Abstract:Layered double hydroxides (LDHs), a typical layered inorganic cationic material, have been widely studied as ion‐exchanger, catalyst and polymer additives. The past few decades have seen rapidly increasing interest in non‐LDH type 2‐dimensional inorganic cationic frameworks. Their novel properties derived from structural and compositional diversity cast a light on the field where LDHs show limited performance. This minireview will discuss the structure, synthesis and applications including anion‐exchange and c… Show more
“…LYH-Br belongs to a new family of anion-exchangeable layered metal hydroxides, exhibiting various potential applications in catalysis, − adsorption, , luminescence, − etc. − LYH-Br was proposed to adopt the crystal structure of LYbH-Cl (Yb 4 (OH) 10 Cl 2 ·3H 2 O), and its unit cell parameters and atomic coordinates were obtained by a combination of 1D and 2D 89 Y solid-state NMR, PXRD, and DFT methods . As Figure illustrates, LYH-Br consists of positively charged yttrium hydroxide layers and intercalated charge-balancing anions.…”
Hydrous materials such as clays, cements, hydroxyapatite, and metal hydroxides have been known and extensively used since antiquity. However, experimental elucidation of hydrogen in hydrous materials remains challenging due to the intrinsic insensitivity, limited accessibility, sample damage, or poor spectral resolution of many characterization methods. 1 H solid-state NMR spectroscopy has evolved into an ideal site-specific characterization tool of hydrogen-containing materials, but its current application in hydrous materials is hampered by the low resolution of 1 H NMR spectra in the solid state due to the presence of intense dipolar coupling networks and a narrow 1 H chemical shift range. Herein, a significant advance in the characterization of hydrogens in hydrous materials is reported. A combination of magic-angle spinning (MAS) NMR, moderate 2 H substitution, and high magnetic fields has unlocked the capacity of identifying many chemically similar while crystallographically distinct hydrogen sites in a prototypical hydrous material Y 4 (OH) 10 Br 2 •3H 2 O (LYH-Br) by 1D 1 H solid-state NMR experiments. 1 H NMR peaks were first tentatively assigned in accordance with the density functional theory (DFT) calculation results, and the assignment was further refined by 2D 1 H− 89 Y heteronuclear correlation (HETCOR) and 1 H− 1 H doublequantum (DQ) MAS NMR data. The order of 1 H chemical shift (δ iso ) values provides valuable information on the relative strength of hydrogen bond for ten hydroxide hydrogen sites. The power of very high spectral resolution is further described by observing all triple-quantum (TQ) coherences in the 2D 1 H− 1 H TQ MAS NMR spectrum, in which all spatial proximities among three hydrogen sites are resolved. This demonstration of the very high spectral resolution obtained in 1D and 2D 1 H solid-state NMR experiments illustrates how scientists in various communities can now study the multiple hydrous species of hydrous materials and obtain previously inaccessible fine structural information.
“…LYH-Br belongs to a new family of anion-exchangeable layered metal hydroxides, exhibiting various potential applications in catalysis, − adsorption, , luminescence, − etc. − LYH-Br was proposed to adopt the crystal structure of LYbH-Cl (Yb 4 (OH) 10 Cl 2 ·3H 2 O), and its unit cell parameters and atomic coordinates were obtained by a combination of 1D and 2D 89 Y solid-state NMR, PXRD, and DFT methods . As Figure illustrates, LYH-Br consists of positively charged yttrium hydroxide layers and intercalated charge-balancing anions.…”
Hydrous materials such as clays, cements, hydroxyapatite, and metal hydroxides have been known and extensively used since antiquity. However, experimental elucidation of hydrogen in hydrous materials remains challenging due to the intrinsic insensitivity, limited accessibility, sample damage, or poor spectral resolution of many characterization methods. 1 H solid-state NMR spectroscopy has evolved into an ideal site-specific characterization tool of hydrogen-containing materials, but its current application in hydrous materials is hampered by the low resolution of 1 H NMR spectra in the solid state due to the presence of intense dipolar coupling networks and a narrow 1 H chemical shift range. Herein, a significant advance in the characterization of hydrogens in hydrous materials is reported. A combination of magic-angle spinning (MAS) NMR, moderate 2 H substitution, and high magnetic fields has unlocked the capacity of identifying many chemically similar while crystallographically distinct hydrogen sites in a prototypical hydrous material Y 4 (OH) 10 Br 2 •3H 2 O (LYH-Br) by 1D 1 H solid-state NMR experiments. 1 H NMR peaks were first tentatively assigned in accordance with the density functional theory (DFT) calculation results, and the assignment was further refined by 2D 1 H− 89 Y heteronuclear correlation (HETCOR) and 1 H− 1 H doublequantum (DQ) MAS NMR data. The order of 1 H chemical shift (δ iso ) values provides valuable information on the relative strength of hydrogen bond for ten hydroxide hydrogen sites. The power of very high spectral resolution is further described by observing all triple-quantum (TQ) coherences in the 2D 1 H− 1 H TQ MAS NMR spectrum, in which all spatial proximities among three hydrogen sites are resolved. This demonstration of the very high spectral resolution obtained in 1D and 2D 1 H solid-state NMR experiments illustrates how scientists in various communities can now study the multiple hydrous species of hydrous materials and obtain previously inaccessible fine structural information.
