Zuo-Shu Sun , Xue-Yan Xiang , Qiu-Ping Zhao , Zhao Tang , Shi-Yi Jiang , Tong-Bu Lu , Zhi-Ming Zhang , Baifan Wang , Hua-Qing Yin
{"title":"在规模化生产的铁镍合金装饰纳米多孔碳上高效电催化二氧化碳和硝酸盐合成尿素","authors":"Zuo-Shu Sun , Xue-Yan Xiang , Qiu-Ping Zhao , Zhao Tang , Shi-Yi Jiang , Tong-Bu Lu , Zhi-Ming Zhang , Baifan Wang , Hua-Qing Yin","doi":"10.1016/S1872-2067(24)60111-7","DOIUrl":null,"url":null,"abstract":"<div><div>Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis, but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging. Herein, we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts, named FeNi@<em>n</em>C-<em>T</em> (<em>n</em> represents the content of nanoporous carbon as 1, 3, 5, 7 or 9 g and <em>T</em> = 900, 950, 1000 or 1100 °C), for highly performed urea synthesis <em>via</em> NO<sub>3</sub><sup>−</sup> and CO<sub>2</sub> co-reduction. The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h<sup>−1</sup> g<sub>FeNi</sub><sup>−1</sup> with a Faradaic efficiency of 15.56% at –1.2 V <em>vs</em>. RHE. Moreover, the scale-up synthesized FeNi@7C-950-S (over 140 g per batch) was achieved with its high catalytic performance and high stability maintained. Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key *CO and *N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.</div></div>","PeriodicalId":9832,"journal":{"name":"Chinese Journal of Catalysis","volume":"65 ","pages":"Pages 153-162"},"PeriodicalIF":15.7000,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient electrocatalytic urea synthesis from CO2 and nitrate over the scale-up produced FeNi alloy-decorated nanoporous carbon\",\"authors\":\"Zuo-Shu Sun , Xue-Yan Xiang , Qiu-Ping Zhao , Zhao Tang , Shi-Yi Jiang , Tong-Bu Lu , Zhi-Ming Zhang , Baifan Wang , Hua-Qing Yin\",\"doi\":\"10.1016/S1872-2067(24)60111-7\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis, but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging. Herein, we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts, named FeNi@<em>n</em>C-<em>T</em> (<em>n</em> represents the content of nanoporous carbon as 1, 3, 5, 7 or 9 g and <em>T</em> = 900, 950, 1000 or 1100 °C), for highly performed urea synthesis <em>via</em> NO<sub>3</sub><sup>−</sup> and CO<sub>2</sub> co-reduction. The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h<sup>−1</sup> g<sub>FeNi</sub><sup>−1</sup> with a Faradaic efficiency of 15.56% at –1.2 V <em>vs</em>. RHE. Moreover, the scale-up synthesized FeNi@7C-950-S (over 140 g per batch) was achieved with its high catalytic performance and high stability maintained. Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key *CO and *N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.</div></div>\",\"PeriodicalId\":9832,\"journal\":{\"name\":\"Chinese Journal of Catalysis\",\"volume\":\"65 \",\"pages\":\"Pages 153-162\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2024-10-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chinese Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1872206724601117\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chinese Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1872206724601117","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Efficient electrocatalytic urea synthesis from CO2 and nitrate over the scale-up produced FeNi alloy-decorated nanoporous carbon
Electrocatalytic urea synthesis provides a favorable strategy for conventional energy-consuming urea synthesis, but achieving large-scale catalyst synthesis with high catalytic efficiency remains challenging. Herein, we developed a simple method for the preparation of a series of FeNi-alloy-based catalysts, named FeNi@nC-T (n represents the content of nanoporous carbon as 1, 3, 5, 7 or 9 g and T = 900, 950, 1000 or 1100 °C), for highly performed urea synthesis via NO3− and CO2 co-reduction. The FeNi@7C-1000 achieved a high urea yield of 1041.33 mmol h−1 gFeNi−1 with a Faradaic efficiency of 15.56% at –1.2 V vs. RHE. Moreover, the scale-up synthesized FeNi@7C-950-S (over 140 g per batch) was achieved with its high catalytic performance and high stability maintained. Mechanism investigation illuminated that the Ni and Fe sites catalyze and stabilize the key *CO and *N intermediates and minimize the C–N coupling reaction barriers for highly efficient urea synthesis.
期刊介绍:
The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.