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化学进展 2022, Vol. 34 Issue (7): 1454-1491 DOI: 10.7536/PC220325   后一篇

• 综述 •

凝聚液态水溶液中的化学反应

闫文付, 徐如人*()   

  1. 吉林大学无机合成与制备化学国家重点实验室 化学学院 长春 130012
  • 收稿日期:2022-12-20 修回日期:2022-03-25 出版日期:2022-07-24 发布日期:2022-06-20
  • 通讯作者: 徐如人
  • 基金资助:
    国家自然科学基金项目(U1967215)
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Chemical Reactions in Aqueous Solutions with Condensed Liquid State*

Wenfu Yan, Ruren Xu()   

  1. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University,Changchun 130012, China
  • Received:2022-12-20 Revised:2022-03-25 Online:2022-07-24 Published:2022-06-20
  • Contact: Ruren Xu
  • Supported by:
    National Natural Science Foundation of China(U1967215)

液态水是进行化学反应的最重要介质与溶剂之一,也是研究在凝聚(液)态中进行化学反应的主要对象。在不同的外界条件下(特别是极端条件下),液态水的组成、结构与性能会发生很大的变化,促使在其中进行的化学反应呈现不同的特点,因而形成了温和条件下、水热条件下(Hydrothermal condition)与超临界水热条件下(Supercritical water codition)三大类型反应的凝聚态化学。本文立足凝聚态,讨论了在温和(一般)条件下,液态水与水溶液的组成、结构与性能对发生于其中的化学反应(包括溶解与结晶反应、盐类复分解反应、酸碱反应、沉淀反应、成胶与晶化反应、水解反应、氧化-还原反应以及配位化学反应)的影响,包括对反应物存在状态与化学活性,化学反应的过程与机理,反应的中间与最后产物的组成、结构等造成的影响,以及产生的结果与规律等有关的反应化学。通过这些讨论我们提出应从凝聚态的角度看待发生于液态水溶液中的化学反应,并希望这种新视角对研究在其他类型液体(诸如有机溶剂、离子液体、分子熔体等)中进行的化学反应时有所帮助,同时能加强彼此间的交流、讨论与批判,协力为推动以液态为主要研究对象的凝聚态化学的研究与学科建设提供有益的基础。

关键词： 凝聚态, 液态, 多层次结构, 化学反应, 构筑

Liquid water is one of the most important media and solvent for chemical reactions, which is also the main object in scholarly investigation of the chemical reactions occurring in condensed (liquid) matter. The composition, structure, and characteristics of water may vary significantly under different conditions, especially under extreme conditions, which may change both the rates (kinetics) and favorability (thermodynamics) of individual chemical reactions in solution. Thus, the condensed matter chemistry under (normal) mild conditions, hydrothermal conditions, and supercritical water conditions may differ considerably. In this review, we discuss the influences of the composition, structure, and characteristics of liquid water and solution on the chemical reactions within, which includes the state and reactivity of the reactants, processes and mechanisms of reactions, compositions and structures of the intermediate and final products. Examples of these reactions are dissolution and crystallization, double decomposition reaction of salts, acid-base reaction, precipitation, gelation and crystallization, hydrolysis, redox reaction, and coordination reactions. In our discussions, we emphasize that it is essential to consider the chemical reactions occurring in aqueous solutions at the level of condensed matter physical science; and similarly it is also essential to investigate chemical reactions occurring in other types of liquids such as organic solvents, ionic liquids, and molecular substances in molten state. We well understand that this review will result in more in-depth discussions and possibly criticisms about the topics of condensed matter chemistry as well as our perspectives among our peer researchers, which will definitely advance this emerging science in liquids and possibly serve as a base for establishing the new discipline of condensed matter chemistry.

