{"title":"选择性电还原CO2为增值化学品的碲化钴电催化剂","authors":"Apurv Saxena, Harish Singh, Manashi Nath","doi":"10.1007/s40243-022-00211-6","DOIUrl":null,"url":null,"abstract":"<div><p>Recent emphasis on carbon dioxide utilization has necessitated the exploration of different catalyst compositions other than copper-based systems that can significantly improve the activity and selectivity towards specific CO<sub>2</sub> reduction products at low applied potential. In this study, a binary CoTe has been reported as an efficient electrocatalyst for CO<sub>2</sub> reduction in aqueous medium under ambient conditions at neutral pH. CoTe showed high Faradaic efficiency and selectivity of 86.83 and 75%, respectively, for acetic acid at very low potential of − 0.25 V vs RHE. More intriguingly, C1 products like formic acid was formed preferentially at slightly higher applied potential achieving high formation rate of 547.24 μmol cm<sup>−2</sup> h<sup>−1</sup> at − 1.1 V vs RHE. CoTe showed better CO2RR activity when compared with Co<sub>3</sub>O<sub>4</sub>, which can be attributed to the enhanced electrochemical activity of the catalytically active transition metal center as well as improved intermediate adsorption on the catalyst surface. While reduced anion electronegativity and improved lattice covalency in tellurides enhance the electrochemical activity of Co, high d-electron density improves the intermediate CO adsorption on the catalyst site leading to CO<sub>2</sub> reduction at lower applied potential and high selectivity for C<sub>2</sub> products. CoTe also shows stable CO2RR catalytic activity for 50 h and low Tafel slope (50.3 mV dec<sup>–1</sup>) indicating faster reaction kinetics and robust functionality. Selective formation of value-added C<sub>2</sub> products with low energy expense can make these catalysts potentially viable for integration with other CO<sub>2</sub> capture technologies thereby, helping to close the carbon loop.</p></div>","PeriodicalId":692,"journal":{"name":"Materials for Renewable and Sustainable Energy","volume":"11 2","pages":"115 - 129"},"PeriodicalIF":3.6000,"publicationDate":"2022-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s40243-022-00211-6.pdf","citationCount":"6","resultStr":"{\"title\":\"Cobalt telluride electrocatalyst for selective electroreduction of CO2 to value-added chemicals\",\"authors\":\"Apurv Saxena, Harish Singh, Manashi Nath\",\"doi\":\"10.1007/s40243-022-00211-6\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Recent emphasis on carbon dioxide utilization has necessitated the exploration of different catalyst compositions other than copper-based systems that can significantly improve the activity and selectivity towards specific CO<sub>2</sub> reduction products at low applied potential. In this study, a binary CoTe has been reported as an efficient electrocatalyst for CO<sub>2</sub> reduction in aqueous medium under ambient conditions at neutral pH. CoTe showed high Faradaic efficiency and selectivity of 86.83 and 75%, respectively, for acetic acid at very low potential of − 0.25 V vs RHE. More intriguingly, C1 products like formic acid was formed preferentially at slightly higher applied potential achieving high formation rate of 547.24 μmol cm<sup>−2</sup> h<sup>−1</sup> at − 1.1 V vs RHE. CoTe showed better CO2RR activity when compared with Co<sub>3</sub>O<sub>4</sub>, which can be attributed to the enhanced electrochemical activity of the catalytically active transition metal center as well as improved intermediate adsorption on the catalyst surface. While reduced anion electronegativity and improved lattice covalency in tellurides enhance the electrochemical activity of Co, high d-electron density improves the intermediate CO adsorption on the catalyst site leading to CO<sub>2</sub> reduction at lower applied potential and high selectivity for C<sub>2</sub> products. CoTe also shows stable CO2RR catalytic activity for 50 h and low Tafel slope (50.3 mV dec<sup>–1</sup>) indicating faster reaction kinetics and robust functionality. 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引用次数: 6
摘要
最近对二氧化碳利用的重视,使得探索除铜基系统以外的不同催化剂组成成为必要。铜基系统可以在低应用潜力下显著提高对特定二氧化碳还原产物的活性和选择性。在本研究中,在中性ph的环境条件下,二元CoTe作为一种高效的电催化剂在水介质中还原CO2。在−0.25 V vs RHE的极低电位下,CoTe对乙酸的法拉第效率和选择性分别为86.83%和75%。更有趣的是,甲酸等C1产物在稍高的施加电位下优先生成,在−1.1 V vs RHE下,生成率高达547.24 μmol cm−2 h−1。与Co3O4相比,CoTe表现出更好的CO2RR活性,这可以归因于具有催化活性的过渡金属中心的电化学活性增强以及催化剂表面对中间体的吸附改善。虽然碲中阴离子电负性的降低和晶格共价的提高提高了Co的电化学活性,但高d-电子密度提高了Co在催化剂上的中间吸附,从而在较低的应用电位下还原CO2,提高了C2产物的选择性。CoTe还表现出50小时稳定的CO2RR催化活性和低Tafel斜率(50.3 mV dec1),表明更快的反应动力学和强大的功能。选择性形成低能耗的增值C2产品可以使这些催化剂与其他二氧化碳捕获技术相结合,从而有助于关闭碳循环。
Cobalt telluride electrocatalyst for selective electroreduction of CO2 to value-added chemicals
Recent emphasis on carbon dioxide utilization has necessitated the exploration of different catalyst compositions other than copper-based systems that can significantly improve the activity and selectivity towards specific CO2 reduction products at low applied potential. In this study, a binary CoTe has been reported as an efficient electrocatalyst for CO2 reduction in aqueous medium under ambient conditions at neutral pH. CoTe showed high Faradaic efficiency and selectivity of 86.83 and 75%, respectively, for acetic acid at very low potential of − 0.25 V vs RHE. More intriguingly, C1 products like formic acid was formed preferentially at slightly higher applied potential achieving high formation rate of 547.24 μmol cm−2 h−1 at − 1.1 V vs RHE. CoTe showed better CO2RR activity when compared with Co3O4, which can be attributed to the enhanced electrochemical activity of the catalytically active transition metal center as well as improved intermediate adsorption on the catalyst surface. While reduced anion electronegativity and improved lattice covalency in tellurides enhance the electrochemical activity of Co, high d-electron density improves the intermediate CO adsorption on the catalyst site leading to CO2 reduction at lower applied potential and high selectivity for C2 products. CoTe also shows stable CO2RR catalytic activity for 50 h and low Tafel slope (50.3 mV dec–1) indicating faster reaction kinetics and robust functionality. Selective formation of value-added C2 products with low energy expense can make these catalysts potentially viable for integration with other CO2 capture technologies thereby, helping to close the carbon loop.
期刊介绍:
Energy is the single most valuable resource for human activity and the basis for all human progress. Materials play a key role in enabling technologies that can offer promising solutions to achieve renewable and sustainable energy pathways for the future.
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