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Progress in Chemistry 2020, Vol. 32 Issue (8): 1017-1048 DOI: 10.7536/PC200428 Previous Articles   Next Articles

• Review •

Goals and Major Scientific Issues in Condensed Matter Chemistry

Ruren Xu1,**(), Jihong Yu1, Wenfu Yan1   

  1. 1. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China
  • Received: Revised: Online: Published:
  • Contact: Ruren Xu
  • About author:
    ** e-mail:
  • Supported by:
    the National Natural Science Foundation of China(U1967215); the National Natural Science Foundation of China(21835002); the National Natural Science Foundation of China(21621001)
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The concept of condensed matter chemistry is proposed as a new scientific discipline. It studies the composition, the multi-level structure, properties and chemical reactions of matters in condensed states formed via stable adhesions. This compares to the classical chemistry, which studies more localized issues, namely the properties of basic particles like atoms, ions and molecules and their electron-moving reactions. In this article, we use examples from solid state matters to illustrate cutting-edge research issues related to(1) the multi-level structures,(2) chemical properties and reactions,(3) constructive chemistry, and(4) novel characterization techniques of condensed matters. In-depth discussions regarding key scientific questions of the new discipline are presented, to set a stage enabling us to reexamine the core scientific issues in the classical chemistry, namely chemical reactions, in the new and larger context and to study the relationships among multi-level structures of condensed matters, chemical properties and reactions, and construction rational synthesis and precision preparation for materials in condensed matter states. The goals are to develop theories of “condensed matter organization” and “chemical reactions”, leading to the full development of the science of condensed matter chemistry as well as condensed matter engineering.

Contents

1 Goals of condensed matter chemistry

2 Major scientific issues in condensed matter chemistry

2.1 Multi-level structures of condensed matter

2.2 Chemical properties and chemical reactions of condensed matter

2.2.1 Chemical reactions in multilevel structured atomic(ionic) crystalline matter

2.2.2 Chemical reactions in molecular crystalline coordination compounds

2.2.3 Chemical reactions in isomeric atomic crystal solid matter

2.2.4 Properties and chemical reactions in allotropes of(molecular and atomic crystals) solid matter

2.2.5 “State” - “state” reactions in atomic(ionic) and molecular crystals in solid matter

