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化学进展 2019, Vol. 31 Issue (2/3): 394-412 DOI: 10.7536/PC180505 前一篇   后一篇

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层状双氢氧化物（LDHs）的合成与应用

Saba Jamil1, Afaaf Rahat Alvi1, Shanza Rauf Khan1, Muhammad Ramzan Saeed Ashraf Janjua2,*()   

  • 收稿日期:2018-05-08 出版日期:2019-02-15 发布日期:2018-10-22
  • 通讯作者: Muhammad Ramzan Saeed Ashraf Janjua
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Layered Double Hydroxides(LDHs): Synthesis & Applications

Saba Jamil1, Afaaf Rahat Alvi1, Shanza Rauf Khan1, Muhammad Ramzan Saeed Ashraf Janjua2,*()   

  1. 1. Department of Chemistry, University of Agriculture, Faisalabad 38000, Pakistan
    2. Department of Chemistry, King Fahd University of Petroleum and Minerals, Dhahran 31261, Saudi Arabia
  • Received:2018-05-08 Online:2019-02-15 Published:2018-10-22
  • Contact: Muhammad Ramzan Saeed Ashraf Janjua
  • About author:
    * E-mail:

Layered double hydroxides, a class of anionic clays possessing sandwich like structure in which negative anions are sandwiched into positively charged metal layers in a repeating manner, have been studied extensively. Layered double hydroxides could be fabricated with combination of different divalent(Cd2+, Mn2+, Fe2+, Pb2+) and trivalent(Al3+, Cr3+, Fe3+) metals and layered arrangement imparts unique properties such as adsorption properties and catalytic properties in these compounds. Exciting feature of these compounds is the memory effect. There are a number of methods to synthesize these layered compounds, such as co-precipitation, hydrothermal, sol-gel, urea hydrolysis, etc. The synthesized LDHs can be characterized morphologically and compositionally i.e. scanning electron microscopy, transmission electron microscopy, powder X-Ray diffraction, Mossbauer spectroscopy, thermogravimetric analysis, XPS, etc. The wonderful feature of layered double hydroxides is the pliancy of interlayer space enabling them to accommodate various anionic species, and high surface area making them efficient in numerous applications such as adsorbents, anion exchange, catalysts, and biological compatible.

