳定构型(球棍模型)及相应的STM模拟图像(UT=–1.35 V, 等值面=3×10–4 e/nm3). (b) 约100 K温度下, [BMP][NTFI]在Ag(111)表面有序二维(2D)晶相的高分辨STM图像(UT=–0.33 V, IT=150 pA), 右侧叠加的长条状和圆形图案代表阴离子和阳离子, 白色方框代表单胞大小, 左下角插图为STM结构的三维放大图[71]

Figure 5. (a) Ball-and-stick presentation of two stable configurations of the adsorbed IL ions together with the corresponding simulated STM images (UT=–1.35 V, isosurface value=3×10–4 e/nm3) of the adsorption structures of [BMP][NTFI] on Ag(111). (b) High-resolution STM images of the ordered two dimensional (2D) crystalline phase of [BMP][NTFI] on Ag(111) recorded at about 100 K (UT=–0.33 V, IT=150 pA). On the right-hand side, the anion and cations are labeled by the superimposed longish protrusions and dots, the unit cell is marked by the white square. The inset in the left lower corner shows a three-dimensional STM image with a magnified scale[71]

图6. [BMP][NTFI]在(a) HOPG(0001)、(b) TiO2(110)、(c, d) Cu(111)和(e, f) Au(111)基底上二维结构的STM图像[70,72⇓-74,76,95]

Figure 6. STM images of two-dimensional structures for [BMP][NTFI] on (a) HOPG(0001), (b) TiO2(110), (c, d) Cu (111) and (e, f) Au (111) substrates[70,72⇓-74,76,95]

图7. (a) [Mmim][NTFI]在Ni(111)表面不同覆盖率下的结构示意图. (b) IL在Au(111)表面单层结构示意图[77]

Figure 7. (a) Schematic diagram of low dimensional [Mmim][NTFI] structure at different coverage on the Ni(111). (b) Monolayer structure of IL on the Au(111) surface[77]

图8. (a) 在亚单层覆盖率下, [Emim][NTFI]二维结构在Au(111)表面两种晶相结构(标记为#2和#3的区域)共存的STM图像(T=107 K, UT=–1.28 V, IT=40 pA). (b) 二维(2D)晶相(图a中的#2区域)的不同畴区(T=113 K, UT=–1.28 V, IT=80 pA). (c) [Emim][NTFI]二维结构在Ag(111)表面二维晶相与二维玻璃相共存的STM图像(T=108 K, UT=–1.13 V, IT=60 pA). (d) 二维晶相结构的高分辨STM图像(T=117 K, UT=–0.97 V, IT=70 pA)[28]

Figure 8. (a) STM images of two-dimensional structures of [Emim]- [NTFI] on Au(111) surface at submonolayer coverage with two kinds of crystalline phases marked by #2 and #3 (T=107 K, UT=–1.28 V, IT=40 pA). (b) Various domains of 2D crystalline structure (#2) (T=113 K, UT=–1.28 V, IT=80 pA). (c) STM images of two-dimensional structures of [Emim][NTFI] on Ag(111) surface at monolayer coverage with 2D glass structure and 2D crystalline domains (T=108 K, UT=–1.13 V, IT=60 pA), (d) High resolution STM image of the 2D crystalline structure (T=117 K, UT=–0.97 V, IT=70 pA)[28]

图9. [Emim][OTf]在Pd(111)上的结构排列转变示意图[83]

Figure 9. Schematic diagram of structural alignment transition of [Emim][OTf] on Pd(111)[83]

图10. 在亚单层覆盖率下, [Omim][NTFI]二维结构在Au(111)和Ag(111)表面的STM图像. (a) 二维(2D)晶体结构(标记为1的区域), 二维玻璃结构(标记为2的区域)和裸露的Au(111)表面(标记为3的区域)共存(T=102 K, UT=–0.76 V, IT=50 pA). (b) 图(a)中黑色矩形区域对应的2D晶相的高分辨STM图像, (阳离子: 黑色圆形突起, 阴离子: 一对黑色椭圆长突起). 单胞结构用红色平行四边形表示(尺寸: (2.5±0.1) nm×(3.5±0.1) nm, 方向: 箭头1×箭头2), a和b代表阴离子所在列位置, 白色的数字3, 4代表阴离子, 黑色的数字3, 4代表阳离子(T=151 K, UT=–1.16 V, IT=70 pA). (c) 二维晶相结构(标记为1的区域)和二维玻璃结构(标记为2的区域)以及Ag(111)表面(标记为3的区域)共存的STM图像(T=110 K, UT=–1.16 V, IT=130 pA). (d) 图(c)中白色矩形对应的2D晶相的高分辨STM图像, (阳离子: 黑色圆形突起, 阴离子: 一对黑色椭圆长突起). 二维晶体结构的单胞用黑色平行四边形表示(尺寸: (2.0±0.1) nm×(2.2±0.1) nm, 方向: 黑线×虚线黑线, 角度为82°) (T=118 K, UT=–1.10 V, IT=90 pA)[28]