Contents

1 Introduction

1.1 Property and structure of liquid water

1.2 Composition and structure of aqueous solution

2 Dissolution and crystallization

2.1 dissolution and conversion of salts

2.2 Solubility under thermodynamics equilibrium state

2.3 Condensed matter chemistry in crystallization

3 Double decomposition reaction

4 Acid-base reaction

5 Precipitation reaction

5.1 Crystalline precipitation

5.2 Non-crystalline precipitation

5.3 Non-crystalline nickel borate

5.4 Silica gel and amorphous SiO2 precipitation

6 Gelation and crystallization

6.1 Polymerization of aluminosilicate

6.2 Hydrated aluminosilicate gel and crystallization of zeolites

7 Hydrolysis reaction

8 Redox reaction

8.1 Redox reactions of media water

8.2 pH and redox potential

8.3 Disproportionation reactions

8.4 Influence of precipitation on oxidation-reduction (redox) reactions

8.5 Influence of complexation on redox potential

8.6 Influence of trace amount of oxygen on oxidation-reduction (redox) reactions

8.7 Hydration of electron

9 Coordination reaction

10 Conclusion and outlook

Key words: condensed state, liquid state, multi-level structure, chemical reaction, construction
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图1 水的多面体结构模型:(a)五角十二面体(512); (b)十四面体(51262); (c)十五面体(51263)[3]
Fig. 1 Structures of some polyhedra for liquid water: (a) pentagonal dodecahedron (512), (b) 14-hedron (51262), and (c) 15-hedron (51263)[3]
图式1 MgSO4水溶液中主要物种的结构示意图[7]
Scheme 1 Schematic diagrams of the main species for aqueous MgSO4 solutions[7]
图2 水分子的极性结构以及溶解NaCl过程示意图
Fig. 2 Schematic drawing of the polar structure of H2O and the dissolution process of NaCl in aqueous solution.
图3 卤化物溶解焓与两种离子水合焓差值之间的关系:差值越大溶解过程中放热越强烈[15]
Fig. 3 The correlation between enthalpies of solution of halides and the differences between the hydration enthalpies of the ions. Dissolution is most exothermic when the difference is large[15]
图4 MgCl2-H2O二元体系多温溶解度相图[16]
Fig. 4 The phase diagram of MgCl2-H2O on solubility at various temperatures[16]
表1 MgCl2-H2O二元体系在不同温度时的浓度数据和固相组成[17]
Table 1 The concentration of MgCl2 in aqueous solution at various temperatures and the composition of the solid phase[17]
温度/℃ 液相组成MgCl2(质量分数)% 晶体固相组成 温度/℃ 液相组成MgCl2(质量分数)% 晶体固相组成
-10 11.7 冰 75 39.2 MgCl2·6H2O
-20 16.9 冰 100 42.2 MgCl2·6H2O
-33.5 21.4 冰+MgCl2·12H2O 116 46.5 MgCl2·6H2O+ MgCl2·4H2O
-25 24.2 MgCl2·12H2O 125 47.0 MgCl2·4H2O
-16.3 30.6 MgCl2·12H2O 150 48.8 MgCl2·4H2O
-16.7 32.2 MgCl2·12H2O+ MgCl2·8H2O 175 52.0 MgCl2·4H2O
-10 33.4 MgCl2·8H2O 181 55.7 MgCl2·4H2O+ MgCl2·2H2O
3.4 34.6 MgCl2·8H2O+ MgCl2·6H2O 200 57.5 MgCl2·2H2O
25 35.7 MgCl2·6H2O 250 63.0 MgCl2·2H2O
50 37.4 MgCl2·6H2O 300 67.8 MgCl2·2H2O
图5 MgCl2·12H2O 中的由[Mg(H2O)6]2+和[Cl(H2O)6]- 通过点共享形成的层状结构,四边形代表[Mg(H2O)6]2+,菱形代表[Cl(H2O)6]-。为了清晰起见,两个未被共享的边(即H2O)未画出[18]
Fig. 5 Layer formed from vertex-sharing [Mg(H2O)6]2+ and [Cl(H2O)6]- groups in MgCl2·12 H2O (diagrammatic). The squares represent [Mg(H2O)6]2+ and the rhombuses [Cl(H2O)6]- groups. Two (unshared) vertices of each octahedron are not shown[18]
表2 MxXy·zH2O型盐水合物的分类[21]
Table 2 A classification of salt hydrates MxXy·zH2O[21]
M fully hydrated M incompletely hydrated
z/xn excess H2O
Ⅰ
Ⅱ		 excess H2O
Ⅲ
Ⅳ







