固溶体衍生的Cu簇在部分还原的CuCeO2上具有丰富的氧空位,实现了高效的水煤气反反应。

IF 3.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Jianhong Xu, Zihao Liu, Ruoyu Zhang, Qingfeng Ge, Xinli Zhu
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引用次数: 0

摘要

逆水气转换(RWGS)反应为CO2转化为CO提供了一种便捷的途径,有利于实现碳峰值和碳中和的目标。其中,以Na2CO3和NaOH的混合物为原料,在pH = 10的条件下(样品Cu/CeO2-10),采用共沉淀法制备Cu/CeO2催化剂,在400℃、CO2/H2比为1:4的条件下,Cu/CeO2催化剂的本然反应速率为428.4 mmol•gcat-1•h-1,具有100%的CO选择性,远高于浸渍法制备的Cu/CeO2催化剂。各种表征结果表明,煅烧Cu/CeO2-10中CuCeO2固溶体的含量最高,在部分还原的CuCeO2固溶体上形成高度分散(~2.5 nm)的Cu团簇,还原后形成丰富的氧空位。Cu和氧空位分别有利于H2和CO2的活化,导致H2和CO2的反应顺序降低。因此,这两种成分之间的协同作用增强了RWGS的整体活性,同时降低了活化能。在24h稳定性测试中,最佳催化剂表现出良好的稳定性,没有出现铜团簇的团聚现象。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Solid Solution Derived Cu Clusters on Partially Reduced CuCeO2 with Abundant Oxygen Vacancies Enable Efficient Reverse Water Gas Reaction

Solid Solution Derived Cu Clusters on Partially Reduced CuCeO2 with Abundant Oxygen Vacancies Enable Efficient Reverse Water Gas Reaction

Solid Solution Derived Cu Clusters on Partially Reduced CuCeO2 with Abundant Oxygen Vacancies Enable Efficient Reverse Water Gas Reaction

Solid Solution Derived Cu Clusters on Partially Reduced CuCeO2 with Abundant Oxygen Vacancies Enable Efficient Reverse Water Gas Reaction

Solid Solution Derived Cu Clusters on Partially Reduced CuCeO2 with Abundant Oxygen Vacancies Enable Efficient Reverse Water Gas Reaction

The reverse water gas shift (RWGS) reaction provides a convenient approach to convert CO2 to CO, which facilitates to achieve the goals of carbon peaking and carbon neutrality. Herein, the Cu/CeO2 catalyst prepared by a co-precipitation method using a mixture of Na2CO3 and NaOH at pH of 10 (sample Cu/CeO2-10) achieved an intrinsic reaction rate of 428.4 mmol ⋅ gcat−1 ⋅ h−1 with 100 % CO selectivity at 400 °C and CO2/H2 ratio of 1 : 4, which is much higher than Cu/CeO2 prepared by impregnation and other methods. Various characterizations showed the highest fraction of CuCeO2 solid solution in the calcined Cu/CeO2-10, and formed highly dispersed Cu clusters (~2.5 nm) on partially reduced CuCeO2 solid solution with abundant of oxygen vacancies upon reduction. The Cu and oxygen vacancies facilitates the activation of H2 and CO2, respectively, resulting in lowered H2 and CO2 reaction orders. As a result, the synergy between the two components enhanced the overall RWGS activity with lowered activation energy. Moreover, the optimal catalyst is very stable in 24 h stability test without detectable agglomeration of Cu clusters.

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来源期刊
Chemistry - An Asian Journal
Chemistry - An Asian Journal 化学-化学综合
CiteScore
7.00
自引率
2.40%
发文量
535
审稿时长
1.3 months
期刊介绍: Chemistry—An Asian Journal is an international high-impact journal for chemistry in its broadest sense. The journal covers all aspects of chemistry from biochemistry through organic and inorganic chemistry to physical chemistry, including interdisciplinary topics. Chemistry—An Asian Journal publishes Full Papers, Communications, and Focus Reviews. A professional editorial team headed by Dr. Theresa Kueckmann and an Editorial Board (headed by Professor Susumu Kitagawa) ensure the highest quality of the peer-review process, the contents and the production of the journal. Chemistry—An Asian Journal is published on behalf of the Asian Chemical Editorial Society (ACES), an association of numerous Asian chemical societies, and supported by the Gesellschaft Deutscher Chemiker (GDCh, German Chemical Society), ChemPubSoc Europe, and the Federation of Asian Chemical Societies (FACS).
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