2.2.6 Chemical reactions between organic solid matter

2.2.7 Chemical reactions of crystalline polymorphs and amorphous forms in solid matter

2.2.8 Influence of multi-level structure on catalysis in solid matter

2.2.9 Influence of crystal intergrowth on catalysis in crystalline solid matter

2.2.10 Influence of polymorphs on catalysis in crystalline solid matter

2.3 Emerging scientific issues in the constructive chemistry of condensed matter

2.4 State-of-the-art characterization techniques for condensed matter

3 Conclusion and outlook

Key words: condensed state, solid state, multi-level structure, chemical reaction, catalysis, construction, characterization
Fig.1 Part of phase diagram of Fe-O(Dashed line indicates the stoichiometric composition of FeO)[5]
Table 1 Composition of Pr n O2 n -2 at varied temperatures[8]
Oxide n x in PrOx n at T/K T/K
Pr4O6(Pr2O3) 4 1.500 1.500~1.503 1273
Pr7O12(l) 7 1.714 1.713~1.719 973
Pr9O16(ζ) 9 1.778 1.776~1.778 773
Pr5O9(ε) 10 1.800 1.779~1.801 723
Pr11O20(δ) 11 1.818 1.817~1.820 703
Pr6O11(β) 12 1.833 1.831~1.836 673
Table 2 Loading and surface area of As-synthesized catalysts[33]
TiO2 support type Synthesis loading ICP loading(%) XANES loading(%) Surface area (m2/g) Au areal density in units of(111) monolayers a
anatase 13 13 10.0 b 225 0.12
anatase 6 5.2 n/a 225 0.051
anatase 3 2.8 n/a 225 0.027
brookite 13 3.3 2.7 b 106 0.069
rutile 13 14 11.9 b 77 0.39
rutile 6 2.9 n/a 77 0.083
P25 13 5.7 4.1 b 47 0.27
P25 13 7.2 8 47 0.34
P25 6.5 4.5 5 47 0.21
Fig.2 Chain-like structure of M7O12 containing vacancy pair(octahedrally coordinated metal atom is presented as MO6(Vo)2)[8]
Fig.3 Alternative stacking of metal chain along all(111) axes in c-type cubic-centered oxides[8]
Fig.4 The dependence of the ΔG on the temperature of the reactions (1) and (2)[9]
Fig.5 Mechanochemical decomposition of MBrO3, 1-NaBrO3, 2-KBrO3, 3-CBrO3, 4-RbBrO3 [9]
Fig.6 Lattice constant for the mono-chalcogenides of the rare earth elements[10]
Fig.7 The formation of 3D framework of [Fe(μ-atrz)3(BF4)2] by the linear 1D chain coordination polymer of [Fe(μ-atrz)(atrz)2(H2O)2]·4H2O(BF4)2 along the b-axis(counter anions, water molecules in the lattice and hydrogen atoms are omitted) via dehydration[14, 15]
Fig.8 CO oxidation activity over Au-TiO2 catalysts with different supports:(a) from the as-synthesized sample;(b) following treatment in 8% O2-He pretreated at 573 K for 30 min[33]
Fig.9 Phase transition of SiO2 at ambient pressure[37]
Fig.10 Phase diagram of BaO and SiO2 [38]
Fig.11 Structure of black phosphorus:(a) orthorhombic,(b) rhombohedral, and(c) cubic black phosphorus[39]
Fig.12 Phase relations in the BaO-TiO2 system for compositions with > 60 % mole fraction TiO2. Abbreviations and symbols used include: BT(BaTiO3); B6T17(Ba6Ti17O40); B4T13(Ba4Ti13O30); BT4(BaTi4O9); B2T9(Ba2Ti9O20); L(liquid);(·) solid phases, quenched;(o) melted, quenched[40, 41]
Fig.13 Diagonal cross section of triternary mutual system Ag,Pb‖Cl,Br-liquidus[42]
Fig.14 Diagonal cross section of triternary mutual system K,Na‖Cl,SO4-liquids[43]
Table 3 Diagonal cross section of triternary mutual system K,Na‖Cl,SO4 liquidus[43]
%
(KCl)2 		t° Твердые
Фазы		 %
(KCl)2 		t° Твердые
Фазы		 %
(KCl)2 		t° Твердые
Фазы
