Accessory ligand strategies for hexacyanometallate networks deriving perovskite polycrystalline electromagnetic absorbents

doi:10.1016/j.jmst.2020.11.071

Abstract

Abstract:

The controllable adjustment of electromagnetic (EM) properties for high-efficiency EM absorbents are indispensable, nonetheless, rare in crystals engineering regulation. Herein, for the first time, regulated amount of sodium citrate was employed as accessory ligand of cobalt cation in aqueous solution to kinetically assist the controllable fabrication of Prussian blue analogs (PBAs) and corresponding lanthanide perovskite hybrid CoFe alloy polycrystals. Especially, the multi-phase features were analyzed based on Rietveld refinement of XRD patterns, illustrating the existence of distortions, defects and heterogeneous interfaces in resultant polycrystals. Benefited to the dielectric and magnetic adjustment, polycrystalline absorbents achieved excellent impedance matching and EM attenuation, as the minimum reflection loss of CoFe/LaFeO₃ and CoFe/LaFeO₃/La₂O₃ reached -44.13 and -33.95 dB, ranking broadest effective bands up to 4.88 and 3.36 GHz. The validity of the strategy provided a novel sight into the controllable fabrication of high-performance magnetic semiconductor polycrystalline devices.

Key words: Sodium citrate, Prussian blue analogs, Polycrystalline, Electromagnetic absorption, Interfacial polarization

Zhenguo Gao, Zehao Zhao, Di Lan, Kaichang Kou, Jiaoqiang Zhang, Hongjing Wu. Accessory ligand strategies for hexacyanometallate networks deriving perovskite polycrystalline electromagnetic absorbents[J]. J. Mater. Sci. Technol., 2021, 82: 69-79.

Figures/Tables 12

Table 1 Prime information summary of PBAs fabricated with different amounts of chelating agents and their corresponding prologized products.

Samples	Sodium citrate /mmol	Phases	Space group	Crystal system
PB1-La	2	Co₂Fe(CN)₆	F - 43 m	Cubic
PB2-La	4	Co₂Fe(CN)₆	F - 43 m	Cubic
PB3-La	6	Co₂Fe(CN)₆	F - 43 m	Cubic
PB3-La	6	Co₃[Fe(CN)₆]₂·H₂O	F - 43 m	Cubic
PB4-La	8	Co₂Fe(CN)₆	F - 43 m	Cubic
PB4-La	8	Co₃[Fe(CN)₆]₂·H₂O	F - 43 m	Cubic
PB1-La-C	/	CoFe	Pm - 3 m	Cubic
PB2-La-C	/	CoFe	Pm - 3 m	Cubic
PB2-La-C	/	La₂O₃	P - 3 m1	Hexagonal
PB3-La-C	/	CoFe	Pm - 3 m	Cubic
PB3-La-C	/	LaFeO₃	Pnma	Tetragonal
PB4-La-C	/	CoFe	Pm - 3 m	Cubic
		La₂O₃	P - 3 m1	Hexagonal
		LaFeO₃	Pnma	Tetragonal

Scheme 1. Schematic illustration of PBA microcubes formation and CoFe alloy-based lanthanum polycrystals.

Fig. 1. (a) Schematic process of phase transition of PBA crystals; XRD patterns of (b) PBAs with no La decoration and their corresponding (c) annealed products; (d) XRD patterns of La decorative PBAs and (e) their corresponding pyrolyzed products.

Fig. 2. Rietveld refinement results for the XRD patterns of (a) PB1-La-C, (b) PB2-La-C, (c) PB3-La-C and (d) PB4-La-C.

Table 2 Rietveld refined structural parameters for La decorative CoFe alloy polycrystals.

Samples	Phases	Atoms	a/Å	b/Å	c/Å	V/Å³	x	y	z	Occ.	R_wp/%	R_p/%
PB1-La-C	CoFe [Pm - 3 m]	Co(1a)	2.857	2.857	2.857	23.317	0.000	0.000	0.000	0.835	18.5	15.6
PB1-La-C	CoFe [Pm - 3 m]	Fe(1b)	2.857	2.857	2.857	23.317	0.500	0.500	0.500	0.420	18.5	15.6
PB2-La-C	CoFe [Pm - 3 m]	Co(1a)	2.861	2.861	2.861	23.421	0.000	0.000	0.250	0.725	13.1	11.0
	CoFe [Pm - 3 m]	Fe(1b)	2.861	2.861	2.861	23.421	0.000	0.000	0.000	0.383
	La₂O₃ [P - 3 m1]	La(4f)	3.958	3.958	6.160	82.583	0.333	0.667	0.245	0.713
		O1(2a)					0.000	0.000	0.000	0.860
		O2(4f)					0.333	0.667	0.679	1.000
PB3-La-C	CoFe [Pm - 3 m]	Co(1a)	2.853	2.853	2.853	23.226	0.000	0.000	0.000	0.805	19.8	17.7
	CoFe [Pm - 3 m]	Fe(1b)	2.853	2.853	2.853	23.226	0.500	0.500	0.500	0.487
	LaFeO₃ [Pnma]	O1(8d)	5.574	5.596	7.883	245.858	0.719	0.302	0.029	1.000
		Fe1(4b)					0.000	0.500	0.000	0.402
		O2(4c)					0.080	0.485	0.250	0.288
		La1(4c)					0.993	0.030	0.250	0.405
PB4-La-C	CoFe [Pm - 3 m]	Co(1a)	2.853	2.853	2.853	23.232	0.000	0.000	0.000	0.478	18.9	12.9
	CoFe [Pm - 3 m]	Fe(1b)	2.853	2.853	2.853	23.232	0.500	0.500	0.500	0.289
	La₂O₃ [P - 3 m1]	La(4f)	3.960	3.960	6.176	83.870	0.333	0.667	0.234	0.544
		O1(2a)					0.000	0.000	0.000	1.000
		O2(4f)					0.333	0.667	0.639	0.739
	LaFeO₃ [Pnma]	O1(8d)	5.566	5.654	7.880	247.795	0.754	0.333	0.028	0.912
		Fe1(4b)					0.000	0.000	0.000	0.510
		O2(4c)					0.163	0.494	0.250	0.325
		La1(4c)					0.972	0.045	0.250	0.474

