{"title":"原子缺陷工程促进尿素合成,实现二氧化碳和硝酸盐共电还原。","authors":"Zifan Xu, Zhengwu Yang, Huan Lu, Jiangchen Zhu, Junlin Li, Ming-Hui Fan, Zhi Zhao, Xiangdong Kong, Ke Wang, Zhigang Geng","doi":"10.1021/acs.nanolett.4c03451","DOIUrl":null,"url":null,"abstract":"<p><p>The atomic defect engineering could feasibly decorate the chemical behaviors of reaction intermediates to regulate catalytic performance. Herein, we created oxygen vacancies on the surface of In(OH)<sub>3</sub> nanobelts for efficient urea electrosynthesis. When the oxygen vacancies were constructed on the surface of the In(OH)<sub>3</sub> nanobelts, the faradaic efficiency for urea reached 80.1%, which is 2.9 times higher than that (20.7%) of the pristine In(OH)<sub>3</sub> nanobelts. At -0.8 V versus reversible hydrogen electrode, In(OH)<sub>3</sub> nanobelts with abundant oxygen vacancies exhibited partial current density for urea of -18.8 mA cm<sup>-2</sup>. Such a value represents the highest activity for urea electrosynthesis among recent reports. Density functional theory calculations suggested that the unsaturated In sites adjacent to oxygen defects helped to optimize the adsorbed configurations of key intermediates, promoting both the C-N coupling and the activation of the adsorbed CO<sub>2</sub>NH<sub>2</sub> intermediate. In-situ spectroscopy measurements further validated the promotional effect of the oxygen vacancies on urea electrosynthesis.</p>","PeriodicalId":53,"journal":{"name":"Nano Letters","volume":null,"pages":null},"PeriodicalIF":9.6000,"publicationDate":"2024-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Atomic Defects Engineering Boosts Urea Synthesis toward Carbon Dioxide and Nitrate Coelectroreduction.\",\"authors\":\"Zifan Xu, Zhengwu Yang, Huan Lu, Jiangchen Zhu, Junlin Li, Ming-Hui Fan, Zhi Zhao, Xiangdong Kong, Ke Wang, Zhigang Geng\",\"doi\":\"10.1021/acs.nanolett.4c03451\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>The atomic defect engineering could feasibly decorate the chemical behaviors of reaction intermediates to regulate catalytic performance. Herein, we created oxygen vacancies on the surface of In(OH)<sub>3</sub> nanobelts for efficient urea electrosynthesis. When the oxygen vacancies were constructed on the surface of the In(OH)<sub>3</sub> nanobelts, the faradaic efficiency for urea reached 80.1%, which is 2.9 times higher than that (20.7%) of the pristine In(OH)<sub>3</sub> nanobelts. At -0.8 V versus reversible hydrogen electrode, In(OH)<sub>3</sub> nanobelts with abundant oxygen vacancies exhibited partial current density for urea of -18.8 mA cm<sup>-2</sup>. Such a value represents the highest activity for urea electrosynthesis among recent reports. Density functional theory calculations suggested that the unsaturated In sites adjacent to oxygen defects helped to optimize the adsorbed configurations of key intermediates, promoting both the C-N coupling and the activation of the adsorbed CO<sub>2</sub>NH<sub>2</sub> intermediate. In-situ spectroscopy measurements further validated the promotional effect of the oxygen vacancies on urea electrosynthesis.</p>\",\"PeriodicalId\":53,\"journal\":{\"name\":\"Nano Letters\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.6000,\"publicationDate\":\"2024-09-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nano Letters\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.nanolett.4c03451\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/9/9 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nano Letters","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acs.nanolett.4c03451","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/9/9 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
原子缺陷工程可以装饰反应中间产物的化学行为,从而调节催化性能。在此,我们在 In(OH)3 纳米颗粒表面制造了氧空位,以实现高效尿素电合成。在 In(OH)3 纳米颗粒表面形成氧空位后,尿素的远红外效率达到 80.1%,是原始 In(OH)3 纳米颗粒的 2.9 倍(20.7%)。与可逆氢电极相比,在-0.8 V电压下,具有丰富氧空位的In(OH)3纳米颗粒对尿素的部分电流密度为-18.8 mA cm-2。这一数值代表了近期报道的最高尿素电合成活性。密度泛函理论计算表明,与氧缺陷相邻的不饱和 In 位点有助于优化关键中间产物的吸附构型,促进 C-N 偶联和吸附的 CO2NH2 中间产物的活化。原位光谱测量进一步验证了氧空位对尿素电合成的促进作用。
The atomic defect engineering could feasibly decorate the chemical behaviors of reaction intermediates to regulate catalytic performance. Herein, we created oxygen vacancies on the surface of In(OH)3 nanobelts for efficient urea electrosynthesis. When the oxygen vacancies were constructed on the surface of the In(OH)3 nanobelts, the faradaic efficiency for urea reached 80.1%, which is 2.9 times higher than that (20.7%) of the pristine In(OH)3 nanobelts. At -0.8 V versus reversible hydrogen electrode, In(OH)3 nanobelts with abundant oxygen vacancies exhibited partial current density for urea of -18.8 mA cm-2. Such a value represents the highest activity for urea electrosynthesis among recent reports. Density functional theory calculations suggested that the unsaturated In sites adjacent to oxygen defects helped to optimize the adsorbed configurations of key intermediates, promoting both the C-N coupling and the activation of the adsorbed CO2NH2 intermediate. In-situ spectroscopy measurements further validated the promotional effect of the oxygen vacancies on urea electrosynthesis.
期刊介绍:
Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including:
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- Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance
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