0 884 Na2SO4 25 624 ФазаX* 40 532 ФазаX*
5 824 ″ 27 608 ″ 45 540 KCl
10 772 ″ 30 594 ″ 50 564 ″
15 718 ″ 33 578 ″ 55 588 ″
18 690 ″ 36 560 ″ 65 635 ″
21 662 ″ 38 548 ″ 70 682 ″
Table 4 Nonvarint point and solid phase in(KCl)2-Na2SO4 [43]
t° %(KCl)2 Tвepдыe Фaзы
624 24.6 Na2SO4,Фaзa X
525 41.5 KCl,Фaзa X
Table 5 Eutectic temperature and composition, solid phase in(KCl)2-Na2SO4 [43]
Обозна-
чення нарнс.270		 t° %W Твердые Фазы
(KCl)2 (NaCl)2 Na2SO4 K2SO4
P1 534 25.5 13.5 61 - Na2SO4,Фаза X,NaCl
E 514 39 2.5 58.5 - NaCl,
Фаза X,KCl
P2 538 41.5 - 53 5.5 KCl,Фаза X,K2SO4
Table 6 Stabilization of unusual oxidation states of transition metals of the first raw under high oxygen pressures[47]
Element Oxidation state Electronic configuration Oxide
Cr Cr(Ⅴ) t 2 g 2 e g 0 La2LiV1- x Cr x O6
Fe Fe(Ⅳ) t 2 g 3 d z 2 1 d x 2 - y 2 0 A0.5La1.5Li0.5Fe0.5O4
A=Ca, Sr, Ba
(SrLa)M0.5Fe0.5O4
M=Mg, Zn
Fe Fe(Ⅴ) t 2 g 3 e g 0 La2LiFeO6
Co Co(Ⅲ) LS→HS
LS→HS		 LnCoO3
(Ln=La→Lu)
SrLnCoO4
Co Co(Ⅳ) t 2 g 6 e g 0 (Sr0.5La1.5)Li0.5Co0.5O4
Ni Ni(Ⅲ) t 2 g 6 σ * 1 LnNiO3(Ln=La→Lu)
SrLnNiO4
Cu Cu(Ⅳ) t 2 g 6 d z 2 2 d x 2 - y 2 2
t 2 g 6 σ * 2 		La2Li0.5Cu0.5O4
LaCuO3
SrLaCuO4
Fig.15 Phase relations involving BaFeO3- x . Stippled areas are single-phase regions for high- and low-temperature forms of BaFeO3- x . Oxygen isobars are shown as light lines with experimental points as open circles. Dashed lines indicate inferred relations[46]
Fig.16 Preparation of supramolecular materials via grinding the mixture of cis-[Pt(NO3)2(en)2](1b) and 4,4'-bpy(2) and cis-[Pd(NO3)2(en)2](1a) and triazine based ligand(4) at ambient temperature[56, 57]
Table 7 Solid-state reaction types[59]
Inclusion reactions
Condensation of carbonyls
Electron transfers
Cycloadditions
Proton transfers
Cycloreversions
Oxygen transfers
Substitutions with RX
Oxygenations
Aromatic substitutions
Hydrogenations
Cyclizations
Additions of RR’NH, H2O, ROH
Methylations
Additions of halogens and HX
Nitrations at N and C
Eliminations
Diazotizations
Rearrangement
Azocouplings
C-C bond formations
Sandmeyer reactions
Carboxylation with CO2
Cascade reactions
Table 8 Quantitatively formed azomethines by solid-solid reaction[66]
Ar Ar’ Reaction condition Yield/(%)
4-MePh 4-ClPh 6 h, r.t. 100
4-BrPh 2 h, r.t. 100
4-NO2Ph 24 h, r.t. 100
4-HOPh 6 h, r.t. 100
4-MeOPh 4-ClPh 6 h, r.t. 100
4-BrPh 6 h, r.t. 100
4-NO2Ph 24 h, 50 ℃ 100
4-ClPh 4-HOPh 6 h, r.t. 100
4-HOPh 4-ClPh 24 h, r.t. 100
4-NO2Ph 4-ClPh 36 h, r.t. 100
Fig.17 Mechanochemistry: reactions of fullerene[67]
Fig.18 Difference in the oxidation of 45 by mechanochemical activation and in solution phase[68]
Fig.19 (a) First synthesis of adamantoid cyclophosphazanes 59 facilitated by mechanochemical activation.(b) Initial unsuccessful attempts to prepare 59[68]
Fig.20 (a)One-dimensional linear tape and(b)crinkled(or zigzag) tape,(c) two dimensional sheet(or layer) and(d) three dimensional network(or framework) held together by the carboxylic acid dimer synthon[69]
Fig.21 Aqueous silicate structures identified in concentrated alkaline solution. Each line in the stick figures represents a Si-O-Si(siloxane) linkage. Of these 48 structures, 41 contain multiple chemically distinct Si sites, making them amenable to characterization by29Si-29Si COSY NMR spectroscopy. All the structural assignments are definitive except for species 6B, 6C, and 7A, for which they were unable to resolve the various isomeric forms[72]