Figure 10. STM images of two-dimensional structures of [Omim][NTFI] on Au(111) and Ag(111) surfaces at sub-layer coverage: (a) 2D crystalline structure (marked by 1), 2D glass structure (marked by 2) and bare Au(111) surface (marked by 3) (T=102 K, UT=–0.76 V, IT=50 pA). (b) High resolution image of the 2D crystalline phase corresponding to the black rectangular in (a) (T=151 K, UT=–1.16 V, IT=70 pA). The size of the image corresponds to the black rectangular in (a), (cations: black round shaped protrusions, anions: pairs of black ellipse longish protrusions). The unit cell of the structure is indicated by a red parallelogram (size: (2.5±0.1) nm×(3.5±0.1) nm, directions: arrow 1×arrow 2), a and b represent the anion rows, white 3 and 4 are for anions while black 3 and 4 for cations (T=151 K, UT=–1.16 V, IT=70 pA). (c) 2D crystalline (marked by 1), 2D glass (marked by 2) structure and bare Ag(111) surface (marked by 3) (T=110 K, UT=–1.16 V, IT=130 pA). (d) High resolution image of the 2D crystalline structure corresponding to the white rectangle in (c), (cations: black round shaped protrusions, anions: pairs of black ellipse longish protrusions). The unit cell of the 2D crystalline structure is marked by a black parallelogram (dimension: (2.0±0.1) nm×(2.2±0.1) nm, directions: black line×dashed black line with the angle of 82°) (T=118 K, UT=–1.10 V, IT=90 pA)[28]

图11. (a) 室温下, 在Ag(111)基底表面, 将[Omim][PF6]逐步沉积到[Omim][NTFI]上的离子交换过程以及在370 K时[Omim][NTFI]的选择性解吸示意图. (b) 在90 K时, 将[Omim][PF6]沉积到[Omim][NTFI]上的加热过程示意图[92]

Figure 11. (a) Schematic diagram of the ion exchange process during step-wise deposition of [Omim][PF6] onto [Omim][NTFI] on Ag(111) at r.t. and the selective desorption of [Omim][NTFI] at 370 K. (b) Schematic for the heating experiment after the deposition of [Omim][PF6] to [Omim][NTFI] on Ag(111) at 90 K[92]

图12. 电喷雾电离沉积示意图[98]

Figure 12. Schematic diagram of electrospray ionization deposition[98]

图13. Au(111)表面的[BMP][NTFI]二维(2D)晶相结构的高分辨STM图像. (a) 单层结构. 单胞用黄色线条标记, 结构由圆形和长条状突起组成, 分别用白色圆形和椭圆标记, 对应阳离子和阴离子. 白色虚线标记Au(111)重构锯齿线(T=116 K, UT=–0.71 V, IT=–0.10 nA). (b) 亚单层结构. 单胞用白色线条标记, 圆形突起用黑点标记, 对应阳离子, 成对长突起用黑线标记, 对应阴离子(T=102 K, UT=–1.846 V, IT=–0.050 nA)[26,73]

Figure 13. High resolution STM images of the 2D crystalline structures for [BMP][NTFI] on Au(111). (a) Detail view of the structure in the monolayer regime. The unit cells are marked with yellow lines. Structures are composed of round shaped and longish protrusions, which are marked with white circles and ellipsoids, corresponding to cations and anions respectively. The dashed white lines mark the zig-zag lines of the Au(111) reconstruction (T=116 K, UT=–0.71 V, IT=–0.10 nA). (b) Detail view of the structure in the submonolayer regime. The unit cell is marked with white lines, the round shaped protrusions are marked with black dots for cations and the pairs of longish protrusions with black lines for anions (T=102 K, UT=–1.846 V, IT=–0.050 nA)[26,73]

图14. (A) Si(110)表面[Bmim][NTFI]AFM形貌图. (B) 在A图中标记点处获取的力-距离曲线. (C) A图中蓝色点所在区域获取的30条针尖-表面位移曲线统计分布图. 插图为Hertz模型拟合最表层离子液体弹性变形段获取的弹性模量[38]

Figure 14. (A) AFM topographic image of [Bmim][NTFI] on Si(110). (B) Representative force-distance curves at different locations as indicated in A. (C) Distribution of tip-surface separation values from 30 force curves collected on the blue region indicated in A. The insert shows the elastic modulus of the topmost terrace structure obtained by fitting the Hertz mode to the elastic compression section[38]

图15. [Emim][NTFI]在蓝宝石上的结构示意图以及实验和MD模拟获取的与厚度相关的离子电导率数据[29]

Figure 15. Schematic diagram of the structure of the [Emim][NTFI] on sapphire and comparison of the thickness-dependent ionic conductivity obtained by experiments and MD simulations[29]

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离子液体二维结构制备及其特性研究进展

Research Progress on the Preparation and Properties of Two Dimensional Structure of Ionic Liquids

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