金属间化合物的合成及其催化应用

doi:10.11901/1005.3093.2019.334

材料研究学报

2020, Vol. 34

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

研究论文

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金属间化合物的合成及其催化应用

侯志全,郭萌,刘雨溪,邓积光,戴洪兴(

)

北京工业大学环境与能源工程学院北京 100124

Synthesis of Intermetallic Compounds and Their Catalytic Applications

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

)

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

引用本文:

侯志全,郭萌,刘雨溪,邓积光,戴洪兴. 金属间化合物的合成及其催化应用[J]. 材料研究学报, 2020, 34(2): 81-91.
Zhiquan HOU, Meng GUO, Yuxi LIU, Jiguang DENG, Hongxing DAI. Synthesis of Intermetallic Compounds and Their Catalytic Applications[J]. Chinese Journal of Materials Research, 2020, 34(2): 81-91.

全文: PDF(2797 KB) HTML

摘要:

简要叙述了合成金属间化合物的化学还原、沉积沉淀还原、化学气相沉积和热退火等方法。这些合成方法各有优缺点，可根据实际需求选择适宜的方法。总结了金属间化合物对加氢、氧化、重整等反应的催化性能，发现金属间化合物是一类性能优良的催化材料，催化活性与其具有的有序原子排列、电子效应、几何效应、空间效应、协同作用等有关。此外，还展望了此类材料的未来研究方向。

关键词 ：评述, 金属材料, 催化应用, 金属间化合物, 合成方法

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

收稿日期: 2019-07-08

ZTFLH:

TG430.40

基金资助:国家自然科学基金(21876006)

作者简介: 侯志全，男，1994年生，博士生

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https://www.cjmr.org/CN/10.11901/1005.3093.2019.334 或 https://www.cjmr.org/CN/Y2020/V34/I2/81

图1 (a) 置换固溶合金、(b) 间隙固溶合金和(c) 金属间化合物的结构示意图[4]

图2 采用多元醇法合成金属间化合物的反应机理示意图[4]

图3 NaAu2(111)和Au(221)晶面上共吸附CO和O2后的反应途径示意图，上、下分别为Au(221)和NaAu2(111)晶面上的反应途径[45]

图4 镍基催化剂在空速为48000 mL/(g·h)条件下对CO加氢反应的CO转化率(a)和甲烷选择性(b)[49]

图5 PdZnAl、PdMgAl和PdMgGa催化剂上MSR反应在250oC时的甲醇反应速率与氢气形成速率[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]

表1 文献报道的金属间化合物的合成方法、物理性质和催化活性

图6 在0.1 mol/L HClO4中实验测量的Pt3M表面上ORR在60oC时的比活性与表面d带中心电位之间的关系[63]

图7 Ni和Ni3M金属间化合物对H2-D2平衡反应的表观活化能与d带中心电位的关系[64]

图8 (a) PdGa(111)和PdGa(1?1?1?)晶面的STM照片；(b) PdGa(111)和PdGa(1?1?1?)晶面上CO吸附的红外谱图[65]

图9 (a) 通过烷基中间体的氢控烯烃异构化、(b) 一个RhSb纳米粒子的晶体形状和相应的表面原子排列和(c) 受限氢靠近RhSb (020)晶面上吸附的顺式-2-丁烯[67]

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