Table 9 Effect of silicate ratio on the percentage of SiO2 in a given silicate ion[71]
Scheme 1 Pt/SiO2 catalyst prepared by direct reduction[78]
Scheme 2 The effect of SMSI on the catalytic behaviors of Pt/SiO2 catalysts in propane dehydrogenation[78]
Fig.22 The effect of reduction temperature in a H2 atmosphere on the activity of Pt/SiO2 catalysts[78]
Table 10 Physical properties and CO adsorption values of Pt/SiO2 catalysts[78]
Catalyst Surface area/
m2·g-1 		Average particle sizea/nm Mass ratio of Pt:Si O 2 b CO adsorptionc/mmol·g-1
SiO2 325 - -
Pt/SiO2_773 K H2 340 2.4±1.2 3.5/96.5 54.9
Pt/SiO2_1073 K H2 320 2.2±0.9 3.9/96.1 40.3
Pt/SiO2_1273 K H2 217 3.2±1.1 4.1/95.9 not detectable
Fig.23 Cluster models of(a) a E’s center, ≡Si·, at the silica surface and(b) a metal atom(Cu, Pd, Cs) adsorbed on the E’s center, ≡Si-M[79]
Scheme 3 Proposed reaction pathway for photocatalytic N2 fixation to NH3·H2O using MWO-1 UTNWs as a catalyst[92]
Fig.24 Topology of channels in(a) ZSM-5(MFI);(b) ZSM-11(MEL);(c) intergrowth of MFI and MEL with varied ratios[106]
Fig.25 Simulated XRPD patterns for the evaluation of MFI/MEL contribution of ZSM-5, composite-a, -b and -c, from 6° to 55° 2 h(quartz phase was not included in the simulation)[107]
Fig.26 Product selectivity of ZSM-5, composite-a, -b and -c. at 450 ℃ at a representative time on stream of 4 h. Propene is the dominant product. The product grouping was carried out in order to highlight the most relevant products in the MTA reaction. C4-C5 isomers: C4 are the 2-butene(cis and trans) and C5 are pentenes derivatives(1-, 2- and the corresponding cis and trans forms). C6-C8 isomers: comprises: hexene isomers, epatanes/eptenes, octanes/octanes with all their possible combinations of double bond in different position, cis and trans form and branched alkanes. C9+ isomers: include branched and unsaturated aromatics products either with alkyl chain or unsaturated branched substituents[107]
Fig.27 Catalytic behaviour of: ZSM-5(squares), composite-a(circles), composite-b(triangles), and composite-c(diamonds) versus time on stream at 450 ℃. Filled and open symbols correspond to conversion and selectivity to propene respectively[107]
Table 11 MFI and MEL contributions, relative crystallinity, micropore volume, surface area and crystallite size for ZSM-5, composite-a, -b and -c[107]
Material ZSM-5 ZSM-11 Relative crysrallinity Micropore volunm Surface area Crystallite size Si:Al ratio
MFI(%) MEL(%) (%) (mL·g-1) (m2·g-1) (μm)
ZSM-5 100 0 100 0.26 229 0.4 16
Composite-a 53 47 82 0.21 242 0.6 50
Composite-b 43 57 71 0.27 286 0.5 58
Composite-c 40 60 50 0.16 62 0.2 56
Fig.28 The RON values and the sulfur contents of the hydrogenated gasoline products over different catalysts[108]
Fig.29 The isomerization(ISO) selectivity over different catalysts[108]
Fig.30 The relationship of RON and the retentions of olefin over different catalysts[108]
Table 12 The hydro-upgrading results of FCC gasoline over different catalysts[108]
Items Catalyst series
Feedstock CoMo/AE-1 CoMo/AE-2 CoMo/AE-3 CoMo/AE-4 CoMo/AE-5 CoMo/AE-6 CoMo/AF CoMo/γ-Al2O3