Key words: layered double hydroxides(LDHs), application
()
Fig.1 Schematic representation of LDH structure[20]
Fig.2 Association of divalent and trivalent metallic cations in LDHs.(◆: monovalent- tetravalent)[22]
Fig.3 Schematic illustration of the possible delamination mechanism for LDHs in formamide[30].
Fig.4 Schematic representation of memory effect[33]
Fig.5 Adsorption of dicamba on calcined-LDH as functions of calcined-LDH concentration under a fixed dicamba concentration(1.36 mmol·dm-3)[34]
Fig.6 Effect of contact time on the uptake of Brilliant Blue R(BBR) by layered double hydroxides(LDHs) and calcined LDHs(CLDHs) at different initial concentrations[43]
Fig.7 Sorption isotherms for Brilliant Blue R(BBR) sorption by layered double hydroxides(LDHs) and calcined LDHs(CLDHs)[43]
Fig.8 Temperature dependent susceptibility plot χT vs T[59]
Fig.9 Schematic representation of spin frustration[62]
Table 1 Structural formula of some natural layered double hydroxides[63,21]
Mineral Structural Formula Intercalated ion Cell Parameters(?) Space Group
Fougerite Fe42+Fe23+(OH)12[CO3]·3H2O OH-, Cl-, CO32- are possible a=3.17~3.18
c=22.7~22.9		 R$\bar{3}$m
Meixnerite [Mg6Al2(OH)16][(OH-)2.4H2O] OH- a=3.046 c=22.93 R$\bar{3}$m
Zincowoodwardite Zn1-xAlx(OH)2[SO4]x/2·nH2O
x<0.5, n<3x/2		 SO42- a=3.063 c=8.91 and
a=3.065 c=25.45		 P$\bar{3}$m and R$\bar{3}$m
Hydrotalcite [Mg6Al2(OH)16][(CO32-)·4H2O] CO32- a=6.13 c=46.15 R$\bar{3}$m
Pyroaurite [Mg6Fe3+(OH)16][(CO32-)·4H2O] CO32- a=6.19 c=46.54 R$\bar{3}$m
M?ssbauerite Fe63+O4(OH)8[CO3]·3H2O CO32- a=3.07 c=22.25 R$\bar{3}$m
Charmarite Mn4Al2(OH)12[CO3]·3H2O CO32- a=10.98 c=15.10 P6322
Fig.10 Experimental device for the preparation of LDHs by the co-precipitation method[22]
Fig.11 PXRD pattern for CaAl-LDH[67]
Fig.12 SEM micrograph of Ni-Ti-CO3 LDH(Ni/Ti=3)[68]
Fig.13 The SEM micrographs of the(a) ZnAl-4,(b) CZnAl-4-300 C and(c) CZnAl-4-500 C sample. The arrows in the left figures indicate where the enlargements(in the right figures) were taken. The marked spots(in the right figures) indicate the part taken for the EDX measurements[69]
Fig.14 SEM images of hydrotalcite samples hydrothermally treated at 160 and 180 ℃ for various times[71]
Fig.15 TEM images of NiAl LDH synthesized at different pH values.(a)5.5;(b)8.5;(c)10.0[75]
Fig.16 Anion exchange process[80]
Fig.17 SEM micrographs of(A)unmodified LDH,(B)LDH-laurate,(C)LDH-SDS,(D)=LDH-SDBS; and(E)LDH-BEHP(the magnification bar indicates 2 μm length)[14]
Fig.18 Scanning electron micrographs of Mg-Al hydrotalcites synthesized by urea hydrolysis[83]
Fig.19 SEM image of [MgAl-CO3] product synthesized by the urea method in water/ethylene glycol(1/4)[84]
Fig.20 Pore size distribution of the uncalcined Mg/Al, Ga, in LDHs[94]
Fig.21 SEM images of the NiAl-LDH/paper film at(A) low magnification and(B) high magnification; the MgAl-LDH/paper film at(C) low magnification and(D) high magnification[89]
Fig.22 TEM images of sol-gel LDHs:(A) MgAl,(B) NiAl-A,(C) NiCoAl,(D) NiAl-N
Fig.23 Adsorption of methylene orange on Mg/Al layered double hydroxide[107]
Table 2 A brief literature of layered double hydroxide with different metal combinations
Metals-anion Preparation methods Charac. techniques ref
Ca-Al-NO3 Co-precipitation PXRD, FTIR 96
Co-Fe-OH
Co-Fe-OH/CO32- (pyroaurite group)		 Topochemical synthesis
Co-precipitation method		 XRD, SEM, TEM, AFM
XRD, FTIR, Mossbauer spectroscopy, DTA		 97
98
Co-La-CH3COO- hydrogen peroxide catalyzed hydrolysis reaction FTIR, PXRD, TGA, PL spectroscopy 99
Cu-Al- CO32- Hydrothermal approach FTIR, PXRD, TGA 100
Zn-Cr-Cl-/CO32-/NO3- Co-precipitation UV-VIS analysis, PXRD, FTIR 101, 102
Zn-Ti-NO3
Zn-Al-CO3
Zn-Al-CO32-/NO3-		 Co-precipitation
Co-precipitation
Co-precipitation at low supersaturation		 TEM, SEM, PXRD, XPS
SEM, TGA, PXRD, TEM
SEM, XRD, EDX, IR, TG/DTG		 103
56
104
Ni-Fe-Cl Topochemical synthesis SEM, TEM, PXRD, XPS, FTIR 105
Mn-Al-CO32-/NO3-/SO42-/Cl- Co-precipitation PXRD, FTIR, DTA/TG, SEM 106
NiTi-CO32- Co-precipitation at high supersaturation PXRD, SEM, ICP-AES, FTIR 68
Mg-Al-CO32- Hydrothermal approach
Urea hydrolysis		 SEM, XRD, TGA, FTIR
XRD, FTIR, BET		 71, 72,
84, 83
Zn-Al LDH films Urea hydrolysis
Sol-gel route		 XRD, SEM, TEM
XRD, SEM		 81
89
Ni-Al/Mg-Al-CO32- Sol-Gel method XRD, SEM, TEM, HRTEM 90
Zn-Al LDH Sol-gel method XRD, TG-DSC 91
Mg-Al/Ga/In Sol-gel method FTIR, XRD, DRIFT 94
Ni-Co-Al/Mg-Ni-Al Sol-gel method XRD, TEM, TGA-DTA 95
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