A		 2
9/6
6/6
7/6
1		 MgCl2·12H2O
FeBr2·9H2O
see text
NiSO4·7H2O
NaOH·7H2O




Sm(BrO3)3·9H2O
Nd(BrO3)3·9H2O
CaO2·8H2O
Sr(OH)2·8H2O
Zn(BrO3)3·6H2O
CoI2·6H2O
MgCl2·6H2O
AlCl3·6H2O
CrCl3·6H2O
Mg(ClO4)2·6H2O
BeSO4·4H2O











CoCl2·6H2O
NiCl2·6H2O
FeCl3·6H2O
CrCl3·6H2O




B		 5/6
3/4

2/3


7/12

1/2		 Na2SO4·10H2O






Na2CO3·10H2O


SrCl2·6H2O
KF·4H2O

Na2HAsO4·4H2O
NaOH·3.5H2O
LiClO4·3H2O		 CuSO4·5H2O


SnCl2·2H2O




FeF3·3H2O
CaCO3·6H2O
GdCl3·6H2O
FeF2·4H2O
FeCl2·4H2O
MnCl2·4H2O


CuSO4·3H2O






C		 4/9




1/4




1/6
1/8

1/9
1/12





















CdSO4· 8 3H2O












KF·2H2O, NaBr·2H2O
CoCl2·2H2O
NiCl2·2H2O
BaCl2·2H2O
SrCl2·2H2O
CaSO4·2H2O
LiOH·H2O
CuSO4·H2O
Li2SO4·H2O
Sr(OH)2·H2O
SrBr2·H2O
Na2CO3·H2O
图6 溶液状态图[24]
Fig. 6 State of solution[24]
图7 Na+、Mg2+‖Cl-、 SO 4 2 --H2O四元交互体系在0 ℃(a)[31]、25 ℃(b)、55 ℃(c)和75 ℃(d)的平衡溶解度相图[32]:Ast: Na2SO4·MgSO4·4H2O; Van: 3Na2SO4·MgSO4; Loe: 6Na2SO4·7MgSO4·15H2O; Bis: MgCl2·6H2O; S10: Na2SO4·10H2O; M1: MgSO4·H2O; M4: MgSO4·4H2O; M6: MgSO4·6H2O; M7: MgSO4·7H2O; 镁乳:MgSO4·H2O,其中含有NaCl和KCl
Fig. 7 The phase diagram of Na+, Mg2+‖Cl-, SO 4 2 --H2O on solubility at 0 ℃ (a)[31], 25 ℃ (b), 55 ℃ (c), and 75 ℃ (d). Ast: Na2SO4·MgSO4·4H2O; Van: 3Na2SO4·MgSO4; Loe: 6Na2SO4·7MgSO4·15H2O; Bis: MgCl2·6H2O; S10: Na2SO4·10H2O; M1: MgSO4·H2O; M4: MgSO4·4H2O; M6: MgSO4·6H2O; M7: MgSO4·7H2O; milk of magnesia:MgSO4·H2O, containing NaCl and KCl[32]
图8 四元体系(Na+、Mg2+‖Cl-、 SO 4 2 --H2O)在35 ℃时介稳相图(实线)与稳定相图(虚线)[33]
Fig. 8 The stablephase (solid line) and meta-stable phase (dash line) diagram of the Na+, Mg2+‖Cl-, SO 4 2 -―H2O system at 35 ℃[33]
表3 图8中缩写所代表的化学式和中文名[33]
Table 3 The formula and Chinese name of the abbreviations in Fig. 8[33]
缩写 化学式 中文名
Ha NaCl 氯化钠
Th Na2SO4 芒硝
Ast Na2SO4·MgSO4·4H2O 白钠镁矾
Eps MgSO4·7H2O 泻利盐
Ko Na2SO4·MgSO4·5H2O 孔矾钠石
Hex MgSO4·6H2O 六水泻盐
Tet MgSO4·4H2O 四水泻盐
Bis MgCl2·6H2O 水氯镁石
图9 水合氢离子H3O+的结构图[37]
Fig. 9 The schematic drawing of the structure of H3 O +[37]
图10 Eigen阳离子H9O4+的结构图[37]
Fig. 10 The schematic drawing of the structure of Eigen cation of H9O4+[37]
图11 不同pH值的磷酸溶液中的物种分布[56]
Fig. 11 The distribution diagram for the various forms of the triprotic acid phosphoric acid in water, as a function of pH[56]
图式2 酸性水溶液中的缩聚反应
Scheme 2 Polycondensation reaction in aeidic aqueous solution
图12 B2O3-H2O相图[63]
Fig. 12 Phase diagram for the B2O3-H2O system[63]
图13 H3BO3的层状结构,虚线表示O—H…O键[64]
Fig. 13 Portion of a layer of H3BO3. Broken lines indicate O—H…O bonds[64]
图14 结晶性偏硼酸的一种层状结构中B3O3(OH)3分子的排列以及其环状(B3O6)3-基本结构单元[63]
Fig. 14 Arrangement of B3O3(OH)3 molecules in a layer of one form of crystalline metaboric acid and the structure of cyclic (B3O63-[63]