Lumped composition of the liquid product(wt%)
n-Paraffin 6.0 12.5 11.1 13.8 10.7 11.2 11.1 11.4 13.0
i-Paraffin 36.6 47.1 47.8 50.8 51.3 52.7 48.6 43.3 47.3
Olefin 27.9 10.3 11.4 5.0 5.2 8.1 10.0 13.0 10.5
Naphthene 6.8 9.8 9.7 10.2 10.4 9.6 8.0 10.4 9.1
Aromatics 22.7 20.3 20.0 20.2 19.5 21.3 22.3 21.9 20.1
RON 90.2 88.6 88.9 87.9 88.5 89.7 89.3 90.1 88.0
ARON -1.6 -1.3 -2.3 -1.7 -0.5 -0.9 -0.1 -2.2
S(mg/L) 401 34.1 44.4 16.8 25.1 22.5 42.1 63.3 46.7
HDS(%) 91.5 88.9 96.1 93.7 94.6 89.5 84.2 88.3
Fig.31 The projections and channel stacking sequences of polymorphs A, B, and C along the a or b direction: the 12-ring channel stacking sequences are ABAB...(a), ABCABC...(b) and AA...(c) types, respectively[109]
Fig.32 Intrinsic activity of Ti-β and Ti-ITQ-17, expressed as turnover frequency number(mmol alkene converted/mmol Ti.h), on the epoxidation of different substrates with H2O2 [110]
Table 13 Cyclohexene and 1-hexene epoxidation over Ti-β and Ti-ITQ-17(Ti-PolC)[110]
Substrate catalyst Si/Ti Time Conversion % S % S % S % S
(min) (%of maximum) epoxide diola H2O2 TBHP
1-hexene Ti-β 59 45 20.1 97.0 2.6 89.9
1-hexene Ti-PolC 240 120 13 97.1 2.2 40.3
cyclohexene Ti-β 59 90 31.2 57.8 28.6 81.8
cyclohexene Ti-PolC 240 90 25.4 70.4 20.2 89.7
cyclohexeneb Ti-β 59 325 40.8 72.4 16.8 90.4
cyclohexeneb Ti-PolC 240 135 43.9 83.7 10.5 93.8
cyclohexene Ti-β 59 90 44.2 98.1 1.7 87.3
cyclohexene Ti-PolC 240 90 69.8 98.5 1.4 96.5
Table 14 Channel sizes and diffusion coefficients obtained from the molecular dynamics[111]
Structure Channel size(Å) <100>a Diffusion coefficient
(106 cm2·s-1) [001]		 2-MNb
(10.0×6.0×2.8 Å)		 2-AMN
(12.3×6.2×2.8 Å)		 1-AMN (10.3×8.1×4.1 Å)
Betac 6.2×7.2 5.5×5.5 21.71 10.44 3.90
ITQ-17 6.2×6.6 6.3×6.3 13.90 9.74 0.33
Table 15 Physicochemical characteristics of zeolites tested in the present work[111]
Sample Si/Gea (Si+Ge)/Ala Area Micropore Crystal Acidity(μmol py)c
BET Volumn Size Brönsted Lewis
(m2·g-1) (cm3·g-1) (μm)b 423 523 623 423 523 623
BEC-1 1.2 48 468 0.216 0.6~1.5×0.2×0.2 20 12 4 1 0 0
BEC-2 9.5 48 436 0.194 0.1~0.2 21 15 8 11 9 8
1.5~1×0.2×0.2
BEC-3 10.2 73 358 0.143 0.1~0.2 8 6 2 10 9 7
1.5~2.5×0.2×0.2
BETA - 50 484 0.192 0.3~0.5 23 20 7 10 7 6
Table 16 Acylation of 2-methoxynaphthalene with acetic anhydride over ITQ-17 in a batch reactor and comparison with Beta zeolitea[111]
Catalyst $r_{1-AMN}^b$ $R_{2-AMN}^b$ $r_{AMN}^b$ $S_{1-AMN}^c\\(M\%)$ $S_{2-AMN}^c\\(M\%)$ $S_{AMN}^c\\(M\%)$ X T2-MN 24 h $S_{1-AMN}^d\\(M\%)$ $S_{2-AMN}^d\\(M\%)$ $S_{AMN}^d\\(M\%)$ $S_{2-NOH}^d\\(M\%)$ $S_{2-dAMN}^d\\(M\%)$
(M%) (M%) (M%) (M%)d (M%) (M%) (M%) (M%) (M%)
BEC-1 15.38 19.39 0 44.2 55.8 0 28 35.7 62.9 1.4 0 0
BEC-2 26.37 21.28 0 55.3 44.7 0 67 44.7 49.8 4.8 0 0.7
BEC-3 38.44 16.14 0 70.4 29.6 0 52 61.4 34.5 3.5 0 0.5
BETA 54.46 41.74 4.24 54.2 41.6 4.2 90 32.1 54.7 11.5 0.4 1.3
Fig.33 Reaction scheme of the acylation of 2-MN with acetic anhydride over zeolites and possible alternative processes:(1) direct acylation;(2) intermolecular transacylation of 1-AMN with 2-MN;(3) protodeacylation of 1-AMN;(4) intramolecular transacylation of 1-AMN;(5) consecutive acylation of monoacylated products;(6) hydrolysis of the terminal O—C bond of 2-MN;(7) transalkylation of 2-MN[111]
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