{"title":"Ni1Mn1合金的相偏析有利于尿素的电解","authors":"Huasen Wang, Weichang Li, Lingxuan Meng, Qinyu Tang, Lixin Zhang, Yu Ding, Chunsheng Li, Yan Sun, Huimin Wu","doi":"10.1016/j.cej.2024.158950","DOIUrl":null,"url":null,"abstract":"To alleviate urea wastewater pollution and achieve sustainable hydrogen production, development of highly active, low-cost, and stable bifunctional catalysts is urgently required. Using a deposition method, Ni<sub>x</sub>Mn<sub>y</sub>/NF (x = 1, y = 1) alloy materials were successfully synthesized, which can effectively generate hydrogen across the full pH range. The overpotentials (η<sub>100</sub>) of Ni<sub>1</sub>Mn<sub>1</sub>/NF in alkaline, acidic, and neutral solutions were 197, 261, and 338 mV, respectively. During the urea oxidation reaction (UOR), HRTEM, XPS, and in-situ Raman results confirmed that the NiMn alloy undergoes reconstruction into a highly active composite structure NiMn/NiMnOOH, achieving an η<sub>100</sub> of just 1.384 V. Density functional theory (DFT) indicates that Mn incorporation optimizes intermediate adsorption (Urea*)/desorption (CO<sub>2</sub>*), accelerating the deprotonation rate of the CONHN* intermediate (rate-determining step, RDS), thus enhancing catalytic activity. Notably, in the dual-electrode electrolyzer composed of Ni<sub>1</sub>Mn<sub>1</sub>/NF, the cell voltage in the overall human urine electrolysis system (HOUS) is 1.724 V@100 mA cm<sup>−2</sup>, which is approximately 333 mV lower than that in the overall water electrolysis system (OWS). Compared to recent studies, Ni<sub>1</sub>Mn<sub>1</sub>/NF demonstrates better catalytic activity and stability. This work presents a fresh perspective on catalyst design for mitigating urine pollution and enabling efficient hydrogen production.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"23 1","pages":""},"PeriodicalIF":13.2000,"publicationDate":"2024-12-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Phase segregation of Ni1Mn1 alloy enable efficient for urea electrolysis\",\"authors\":\"Huasen Wang, Weichang Li, Lingxuan Meng, Qinyu Tang, Lixin Zhang, Yu Ding, Chunsheng Li, Yan Sun, Huimin Wu\",\"doi\":\"10.1016/j.cej.2024.158950\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"To alleviate urea wastewater pollution and achieve sustainable hydrogen production, development of highly active, low-cost, and stable bifunctional catalysts is urgently required. Using a deposition method, Ni<sub>x</sub>Mn<sub>y</sub>/NF (x = 1, y = 1) alloy materials were successfully synthesized, which can effectively generate hydrogen across the full pH range. The overpotentials (η<sub>100</sub>) of Ni<sub>1</sub>Mn<sub>1</sub>/NF in alkaline, acidic, and neutral solutions were 197, 261, and 338 mV, respectively. During the urea oxidation reaction (UOR), HRTEM, XPS, and in-situ Raman results confirmed that the NiMn alloy undergoes reconstruction into a highly active composite structure NiMn/NiMnOOH, achieving an η<sub>100</sub> of just 1.384 V. Density functional theory (DFT) indicates that Mn incorporation optimizes intermediate adsorption (Urea*)/desorption (CO<sub>2</sub>*), accelerating the deprotonation rate of the CONHN* intermediate (rate-determining step, RDS), thus enhancing catalytic activity. Notably, in the dual-electrode electrolyzer composed of Ni<sub>1</sub>Mn<sub>1</sub>/NF, the cell voltage in the overall human urine electrolysis system (HOUS) is 1.724 V@100 mA cm<sup>−2</sup>, which is approximately 333 mV lower than that in the overall water electrolysis system (OWS). Compared to recent studies, Ni<sub>1</sub>Mn<sub>1</sub>/NF demonstrates better catalytic activity and stability. This work presents a fresh perspective on catalyst design for mitigating urine pollution and enabling efficient hydrogen production.\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":\"23 1\",\"pages\":\"\"},\"PeriodicalIF\":13.2000,\"publicationDate\":\"2024-12-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.cej.2024.158950\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2024.158950","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Phase segregation of Ni1Mn1 alloy enable efficient for urea electrolysis
To alleviate urea wastewater pollution and achieve sustainable hydrogen production, development of highly active, low-cost, and stable bifunctional catalysts is urgently required. Using a deposition method, NixMny/NF (x = 1, y = 1) alloy materials were successfully synthesized, which can effectively generate hydrogen across the full pH range. The overpotentials (η100) of Ni1Mn1/NF in alkaline, acidic, and neutral solutions were 197, 261, and 338 mV, respectively. During the urea oxidation reaction (UOR), HRTEM, XPS, and in-situ Raman results confirmed that the NiMn alloy undergoes reconstruction into a highly active composite structure NiMn/NiMnOOH, achieving an η100 of just 1.384 V. Density functional theory (DFT) indicates that Mn incorporation optimizes intermediate adsorption (Urea*)/desorption (CO2*), accelerating the deprotonation rate of the CONHN* intermediate (rate-determining step, RDS), thus enhancing catalytic activity. Notably, in the dual-electrode electrolyzer composed of Ni1Mn1/NF, the cell voltage in the overall human urine electrolysis system (HOUS) is 1.724 V@100 mA cm−2, which is approximately 333 mV lower than that in the overall water electrolysis system (OWS). Compared to recent studies, Ni1Mn1/NF demonstrates better catalytic activity and stability. This work presents a fresh perspective on catalyst design for mitigating urine pollution and enabling efficient hydrogen production.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.