“…To address these shortcomings, a series of cationic inorganic frameworks exhibiting enhanced thermal and hydrolytic stability has been prepared. , Notably, layered double hydroxides (LDHs) consisting of cationic brucite-type layers charge balanced by interlayer anions have received extensive attention as the next generation of inorganic anion exchangers. , LDHs have shown excellent removal efficiency for a variety of harmful oxyanions including chromate, phosphate, arsenate, and selenate . However, high-temperature calcination (usually at or above 450 °C) is usually required before their usage, which is a heavy energy consumption process .…”
Water pollutants
existing in their oxyanion forms have high solubility
and environmental mobility. To capture these anionic pollutants, cost-effective
inorganic materials with cationic frameworks and outstanding removal
performance are ideal adsorbents. Herein, we report that two-dimensional
(2D) cationic aluminoborate BAC(10) sets a new paradigm for highly
selective and efficient capture of Cr(VI) and other oxyanions from
aqueous solution. The structure of Cr(VI)-exchanged BAC(10) sample
(Cr(VI)@BAC(10), H
0.22
·Al
2
BO
4.3
·(HCrO
4
)
0.22
·2.64H
2
O)
has been successfully solved by continuous rotation electron diffraction.
The crystallographic data show that the 2D cationic layer of BAC(10)
is built by AlO
6
octahedra, BO
4
tetrahedra,
and BO
3
triangles. Partial chromate ions exchanged with
Cl
–
ions are located within the interlayer region,
which are chemically bonded to the aluminoborate layer. BAC(10) shows
faster adsorption kinetics compared to the commercial anion exchange
resin (AER) and layered double hydroxides (LDHs), a higher maximum
adsorption capacity of 139.1 mg/g than that of AER (62.77 mg/g), LDHs
(81.43 mg/g), and a vast majority of cationic MOFs, and a much broader
working pH range (2–10.5) than LDHs. Moreover, BAC(10) also
shows excellent Cr(VI) oxyanion removal performance for a solution
with a low concentration (1–10 mg/L), and the residual concentration
can be reduced to below 0.05 mg/L of the WHO drinking water criterion.
These superior properties indicate that BAC(10) is a promising material
for remediation of Cr(VI) and other harmful oxyanions from wastewater.
“…In the past few decades, people have invested a lot of energy into the treatment of dyecontaining effluents [8][9][10][11][12][13][14][15][16]. Various methods to degrade dyes, including chemical [17,18], physical [19][20][21][22] and biological [23,24] methods, have been developed and widely applied for the degradation of organic dyes.…”
Organic dyes are widely used in the textile, biological, medical and other fields. However, a serious environmental problem has appeared because of the presence of organic dyes in industrial aqueous effluents. Thus, the efficient treatment of organic dyes in industrial wastewaters is currently in real demand. The current study investigated the oxidative degradation of the organic dye gentian violet by meso-tetra(carboxyphenyl) porphyriniron(III), [FeIII(TCPP)] as a cytochrome P450 model and iodosylbenzene (PhIO) as an oxidant at room temperature. The degradation reaction was monitored by UV–vis absorption spectroscopy via the observation of UV–vis spectral changes of the gentian violet. The results showed that the efficiency of catalyzed degradation reached more than 90% in 1 h, indicating the remarkable oxidative degradation capacity of the [FeIII(TCPP)]/PhIO system, which provided an efficient approach for the treatment of dyeing wastewater.
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