图式3 [B3O3(OH)4]-和[B4O5(OH)4]2-的结构
Scheme 3 The structure [B3O3(OH)4]- and [B4O5(OH)4]2-
图15 羟化硼酸根和/或多聚硼酸根中的环状B-O体系,a、b、c的下角标指环外的配位O原子,分子式根据该结构单元处于3D结构中时计算得到[66]
Fig. 15 Cyclic boron-oxygen sysems in hydroxyborates and/or polyborates. The subscript is the number of extra-annular O atoms. The formula shows the composition of the 3D anion formed if all of these are shared with other similar units[66]
图16 H3PO4晶体中的氢键[36]
Fig. 16 The hydrogen bonds in crystalline H3PO4[36]
图17 KH2PO4投影在基面上的部分结构(省略了K+)。虚线表示将PO4四面体连接成无限三维网络的氢键[67]
Fig. 17 Part of the structure of KH2PO4 projected on to the basal plane (K+ ions omitted). The broken lines represent hydrogen bonds which link the PO4 tetrahedra into an infinite 3-dimensional network[67]
表4 第III B族元素氢氧化物的溶度积[69]
Table 4 The solubility product of the hydroxides of IIIB group[69]
M3+ radius (pm) Ksp pKsp
SC(OH)3 81 2.22×10-31 30.65
Y(OH)3 83 8.62×10-21 20.06
Yb(OH)3 86 2.5×10-24 23.06
Lu(OH)3 85 1.9×10-24 23.72
图18 Sc(OH)3的晶体结构[21]
Fig. 18 The crystal structure of Sc(OH)3[21]
图19 无定形硼酸镍的局部结构图[77]
Fig. 19 Local structure diagram of amorphous nickel borate[77]
图20 多聚硼酸根离子在不同pH水溶液中的分布[76]
Fig. 20 The distribution of polyborates in the aqueous solution with various pHs[76]
图21 几种SiO2基本胶粒结合方式示意图:(a) 硅溶胶; (b) 硅凝胶; (c) 无定形SiO2粉末[62]
Fig. 21 (a) silica sol; (b) silica gel; (c) silica powder[62]
图22 SiO2的聚合行为。在碱性溶液(pH=7~10)但包含盐时(B),随着胶粒间的自发聚集其尺寸变大;而在pH<7(酸性溶液)或在pH=7~10但同时含有盐时(A),胶粒会聚集成三维网格结构并生成凝胶[78]
Fig. 22 Polymerization behavior of silica. In basic solution (B) particles in sol grow in size with decrease in numbers: in acid solution or in presence of flocculating salts (A), particles aggregate into three-dimensinal networks and form gels[78]
图23 碱性硅溶胶的胶团结构及双电层示意图。δ为紧密层;Δ为扩散层;ϕo为总电位;ζ为电动电位;- - -为表面Si-O基团;+为Na+等阳离子;-为OH-等阴离子;m, x, y, z皆为正整数[79]
Fig. 23 Schematical illustration of the structure and distatic-charge-layer of colloidal particle of alkali silica sol. δ: compact layer;Δ: diffuse layer; ϕo: total potential; ζ: electrokinetic potential; - - -: surface Si-O groups; +: cations such as Na+;-: anions such as OH-; m, x, y, z: integral number[79]
图24 硅溶胶胶凝成凝胶过程中的胶粒间键的形成[62]
Fig. 24 Bond formation between silica particles. With little or no charge repulsion, collision results in formation of interparticle siloxane bonds, catalyzed by base. Once bonded, the particles grow together[62]
表5 硅凝胶胶粒堆积的配位数与密度的关系[80]
Table 5 Correlation between the stacking density and coordination number[80]
Coordination number (C.N.) Stacking density (S)
12 0.7405
6 0.5236
4 0.123~0.338
3 0.056~0.185
表6 硅凝胶孔体积与堆积密度的关系[81]
