{"title":"氧化钴纳米盒中高效Cu─Co双位点电催化还原低浓度NO为NH3","authors":"Dongdong Wang, Guilan Fan, Zhihao Pei, Deyan Luan, Xiaojun Gu, Xiong Wen David Lou","doi":"10.1002/adma.202504497","DOIUrl":null,"url":null,"abstract":"<p>The electrocatalytic conversion of nitric oxide (NO) to ammonia (NH<sub>3</sub>) epitomizes an advanced approach in NH<sub>3</sub> synthesis, crucial for efficiently converting low-concentration industrial NO exhaust and contributing significantly to environmental preservation. Catalyst design remains one pivotal element in addressing this challenge. Here, efficient Cu─Co dual active sites embedded in hollow cobalt oxide nanoboxes are created for the electrocatalytic low-concentration NO reduction reaction (NORR). Cu-modified cobalt oxide (Cu-Co<sub>3</sub>O<sub>4</sub>) and its heterophase interface with copper oxide (Cu-Co<sub>3</sub>O<sub>4</sub>/CuO) both exhibit over 93% Faraday efficiency for NH<sub>3</sub> synthesis, with a yield reaching up to 59.10 µg h<sup>−1</sup> mg<sub>cat</sub><sup>−1</sup> at −0.4 V versus reversible hydrogen electrode by utilizing simulated industrial NO exhaust (1 vol %) as the feedstock, surpassing those of pure cobalt oxide and some reported catalysts. Theoretical calculations and NO temperature-programmed desorption experiments demonstrate that the incorporation of Cu significantly enhances NO adsorption and reduces the energy barrier of the rate-determining step. The integration of Cu-Co<sub>3</sub>O<sub>4</sub> and Cu-Co<sub>3</sub>O<sub>4</sub>/CuO within the cathode of the Zn–NO battery demonstrates a notable power density of 2.02 mW cm<sup>−2</sup>, highlighting a propitious direction for investigating highly efficient conversion of low-concentration NO exhaust gas.</p>","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"37 34","pages":""},"PeriodicalIF":26.8000,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient Cu─Co Dual-Sites in Cobalt Oxide Nanoboxes for Electrocatalytic Reduction of Low-Concentration NO to NH3\",\"authors\":\"Dongdong Wang, Guilan Fan, Zhihao Pei, Deyan Luan, Xiaojun Gu, Xiong Wen David Lou\",\"doi\":\"10.1002/adma.202504497\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The electrocatalytic conversion of nitric oxide (NO) to ammonia (NH<sub>3</sub>) epitomizes an advanced approach in NH<sub>3</sub> synthesis, crucial for efficiently converting low-concentration industrial NO exhaust and contributing significantly to environmental preservation. Catalyst design remains one pivotal element in addressing this challenge. Here, efficient Cu─Co dual active sites embedded in hollow cobalt oxide nanoboxes are created for the electrocatalytic low-concentration NO reduction reaction (NORR). Cu-modified cobalt oxide (Cu-Co<sub>3</sub>O<sub>4</sub>) and its heterophase interface with copper oxide (Cu-Co<sub>3</sub>O<sub>4</sub>/CuO) both exhibit over 93% Faraday efficiency for NH<sub>3</sub> synthesis, with a yield reaching up to 59.10 µg h<sup>−1</sup> mg<sub>cat</sub><sup>−1</sup> at −0.4 V versus reversible hydrogen electrode by utilizing simulated industrial NO exhaust (1 vol %) as the feedstock, surpassing those of pure cobalt oxide and some reported catalysts. Theoretical calculations and NO temperature-programmed desorption experiments demonstrate that the incorporation of Cu significantly enhances NO adsorption and reduces the energy barrier of the rate-determining step. The integration of Cu-Co<sub>3</sub>O<sub>4</sub> and Cu-Co<sub>3</sub>O<sub>4</sub>/CuO within the cathode of the Zn–NO battery demonstrates a notable power density of 2.02 mW cm<sup>−2</sup>, highlighting a propitious direction for investigating highly efficient conversion of low-concentration NO exhaust gas.</p>\",\"PeriodicalId\":114,\"journal\":{\"name\":\"Advanced Materials\",\"volume\":\"37 34\",\"pages\":\"\"},\"PeriodicalIF\":26.8000,\"publicationDate\":\"2025-06-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://advanced.onlinelibrary.wiley.com/doi/10.1002/adma.202504497\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Materials","FirstCategoryId":"88","ListUrlMain":"https://advanced.onlinelibrary.wiley.com/doi/10.1002/adma.202504497","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
电催化氧化氮(NO)转化氨(NH3)是一种先进的NH3合成方法,对于高效转化低浓度工业NO废气和环境保护具有重要意义。催化剂设计仍然是解决这一挑战的关键因素。在这里,高效的Cu─Co双活性位点嵌入在空心氧化钴纳米盒中,用于电催化低浓度NO还原反应(NORR)。以模拟工业NO废气(1 vol %)为原料,cu修饰的氧化钴(Cu-Co3O4)及其与氧化铜的异相界面(Cu-Co3O4/CuO)在−0.4 V条件下与可逆氢电极合成NH3的法拉第效率均超过93%,产率高达59.10µg h−1 mgcat−1,超过了纯氧化钴和一些报道的催化剂。理论计算和NO程序升温解吸实验表明,Cu的加入显著增强了NO吸附,降低了速率决定步骤的能垒。Cu-Co3O4和Cu-Co3O4/CuO在Zn-NO电池正极内的集成显示出显著的功率密度为2.02 mW cm - 2,为研究低浓度NO废气的高效转化提供了有利的方向。
Efficient Cu─Co Dual-Sites in Cobalt Oxide Nanoboxes for Electrocatalytic Reduction of Low-Concentration NO to NH3
The electrocatalytic conversion of nitric oxide (NO) to ammonia (NH3) epitomizes an advanced approach in NH3 synthesis, crucial for efficiently converting low-concentration industrial NO exhaust and contributing significantly to environmental preservation. Catalyst design remains one pivotal element in addressing this challenge. Here, efficient Cu─Co dual active sites embedded in hollow cobalt oxide nanoboxes are created for the electrocatalytic low-concentration NO reduction reaction (NORR). Cu-modified cobalt oxide (Cu-Co3O4) and its heterophase interface with copper oxide (Cu-Co3O4/CuO) both exhibit over 93% Faraday efficiency for NH3 synthesis, with a yield reaching up to 59.10 µg h−1 mgcat−1 at −0.4 V versus reversible hydrogen electrode by utilizing simulated industrial NO exhaust (1 vol %) as the feedstock, surpassing those of pure cobalt oxide and some reported catalysts. Theoretical calculations and NO temperature-programmed desorption experiments demonstrate that the incorporation of Cu significantly enhances NO adsorption and reduces the energy barrier of the rate-determining step. The integration of Cu-Co3O4 and Cu-Co3O4/CuO within the cathode of the Zn–NO battery demonstrates a notable power density of 2.02 mW cm−2, highlighting a propitious direction for investigating highly efficient conversion of low-concentration NO exhaust gas.
期刊介绍:
Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.