Feng-Ya Ma, Pu Huang, Jing Zhou, Hong-Wei Zeng, Jia-Wei Zhang, Hui Zhao, Yu-Ming Dong, Yong-Fa Zhu, Yao Wang
{"title":"在拉伸应变 Ptδ+-Cuδ+ 双基点上原位揭示二氧化碳电还原的 C-C 耦合行为","authors":"Feng-Ya Ma, Pu Huang, Jing Zhou, Hong-Wei Zeng, Jia-Wei Zhang, Hui Zhao, Yu-Ming Dong, Yong-Fa Zhu, Yao Wang","doi":"10.1007/s12598-024-02846-y","DOIUrl":null,"url":null,"abstract":"<p>Engineering the desired dual metal sites to realize C–C coupling of CO<sub>2</sub> is of great importance for the practical applications of CO<sub>2</sub> electroreduction reaction (CER). Herein, an efficient strategy for constructing heterogeneous Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites to strengthen the generation and coupling of *CO and *CHO (or *COH) during CER process is presented in this work. The radii-larger Pt not only stabilizes the Cu<sup><i>δ</i>+</sup> but also induces a tensile strain in Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites. The obtained Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites achieve a total Faradaic efficiency and current density of C<sub>2</sub> products with 70.9% and 586.9 mA·cm<sup>−2</sup> at – 1.20 V (vs. RHE), which is higher than that of Cu<sup><i>δ</i>+</sup> single site (55.4%, 286.9 mA·cm<sup>−2</sup>). The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveals that the Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites can promote the generation of C<sub>1</sub> intermediates (such as *CO, *COOH, *COH, and *CHO) and C–C coupling. Additional in situ surface-enhanced Raman spectra demonstrate that Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites can induce the generation of the high-frequency peak for *CO<sub>atop</sub>, thus accelerating the C–C coupling. This work provides a promising avenue for stabilizing and enhancing the performance of Cu<sup><i>δ</i>+</sup> sites toward CER.</p><h3 data-test=\"abstract-sub-heading\">Graphical abstract</h3>","PeriodicalId":749,"journal":{"name":"Rare Metals","volume":null,"pages":null},"PeriodicalIF":9.6000,"publicationDate":"2024-07-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"In situ revealing C–C coupling behavior for CO2 electroreduction on tensile strain Ptδ+–Cuδ+ dual sites\",\"authors\":\"Feng-Ya Ma, Pu Huang, Jing Zhou, Hong-Wei Zeng, Jia-Wei Zhang, Hui Zhao, Yu-Ming Dong, Yong-Fa Zhu, Yao Wang\",\"doi\":\"10.1007/s12598-024-02846-y\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Engineering the desired dual metal sites to realize C–C coupling of CO<sub>2</sub> is of great importance for the practical applications of CO<sub>2</sub> electroreduction reaction (CER). Herein, an efficient strategy for constructing heterogeneous Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites to strengthen the generation and coupling of *CO and *CHO (or *COH) during CER process is presented in this work. The radii-larger Pt not only stabilizes the Cu<sup><i>δ</i>+</sup> but also induces a tensile strain in Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites. The obtained Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites achieve a total Faradaic efficiency and current density of C<sub>2</sub> products with 70.9% and 586.9 mA·cm<sup>−2</sup> at – 1.20 V (vs. RHE), which is higher than that of Cu<sup><i>δ</i>+</sup> single site (55.4%, 286.9 mA·cm<sup>−2</sup>). The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveals that the Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites can promote the generation of C<sub>1</sub> intermediates (such as *CO, *COOH, *COH, and *CHO) and C–C coupling. Additional in situ surface-enhanced Raman spectra demonstrate that Pt<sup><i>δ</i>+</sup>–Cu<sup><i>δ</i>+</sup> dual sites can induce the generation of the high-frequency peak for *CO<sub>atop</sub>, thus accelerating the C–C coupling. This work provides a promising avenue for stabilizing and enhancing the performance of Cu<sup><i>δ</i>+</sup> sites toward CER.</p><h3 data-test=\\\"abstract-sub-heading\\\">Graphical abstract</h3>\",\"PeriodicalId\":749,\"journal\":{\"name\":\"Rare Metals\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.6000,\"publicationDate\":\"2024-07-09\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Rare Metals\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1007/s12598-024-02846-y\",\"RegionNum\":1,\"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":"Rare Metals","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1007/s12598-024-02846-y","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
In situ revealing C–C coupling behavior for CO2 electroreduction on tensile strain Ptδ+–Cuδ+ dual sites
Engineering the desired dual metal sites to realize C–C coupling of CO2 is of great importance for the practical applications of CO2 electroreduction reaction (CER). Herein, an efficient strategy for constructing heterogeneous Ptδ+–Cuδ+ dual sites to strengthen the generation and coupling of *CO and *CHO (or *COH) during CER process is presented in this work. The radii-larger Pt not only stabilizes the Cuδ+ but also induces a tensile strain in Ptδ+–Cuδ+ dual sites. The obtained Ptδ+–Cuδ+ dual sites achieve a total Faradaic efficiency and current density of C2 products with 70.9% and 586.9 mA·cm−2 at – 1.20 V (vs. RHE), which is higher than that of Cuδ+ single site (55.4%, 286.9 mA·cm−2). The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveals that the Ptδ+–Cuδ+ dual sites can promote the generation of C1 intermediates (such as *CO, *COOH, *COH, and *CHO) and C–C coupling. Additional in situ surface-enhanced Raman spectra demonstrate that Ptδ+–Cuδ+ dual sites can induce the generation of the high-frequency peak for *COatop, thus accelerating the C–C coupling. This work provides a promising avenue for stabilizing and enhancing the performance of Cuδ+ sites toward CER.
期刊介绍:
Rare Metals is a monthly peer-reviewed journal published by the Nonferrous Metals Society of China. It serves as a platform for engineers and scientists to communicate and disseminate original research articles in the field of rare metals. The journal focuses on a wide range of topics including metallurgy, processing, and determination of rare metals. Additionally, it showcases the application of rare metals in advanced materials such as superconductors, semiconductors, composites, and ceramics.