{"title":"强Cu-O-Si界面稳定cuσ+在高效电催化乙炔半加氢中的作用","authors":"Xiaoli Jiang, Wangxin Ge, Yu Fan, Xuedi Sheng, Hongliang Jiang, Chunzhong Li","doi":"10.1002/aic.18663","DOIUrl":null,"url":null,"abstract":"The development of a high-performance electrocatalytic acetylene semi-hydrogenation catalyst is the key to the selective removal of acetylene from industrial ethylene gas and non-oil route to ethylene production. However, it is still hampered by the deactivation of the catalyst and hydrogen evolution interference. Here, we proposed an interface engineering strategy involving the Cu and cupric oxide nanoparticles dispersed on amorphous SiO<sub>2</sub> (Cu/CuO<sub><i>x</i></sub>/SiO<sub>2</sub>) by a simple stöber method. x-ray photoelectron spectroscopy demonstrated the strong interfacial interaction between cupric oxide nanoparticles and SiO<sub>2</sub>. The formed Cu-O-Si interface stabilized the Cu<sup>σ+</sup> at high reduction potentials, thus improving the activity and stability of the acetylene reduction reaction, as confirmed by in situ Raman spectroscopy. Consequently, the electrochemical test results showed that at 0.5 M KHCO<sub>3</sub>, the maximum Faraday efficiency (FE) of ethylene on the optimized Cu/CuO<sub><i>x</i></sub>/SiO<sub>2</sub> reached 96%. And ethylene FE remains above 85% at −100 mA cm<sup>−2</sup> for 40 h.","PeriodicalId":120,"journal":{"name":"AIChE Journal","volume":"196 1","pages":""},"PeriodicalIF":3.5000,"publicationDate":"2024-11-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Stabilization of cuσ+ via strong Cu-O-Si interface for efficient electrocatalytic acetylene semi-hydrogenation\",\"authors\":\"Xiaoli Jiang, Wangxin Ge, Yu Fan, Xuedi Sheng, Hongliang Jiang, Chunzhong Li\",\"doi\":\"10.1002/aic.18663\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The development of a high-performance electrocatalytic acetylene semi-hydrogenation catalyst is the key to the selective removal of acetylene from industrial ethylene gas and non-oil route to ethylene production. However, it is still hampered by the deactivation of the catalyst and hydrogen evolution interference. Here, we proposed an interface engineering strategy involving the Cu and cupric oxide nanoparticles dispersed on amorphous SiO<sub>2</sub> (Cu/CuO<sub><i>x</i></sub>/SiO<sub>2</sub>) by a simple stöber method. x-ray photoelectron spectroscopy demonstrated the strong interfacial interaction between cupric oxide nanoparticles and SiO<sub>2</sub>. The formed Cu-O-Si interface stabilized the Cu<sup>σ+</sup> at high reduction potentials, thus improving the activity and stability of the acetylene reduction reaction, as confirmed by in situ Raman spectroscopy. Consequently, the electrochemical test results showed that at 0.5 M KHCO<sub>3</sub>, the maximum Faraday efficiency (FE) of ethylene on the optimized Cu/CuO<sub><i>x</i></sub>/SiO<sub>2</sub> reached 96%. And ethylene FE remains above 85% at −100 mA cm<sup>−2</sup> for 40 h.\",\"PeriodicalId\":120,\"journal\":{\"name\":\"AIChE Journal\",\"volume\":\"196 1\",\"pages\":\"\"},\"PeriodicalIF\":3.5000,\"publicationDate\":\"2024-11-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"AIChE Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1002/aic.18663\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"AIChE Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1002/aic.18663","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
摘要
研制高性能的电催化乙炔半加氢催化剂是实现工业乙烯气体中乙炔选择性脱除和非油制乙烯的关键。然而,催化剂失活和析氢干扰仍然阻碍了这一过程的进行。在这里,我们提出了一种界面工程策略,通过简单的stöber方法将Cu和氧化铜纳米颗粒分散在无定形SiO2 (Cu/CuOx/SiO2)上。x射线光电子能谱表明,氧化铜纳米颗粒与SiO2之间存在较强的界面相互作用。原位拉曼光谱证实,形成的Cu-O-Si界面使Cuσ+稳定在高还原电位,从而提高了乙炔还原反应的活性和稳定性。因此,电化学测试结果表明,在0.5 M KHCO3条件下,优化后的Cu/CuOx/SiO2上乙烯的最大法拉第效率(FE)达到96%。在−100 mA cm−2条件下,乙烯FE保持在85%以上。
Stabilization of cuσ+ via strong Cu-O-Si interface for efficient electrocatalytic acetylene semi-hydrogenation
The development of a high-performance electrocatalytic acetylene semi-hydrogenation catalyst is the key to the selective removal of acetylene from industrial ethylene gas and non-oil route to ethylene production. However, it is still hampered by the deactivation of the catalyst and hydrogen evolution interference. Here, we proposed an interface engineering strategy involving the Cu and cupric oxide nanoparticles dispersed on amorphous SiO2 (Cu/CuOx/SiO2) by a simple stöber method. x-ray photoelectron spectroscopy demonstrated the strong interfacial interaction between cupric oxide nanoparticles and SiO2. The formed Cu-O-Si interface stabilized the Cuσ+ at high reduction potentials, thus improving the activity and stability of the acetylene reduction reaction, as confirmed by in situ Raman spectroscopy. Consequently, the electrochemical test results showed that at 0.5 M KHCO3, the maximum Faraday efficiency (FE) of ethylene on the optimized Cu/CuOx/SiO2 reached 96%. And ethylene FE remains above 85% at −100 mA cm−2 for 40 h.
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