Yi Song, Yu Liu, Wenwei Liu, Zhiyi Zhao, Xiaoqiong Liu, Ying Xu, Tao Li
{"title":"用不混相钽合金化提高铜的CO氧化性能","authors":"Yi Song, Yu Liu, Wenwei Liu, Zhiyi Zhao, Xiaoqiong Liu, Ying Xu, Tao Li","doi":"10.1021/acsami.4c19374","DOIUrl":null,"url":null,"abstract":"Copper–tantalum (Cu–Ta) immiscible alloy nanoparticles (NPs) have been the subject of extensive research in the field of structural materials, due to their exceptional nanostructural stability and high-temperature creep properties. However, Cu is also a highly active oxidation catalyst due to its abundant valence changes. In this study, we have for the first time obtained homogeneous Cu<sub><i>x</i></sub>Ta<sub>1–<i>x</i></sub> (<i>x</i> = 0.5, 0.7, 0.9, 1) nanoparticles by wet coreduction with an average particle size of approximately 30 nm. Testing verified all the Cu<sub><i>x</i></sub>Ta<sub>1–<i>x</i></sub>/TiO<sub>2</sub> (<i>x</i> = 0.5, 0.7, 0.9) showed higher CO oxidation activity than Cu/TiO<sub>2</sub>, with Cu<sub>0.7</sub>Ta<sub>0.3</sub>/TiO<sub>2</sub> exhibiting the most promising performance. The temperature-programmed reduction with hydrogen demonstrated that Cu<sub>0.7</sub>Ta<sub>0.3</sub>/TiO<sub>2</sub> exhibits enhanced redox properties. While kinetic studies indicated that the reaction of the Cu<sub>0.7</sub>Ta<sub>0.3</sub>/TiO<sub>2</sub> catalyst followed the Langmuir–Hinshelwood mechanism, in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) verified the introduction of Ta induced the generation of bicarbonate as an intermediate product and increased the adsorption capacity of Cu<sup>+</sup> on CO in the catalyst, which facilitated the reaction of surface adsorbed CO with oxygen and led to the enhanced CO oxidation activity.","PeriodicalId":5,"journal":{"name":"ACS Applied Materials & Interfaces","volume":"30 1","pages":""},"PeriodicalIF":8.3000,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing the CO Oxidation Performance of Copper by Alloying with Immiscible Tantalum\",\"authors\":\"Yi Song, Yu Liu, Wenwei Liu, Zhiyi Zhao, Xiaoqiong Liu, Ying Xu, Tao Li\",\"doi\":\"10.1021/acsami.4c19374\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Copper–tantalum (Cu–Ta) immiscible alloy nanoparticles (NPs) have been the subject of extensive research in the field of structural materials, due to their exceptional nanostructural stability and high-temperature creep properties. However, Cu is also a highly active oxidation catalyst due to its abundant valence changes. In this study, we have for the first time obtained homogeneous Cu<sub><i>x</i></sub>Ta<sub>1–<i>x</i></sub> (<i>x</i> = 0.5, 0.7, 0.9, 1) nanoparticles by wet coreduction with an average particle size of approximately 30 nm. Testing verified all the Cu<sub><i>x</i></sub>Ta<sub>1–<i>x</i></sub>/TiO<sub>2</sub> (<i>x</i> = 0.5, 0.7, 0.9) showed higher CO oxidation activity than Cu/TiO<sub>2</sub>, with Cu<sub>0.7</sub>Ta<sub>0.3</sub>/TiO<sub>2</sub> exhibiting the most promising performance. The temperature-programmed reduction with hydrogen demonstrated that Cu<sub>0.7</sub>Ta<sub>0.3</sub>/TiO<sub>2</sub> exhibits enhanced redox properties. While kinetic studies indicated that the reaction of the Cu<sub>0.7</sub>Ta<sub>0.3</sub>/TiO<sub>2</sub> catalyst followed the Langmuir–Hinshelwood mechanism, in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) verified the introduction of Ta induced the generation of bicarbonate as an intermediate product and increased the adsorption capacity of Cu<sup>+</sup> on CO in the catalyst, which facilitated the reaction of surface adsorbed CO with oxygen and led to the enhanced CO oxidation activity.\",\"PeriodicalId\":5,\"journal\":{\"name\":\"ACS Applied Materials & Interfaces\",\"volume\":\"30 1\",\"pages\":\"\"},\"PeriodicalIF\":8.3000,\"publicationDate\":\"2025-01-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Applied Materials & Interfaces\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsami.4c19374\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MATERIALS SCIENCE, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Applied Materials & Interfaces","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsami.4c19374","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
Enhancing the CO Oxidation Performance of Copper by Alloying with Immiscible Tantalum
Copper–tantalum (Cu–Ta) immiscible alloy nanoparticles (NPs) have been the subject of extensive research in the field of structural materials, due to their exceptional nanostructural stability and high-temperature creep properties. However, Cu is also a highly active oxidation catalyst due to its abundant valence changes. In this study, we have for the first time obtained homogeneous CuxTa1–x (x = 0.5, 0.7, 0.9, 1) nanoparticles by wet coreduction with an average particle size of approximately 30 nm. Testing verified all the CuxTa1–x/TiO2 (x = 0.5, 0.7, 0.9) showed higher CO oxidation activity than Cu/TiO2, with Cu0.7Ta0.3/TiO2 exhibiting the most promising performance. The temperature-programmed reduction with hydrogen demonstrated that Cu0.7Ta0.3/TiO2 exhibits enhanced redox properties. While kinetic studies indicated that the reaction of the Cu0.7Ta0.3/TiO2 catalyst followed the Langmuir–Hinshelwood mechanism, in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) verified the introduction of Ta induced the generation of bicarbonate as an intermediate product and increased the adsorption capacity of Cu+ on CO in the catalyst, which facilitated the reaction of surface adsorbed CO with oxygen and led to the enhanced CO oxidation activity.
期刊介绍:
ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.