Synthesis of Intermetallic Compounds and Their Catalytic Applications

doi:10.11901/1005.3093.2019.334

Chinese Journal of Materials Research

2020, Vol. 34

Issue (2): 81-91 DOI: 10.11901/1005.3093.2019.334

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Synthesis of Intermetallic Compounds and Their Catalytic Applications

HOU Zhiquan,GUO Meng,LIU Yuxi,DENG Jiguang,DAI Hongxing(

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College of Environmental and Energy Engineering, Beijing University of Technology, Beijing 100124, China

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HOU Zhiquan,GUO Meng,LIU Yuxi,DENG Jiguang,DAI Hongxing. Synthesis of Intermetallic Compounds and Their Catalytic Applications. Chinese Journal of Materials Research, 2020, 34(2): 81-91.

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Abstract

In this review article, the methods, such as chemical reduction, deposition-precipitation reduction, chemical vapor deposition, and thermal annealing for the synthesis of intermetallic compounds are briefly described. These different synthesis methods possess intrinsically advantages and shortcomings, therefore, suitable methods may be selected according to the actual requirements in practical applications. Catalytic activities of intermetallic compounds for the reactions of oxidation, hydrogenation, and reforming are summarized, from which it is found that intermetallic compounds are a kind of highly efficient catalytic materials, and their high catalytic performance is associated with the ordered atom arrangement, electronic effect, geometric effect, steric effect, and synergistic action. In addition, the future investigation work on such materials is also envisioned.

Key words: review metallic materials catalytic application intermetallic compounds synthesis method

Received: 08 July 2019

ZTFLH:

TG430.40

Fund: National Natural Science Foundation of China(21876006)

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	Zhiquan HOU
	Meng GUO
	Yuxi LIU
	Jiguang DENG
	Hongxing DAI

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https://www.cjmr.org/EN/10.11901/1005.3093.2019.334 OR https://www.cjmr.org/EN/Y2020/V34/I2/81

Fig.1 Structural scheme of (a) substituted solid-solution alloy, (b) interstitial solid-solution alloy, and (c) intermetallic compound^[4]

Fig.2 Schematic illustration of reaction mechanisms for preparation of intermetallic compounds by the polyol method^[4]

Fig.3 Reaction pathways of CO and O₂ coadsorbed on the NaAu₂(111) (down) vs Au(221) (up) crystal planes from initial state (IS) via the intermediate complex OOCO* (MS) to the final state (FS) of CO₂^[45]

Fig.4 (a) CO conversion and (b) CH₄ selectivity on the Ni/SiO₂ and Si-Ni/SiO₂-x (x=250, 350, and 450) catalysts at GHSV=48,000 mL/(g·h) and pressure=1 atm. The short dashed line represented the thermodynamic equilibrium value^[49]

Fig.5 Methanol reaction rates and H₂ formation rates over the PdZnAl, PdMgGa, and PdMgAl catalysts in the MSR at 250^oC^[21]

Intermetallic compound	Synthesis method	Crystal phase	Particle size	Reaction condition	Catalytic performance	Ref.
Pd₅Ga₃	Chemical reduction	Orthorhomibc	5.3 nm	0.5% CH₄, 4% O₂, N₂ balance; space velocity (SV): 80000 mL/(g·h)	T_90% is lower to 372^oC, the special reaction rate of Pd is 23.32×10^-6 mol/(g_Pd s) at 290^oC.	[12]
Ni₃Ga, Ni₃Sn₂	Chemical reduction	Cubic	3.5~7.5 nm	Pretreated with H₂; 1 mmol substrate and 0.5 mmol n-dodecane; H₂: 500 kPa; 1300 r/min	After 13 h continuous reaction, the conversion of various types of alkyne reached more than 90%, and the selectivity of olefins was over 94%.	[15]
Pd_mM_n (M=Ge, In, Sn, Zn)	Gas-phase reduction	-	-	12.5% butylene, butylene: O₂=1:1, He (balance); total gas flow rate: 120 mL/min	PdIn, PdBi or Pd₃Fe catalysts show high selectivity for 1,3-Butadiene and 1-butene (more than 50%) and high yield.	[20]
Pd₂Ga and PdZn	Gas-phase reduction	Cubic	-	H₂O/CH₃OH=1.0, total gas flow rate: 26 mL/min, methanol concentration: 28.4%	PdZnAl exhibited the best catalytic activity, with 87% hydrogen selectivity at 250^oC and hydrogen generation rate of 964 μmol/(g·min).	[21]
Ni₃Sn, Ni₃Sn₂, Ni₃Sn₂, Ni₃Sn₄	Arc melting	-	25~38 μm	The partial pressures of acetylene and hydrogen are 2.7 and 13 kPa, respectively.	The acetylene conversion rates of Ni₃Sn, Ni₃Sn₂and Ni₃Sn₄are 2.3×10^-6 mol/(g·s), 0.6×10^-6 mol/(g·s) and less than 0.001×10^-6 mol/(g·s), respectively.	[22]
Pt₃Sn	Polyol process	-	5.2±1.0 nm	O₂/CO=6:1; room temperature	The initiation temperature of CO oxidation on Pt₃Sn is lower than that on the Pt catalyst.	[31]
Pt₃Ti	Chemical reduction	Cubic	2.5 nm	2 % CO, 1% O₂, 97% He, space velocity (SV): 120000 mL/(g·h)	The ignition temperature of CO oxidation on Pt₃Ti catalyst is 125^oC, which is lower than that on single Pt catalyst.	[43]
Ni₂Si, NiSi or NiSi₂	Chemical vapor deposition	Cubic	3~4 nm	H₂/CO=3:1, Ar balance, space velocity (SV): 48000 mL/(g·h)	The activity of CO methanation on Ni-Si catalyst is much higher than that on single nickel catalyst, with enhanced stability of nickel sintering resistance at high temperature (500~600^oC).	[49]
NiZn	Thermal annealing	Cubic	20~32 μm	methanol:H₂O=1:1; 0.01 mL/min, N₂: 13.2 mL/min, He: 1.6 mL/min	NiZn catalyst has good catalytic performance for methanol reforming (80% conversion at 550^oC) and good hydrogen selectivity (70%).	[57]

Table 1 Synthesis methods, physical properties, and catalytic activities of intermetallic compounds reported in the literature

Fig.6 The relationship of experimentally measured specific activity for the ORR on the Pt₃M surface in 0.1 mol/L HClO₄ at 60^oC with the d-band center position for the Pt-skin surface^[63]

Fig.7 A relationship of the apparent activation energies of Ni and Ni₃M intermetallic compounds for the H₂-D₂ equilibrium reaction with their potentials of the d-band centre^[64]

Fig.8 (a) STM images of CO adsorbed on Pd₃(A) and Pd₁ (B). The atomic surface structure is overlaid on the left-hand site of each image (Pd: cyan, large; Ga: red, small); (b) IR absorption spectra as a function of wavenumber and CO exposure at -183^oC on Pd₃ (left) and Pd₁ (right)^[65]

Fig.9 (a) Hydrogen-mediated alkene isomerization via alkyl intermediate, (b) equilibrium crystal shape and the corresponding surface atomic arrangement of a RhSb nanoparticle, and (c) limited hydrogen access to cis-2-butene adsorbed on RhSb (020) plane^[67]

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