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铜-氧化铟体系中的活性金属-载体相互作用:金属间化合物的形成及其对一氧化碳选择性甲醇蒸汽重整的影响。

Reactive metal-support interaction in the Cu-InO system: intermetallic compound formation and its consequences for CO-selective methanol steam reforming.

作者信息

Ploner Kevin, Schlicker Lukas, Gili Albert, Gurlo Aleksander, Doran Andrew, Zhang Lei, Armbrüster Marc, Obendorf Dagmar, Bernardi Johannes, Klötzer Bernhard, Penner Simon

机构信息

Department of Physical Chemistry, University of Innsbruck, Innsbruck, Austria.

Fachgebiet Keramische Werkstoffe/Chair of Advanced Ceramic Materials, Institut für Werkstoffwissenschaften und -technologien, Berlin, Germany.

出版信息

Sci Technol Adv Mater. 2019 Apr 25;20(1):356-366. doi: 10.1080/14686996.2019.1590127. eCollection 2019.

DOI:10.1080/14686996.2019.1590127
PMID:31068984
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6493314/
Abstract

The reactive metal-support interaction in the Cu-InO system and its implications on the CO selectivity in methanol steam reforming (MSR) have been assessed using nanosized Cu particles on a powdered cubic InO support. Reduction in hydrogen at 300 °C resulted in the formation of metallic Cu particles on InO. This system already represents a highly CO-selective MSR catalyst with ~93% selectivity, but only 56% methanol conversion and a maximum H formation rate of 1.3 µmol g  s. After reduction at 400 °C, the system enters an InO-supported intermetallic compound state with CuIn as the majority phase. CuIn exhibits markedly different self-activating properties at equally pronounced CO selectivities between 92% and 94%. A methanol conversion improvement from roughly 64% to 84% accompanied by an increase in the maximum hydrogen formation rate from 1.8 to 3.8 µmol g  s has been observed from the first to the fourth consecutive runs. The presented results directly show the prospective properties of a new class of Cu-based intermetallic materials, beneficially combining the MSR properties of the catalyst's constituents Cu and InO. In essence, the results also open up the pathway to in-depth development of potentially CO-selective bulk intermetallic Cu-In compounds with well-defined stoichiometry in MSR.

摘要

利用负载在立方晶型粉末状氧化铟载体上的纳米级铜颗粒,评估了铜 - 氧化铟体系中的活性金属 - 载体相互作用及其对甲醇蒸汽重整(MSR)中一氧化碳选择性的影响。在300℃下用氢气还原导致在氧化铟上形成金属铜颗粒。该体系已经是一种具有约93%选择性的高一氧化碳选择性MSR催化剂,但甲醇转化率仅为56%,最大氢气生成速率为1.3 μmol g⁻¹ s⁻¹。在400℃还原后,该体系进入以铜铟为主要相的氧化铟负载金属间化合物状态。在一氧化碳选择性同样显著介于92%至94%之间时,铜铟表现出明显不同的自活化性能。从第一次到第四次连续运行中,观察到甲醇转化率从约64%提高到84%,同时最大氢气生成速率从1.8 μmol g⁻¹ s⁻¹增加到3.8 μmol g⁻¹ s⁻¹。所呈现的结果直接展示了一类新型铜基金属间材料的潜在性能,其有益地结合了催化剂组分铜和氧化铟的MSR性能。本质上,这些结果也为深入开发在MSR中具有明确化学计量比的潜在一氧化碳选择性块状金属间铜 - 铟化合物开辟了道路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/30ea6bc337c3/TSTA_A_1590127_F0006_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/dbab9f5858cd/TSTA_A_1590127_UF0001_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/e4c13a189e54/TSTA_A_1590127_F0001_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/01c7ba2954cd/TSTA_A_1590127_F0002_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/9fa9ed24ce1c/TSTA_A_1590127_F0003_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/3d0c290710aa/TSTA_A_1590127_F0004_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/3877eacfe91c/TSTA_A_1590127_F0005_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/30ea6bc337c3/TSTA_A_1590127_F0006_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/dbab9f5858cd/TSTA_A_1590127_UF0001_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/e4c13a189e54/TSTA_A_1590127_F0001_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/01c7ba2954cd/TSTA_A_1590127_F0002_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/9fa9ed24ce1c/TSTA_A_1590127_F0003_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/3d0c290710aa/TSTA_A_1590127_F0004_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/3877eacfe91c/TSTA_A_1590127_F0005_OC.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e455/6493314/30ea6bc337c3/TSTA_A_1590127_F0006_OC.jpg

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