Fig. 3. Schematic illustration of the kinetic regulation of self-assembly; SEM images of (a) PB1-La, (b) PB2-La, (c) PB3-La and (d) PB4-La; (e) elements mapping images of PB3-La; SEM images of (f) PB1-La-C, (g) PB2-La-C, (h) PB3-La-C and (i) PB4-La-C; (j) elements mapping images of PB3-La-C and (k) PB4-La-C.

Fig. 4. (a) Raman spectrums; (b) XPS spectrums in whole regions; (c) high-resolution Fe2p spectrums of all samples; (d) high-resolution Co2p spectrums of PB4-La-C; (e) schematic illustration of oxygen vacancy in perovskite type LaFeO3 crystal.

Fig. 5. Frequency dependance of (a1) real (ε') and (b1) imaginary (ε”) part of complex permittivity, (c1) real (μ') and (d1) imaginary part (μ”) of complex permeability; Debye relaxation curves (Cole-Cole semicircles) of (a2) PB1-La-C, (b2) PB2-La-C, (c2) PB3-La-C and (d2) PB4-La-C; magnetic hysteresis loops of (a3) PB1-La-C, (b3) PB2-La-C, (c3) PB3-La-C and (d3) PB4-La-C.

Fig. 6. (a1) Dielectric loss tangent (tanδε) and magnetic loss tangent (tanδμ), (c1) α and (d1) normalized matching thickness (tm) curves; Three-dimensional images of calculated RL values of (a2) PB1-La-C, (b2) PB2-La-C, (c2) PB3-La-C and (d2) PB4-La-C; Two-dimensional images of calculated RL values of (a3) PB1-La-C, (b3) PB2-La-C, (c3) PB3-La-C and (d3) PB4-La-C.

Fig. 7. RL and |Zin/Z0| curves of (a1) PB1-La-C, (b1) PB2-La-C, (c1) PB3-La-C and (d1) PB4-La-C; RL and fE histograms of (a2) PB1-La-C, (b2) PB2-La-C, (c2) PB3-La-C and (d2) PB4-La-C; (c) C0 curves; (d) equivalent EM attenuation model of perovskite polycrystals.

Fig. 8. Comparison of EMW absorbability of representative transition metal (Fe, Co, Ni) deriving crystals.

Table 3 Comparison?of EMW absorbability of representative transition metal (Fe, Co, Ni) deriving crystals.

No.	MAMs	RL_min/dB	f_E/dB	t_m/mm	Refs.
1	Fe nanowires	-29.74	3.84	3.0	[41]
2	Fe@Fe₃O₄	-40.00	4.00	1.5	[42]
3	FeSiAl	-39.7	3.20	4.0	[43]
4	FeCoNiCrCuAl_0.3@air@NiO	-41.10	2.67	3.6	[44]
5	Fe_xO_y/Fe-graphite	-42.1	4.40	5.5	[45]
6	Ni@TiO₂	-38.00	1.80	1.8	[46]
7	Nd_0.3Ce_1.7Co₁₇	-30.53	2.24	1.8	[47]
8	FeNi@C	-30.00	4.70	2.0	[48]
9	Co@C microsphere	-30.00	3.00	2.0	[49]
10	Co/CoNiO₂	-30.50	1.40	4.5	[50]
11	NiCo-alloy@tubular-g-C₃N₄	-35.63	4.80	2.0	[51]
12	CoNi@NG-NCP	-24.03	4.32	2.5	[52]
13	CoFe₂@SiO₂	-19.93	4.29	2.0	[53]
14	LaFeO₃/RGO	-36.23	3.92	2.0	[54]
15	CoFe@LaFeO₃	-44.13	4.88	3.0	This work
16	CoFe@LaFeO₃@La₂O₃	-33.95	2.72	2.0	This work

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