Metal-Organic Frameworks Offering Tunable Binary Active Sites toward HighlyEfficient Urea Oxidation Electrolysis
作者机构：School of Optical and Electronic InformationWuhan National Laboratory for OptoelectronicsOptics Valley LaboratoryHuazhong University of Science and TechnologyWuhan 430074China Physics Department and Jiangsu Key Laboratory for Chemistry of Low-Dimensional MaterialsHuaiyin Normal UniversityHuaian 223300China Center for Reliability Science and TechnologiesChang Gung UniversityTaoyuan33302 TaiwanChina School of Chemistry and Materials ScienceUniversity of Science and Technology of ChinaHefei230026 AnhuiChina Department of PhysicsCollege of ScienceShihezi UniversityXinjang 832003China Department of Applied PhysicsGhent UniversityGent 9000Belgium
出 版 物：《Research》 (研究（英文）)
年 卷 期：2022年第2022卷第4期
页 面：309-320页
核心收录：
学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学]
基 金：This work is finically supported by the National Key R&D Program of China(Grant No.2017YFE0120500) the National Natural Science Foundation of China(Grant Nos.51972129,21725102) the Bintuan Science and Technology Program(Grant Nos.2020DB002,2022DB009) the Key Research and Development Program of Hubei(Grant No.2020BAB079) the Science and Technology Innovation Committee Foundation of Shenzhen(Grant No.JCYJ20210324141613032) the Natural Science Foundation of Jiangsu Province of China(BK20211609)
摘 要：Electrocatalytic urea oxidation reaction(UOR)is regarded as an effective yet challenging approach for the degradation of urea in wastewater into harmless N2 and CO_(2).To overcome the sluggish kinetics,catalytically active sites should be rationally designed to maneuver the multiple key steps of intermediate adsorption and ***,we demonstrate that metal-organic frameworks(MOFs)can provide an ideal platform for tailoring binary active sites to facilitate the rate-determining steps,achieving remarkable electrocatalytic activity toward ***,the MOF(namely,NiMn_(0.14)-BDC)based on Ni/Mn sites and terephthalic acid(BDC)ligands exhibits a low voltage of 1.317 V to deliver a current density of 10 mA cm^(-2).As a result,a high turnover frequency(TOF)of 0.15 s^(-1) is achieved at a voltage of 1.4 V,which enables a urea degradation rate of 81.87%in 0.33 M urea *** combination of experimental characterization with theoretical calculation reveals that the Ni and Mn sites play synergistic roles in maneuvering the evolution of urea molecules and key reaction intermediates during the UOR,while the binary Ni/Mn sites in MOF offer the tunability for electronic structure and d-band center impacting on the intermediate *** work provides important insights into active site design by leveraging MOF platform and represents a solid step toward highly efficient UOR with MOF-based electrocatalysts.
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