Table 6 Correlation between the pore volume and stacking density of SiO2 gel[81]
Samples of
SiO2 gel		 Specific surface area (m2/g) Pore volume
(mL/g)		 SiO2 density H2
displacement method		 Stacking density (S) Mean diameter
of micropore(Å)		 Mean diameter of
colloidal particles(Å)
1 344 0.870 2.32 0.331 92 75
2 657 0.348 2.35 0.522 21 29
3 248 0.612 2.32 0.414 73 81
4 478 0.575 2.15 0.443 41 48
图25 配位数为3的SiO2凝胶结构[82]
Fig. 25 Packing of spheres with coordination number of three[82]
图26 配位数为3,2,2,3的SiO2凝胶结构。黑球同一对白球相邻后再与另外三个黑球相邻[83]
Fig. 26 Packing of spheres with coordination numbers of 3, 2, 2, 3. Black spheres touch three others[83]
图27 不同浓度硅酸的胶凝时间和pH,硅酸浓度:(1) 0.0582 M;(2) 0.0713 M;(3) 0.0855 M;(4) 0.113 M;(5) 0.129 M;(6) 0.194 M[60]
Fig. 27 The gelation time and pH of the solution with various silica concentrations (1) 0.0582 M; (2) 0.0713 M; (3) 0.0855 M; (4) 0.113 M; (5) 0.129 M; (6) 0.194 M[60]
图28 Silicalite-1结构示意图及沿[010]方向观察(a)和沿[100]方向观察(b)模板剂在孔道中的位置[84]
Fig. 28 The schematic drawing of the structure of silicalite-1 (Si-ZSM-5) and the position of the template of TPA+ in the channels viewed along the direction of [010] (a) and [100] (b)[84]
图29 Na2O-Al2O3-SiO2-H2O体系凝胶相图(85%H2O)[89]
Fig. 29 Component correlations in initial Na-aluminosilicate gels (starred circles); in gel skeletons washed free of excess alkali (open circles); in gel liquid phases (black circles) in mole percent[89]
表7 硅铝凝胶组成与晶化产物NaA、NaX、NaY型沸石组成与结构[90,91]
Table 7 Molar composition of the initial mixtures for the crystallization of NaA, NaX, and NaY and the composition and structure type of the corresponding products[90,91]
分子筛 结构类型 结构中Si/Al 晶体组成 硅-铝水凝胶组成
NaA Linde Type A Si(50), Al(50) Na2O·Al2O3·2SiO2 3.165Na2O∶Al2O3∶1.926SiO2∶128 H2O
NaX Linde Type X Si(55), Al(45) NaAlO2·1.24SiO2 5.5Na2O∶1.65K2O∶Al2O3∶2.2SiO2∶122H2O
NaY Linde Type Y Si(71), Al(29) NaAlO2·2.43SiO2 4.62Na2O∶Al2O3∶10SiO2∶180H2O
图30 NaA型沸石的晶体结构[92]
Fig. 30 The crystal structure of NaA (LTA) zeolite[92]
图31 NaX与NaY型(FAU)沸石的晶体结构[93]
Fig. 31 The crystal structure of NaX and NaY (FAU) zeolite[93]
图32 具有球形对称性(a)、圆柱形对称性(b)和极化导致四面体电荷分布状态的OH-(c),以及导致三种OH-结构状态的对应的金属离子和其极化指数[95]
Fig. 32 The OH- with effective spherical symmetry (a), cylindrical symmetry (b), or polarized so that tetrahedral charge distributin is developed (c) and the corresponding cations with different polarizing power[95]
图33 理想情况下Al(OH)3中的层结构,圆圈代表位于Al(带阴影的小圆圈)平面上侧和下侧的OH基团[97]
Fig. 33 Part of a layer of Al(OH)3 (idealized). The heavy and light open circles represent OH groups above and below the plane of the Al atoms (shaded)[97]
图34 Al(OH)3沿平行于层的方向的结构示意图,显示了不同层之间的OH基团的不同堆垛情形[98]
