Paick Jihun, Hong Seunghee, Bae Ji-Young, Jyoung Jy-Young, Lee Eun-Sook, Lee Doohwan
Department of Chemical Engineering, The University of Seoul, Siripdae-gil 13, Jeonnong-dong, Seoul 02504, Republic of Korea.
JNTG Co., Ltd., 240-11 Naehyangan-gil, Jeongnam-myeon, Hwaseong-si, Gyeonggi-do 18523, Republic of Korea.
ACS Omega. 2023 Jun 14;8(25):22646-22655. doi: 10.1021/acsomega.3c01305. eCollection 2023 Jun 27.
Atomic nitrogen doping on CeO nanoparticles (NPs) by an efficient and environmentally benign urea thermolysis approach is first studied, and its effects on the intrinsic scavenging activity of the CeO NPs for reactive oxygen radicals are investigated. The N-doped CeO (N-CeO) NPs, characterized by X-ray photoelectron and Raman spectroscopy analyses, showed considerably high levels of N atomic doping (2.3-11.6%), accompanying with an order of magnitude increase of the lattice oxygen vacancies on the CeO crystal surface. The radical scavenging properties of the N-CeO NPs are characterized by applying Fenton's reaction with collective and quantitative kinetic analysis. The results revealed that the significant increase of surface oxygen vacancies is the leading cause for the enhancements of radical scavenging properties by the N doping of CeO NPs. Enriched with abundant surface oxygen vacancies, the N-CeO NPs prepared by urea thermolysis provided about 1.4-2.5 times greater radical scavenging properties than the pristine CeO. The collective kinetic analysis revealed that the surface-area-normalized intrinsic radical scavenging activity of the N-CeO NPs is about 6- to 8-fold greater than that of the pristine CeO NPs. The results suggest the high effectiveness of the N doping of CeO by the environmentally benign urea thermolysis approach to enhance the radical scavenging activity of CeO NPs for extensive applications such as that in polymer electrolyte membrane fuel cells.
首次研究了通过高效且环境友好的尿素热解方法在CeO纳米颗粒(NPs)上进行原子氮掺杂,并研究了其对CeO NPs清除活性氧自由基的固有活性的影响。通过X射线光电子能谱和拉曼光谱分析表征的N掺杂CeO(N-CeO)NPs显示出相当高的N原子掺杂水平(2.3-11.6%),同时CeO晶体表面的晶格氧空位增加了一个数量级。通过应用Fenton反应并进行集体和定量动力学分析来表征N-CeO NPs的自由基清除特性。结果表明,表面氧空位的显著增加是CeO NPs通过N掺杂提高自由基清除特性的主要原因。通过尿素热解制备的N-CeO NPs富含大量表面氧空位,其自由基清除特性比原始CeO高约1.4-2.5倍。集体动力学分析表明,N-CeO NPs的表面积归一化固有自由基清除活性比原始CeO NPs高约6至8倍。结果表明,通过环境友好的尿素热解方法对CeO进行N掺杂以提高CeO NPs的自由基清除活性具有很高的有效性,可广泛应用于聚合物电解质膜燃料电池等领域。