Fig. 34 The structure of Al(OH)3, viewed in a direction parallel to the layers, to illustrate the difference in packing of OH groups of different layers[98]
图35 (a)水铝石α-AlO(OH)和(b)纤铁矿γ-FeO(OH)的结构正视图[99]
Fig. 35 Elevations of (a) the α-AlO(OH), diaspore, (b) the γ-FeO(OH), lepidocrocite, structures[99]
图36 水铝石α-AlO(OH)结构中O和OH基团的空间位置关系[99]
Fig. 36 The spatial correlation between O and OH group in the structure of α-AlO(OH), diaspore[99]
图37 水的还原电位随pH的变化:两条斜线分别为两个电对(O2/H2O和H+/H2)的电位,是热力学上水稳定的上限和下限[100]
Fig. 37 The variation of the reduction potentials of water with pH. The sloping lines defi ning the upper and lower limits of thermodynamic water stability are the potentials for the O2/H2O and H+/H2 couples, respectively. The central zone represents the stability range of natural waters[100]
图38 铬体系的pH-电位图[101]
Fig. 38 The variation of the reduction potentials of Cr-water system with pH[101]
图39 As和I体系的E-pH图[102]
Fig. 39 The variation of the reduction potentials of As-water system with pH[102]
图40 热力学循环。该循环示出配体L的存在如何改变Mv+/M(v-1)+的标准电极电位[103]
Fig. 40 Thermodynamic cycle showing how the standard potential of the couple Mv+/M(v-1)+ is altered by the presence of a ligand L[103]
图41 水合电子的结构示意图[106]
Fig. 41 Diagrammatic representation of a hydrated electron[106]
表8 反应[M(H2O)n]m+ + L ↔ [M(L)(H2O)n-1]m+ + H2O的形成常数[107]
Table 8 Formation constants for the reaction [M(H2O)n]m+ + L ↔ [M(L)(H2O)n-1]m+ + H2O[107]
Ion Ligand Kf logKf Ion Ligand Kf logKf
Mg2+ NH3 1.7 0.23 Pd2+ Cl- 1.25×105 6.1
Ca2+ NH3 0.64 -0.2 Na+ SCN- 1.2×104 4.08
Ni2+ NH3 525 2.72 Cr3+ SCN- 1.2×103 3.08
Cu+ NH3 8.50×105 5.93 Fe3+ SCN- 234 2.37
Cu2+ NH3 2.0×104 4.31 Co2+ SCN- 11.5 1.06
Hg2+ NH3 6.3×108 8.8 Fe2+ pyridine 5.13 0.71
Rb+ Cl- 0.17 -0.77 Zn2+ pyridine 8.91 0.95
Mg2+ Cl- 4.17 0.62 Cu2+ pyridine 331 2.52
Cr3+ Cl- 7.24 0.86 Ag+ pyridine 93 1.97
Co2+ Cl- 4.90 0.69
表9 Ni(Ⅱ)氨配合物[Ni(NH3)n(H2O ) 6 - n]2+的形成常数[108]
Table 9 Formation constants of Ni(Ⅱ) ammines, [Ni(NH3)n(H2O ) 6 - n]2+[108]
n Kf lgKf Kn/Kn-1(experimental) Kn/Kn-1(statistical)*
1 525 2.72
2 148 2.17 0.28 0.42
3 45.7 1.66 0.31 0.53
4 13.2 1.12 0.29 0.56
5 4.7 0.63 0.35 0.53
6 1.1 0.03 0.23 0.42
图42 水合配合物中H2O分子交换的特征寿命[109]
Fig. 42 Characteristic lifetimes for exchange of water molecules in aqua complexes[109]
图43 在不同溶剂中合成[RhX2(py)4 ] + [ 113 ]
Fig. 43 Synthesis of [RhX2(py)4]+ in various solvents[113]
图44 水-乙醇溶剂中电子转移催化合成trans-[RhCl2(py)4]+的可能机理[113]
Fig. 44 The possible mechanism for the catalytic synthesis of trans-[RhCl2(py)4]+ via electron transfer in water-ethanol solution[113]
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摘要

凝聚液态水溶液中的化学反应