Scanning transmission electron microscopy（STEM） has been shown as powerful tools for material characterization,especially after the appearance of aberration-corrector which greatly enhances the resolution of STEM. H...Scanning transmission electron microscopy（STEM） has been shown as powerful tools for material characterization,especially after the appearance of aberration-corrector which greatly enhances the resolution of STEM. High angle annular dark field（HAADF） and annular bright field（ABF） imaging of the aberration-corrected STEM are widely used due to their high-resolution capabilities and easily interpretable image contrasts. However, HAADF mode of the STEM is still limited in detecting light elements due to the weak electron-scattering power. ABF mode of the STEM could detect light and heavy elements simultaneously, providing unprecedented opportunities for probing unknown structures of materials. Atomiclevel structure investigation of materials has been achieved by means of these imaging modes, which is invaluable in many fields for either improving properties of materials or developing new materials. This paper aims to provide a introduction of HAADF and ABF imaging techniques and reviews their applications in characterization of cathode materials, study of electrochemical reaction mechanisms, and exploring the effective design of lithium-ion batteries（LIBs）. The future prospects of the STEM are also discussed.展开更多
为了研究Mg_(97)Gd_(2)Y_(1)合金中β'相的粗化过程以及相关析出结构的形成和演变机制,使用原子分辨的高角度环形暗场-扫描透射电子显微镜(high angle annular dark field scanning transmission electron microscope,HAADF-STEM)...为了研究Mg_(97)Gd_(2)Y_(1)合金中β'相的粗化过程以及相关析出结构的形成和演变机制,使用原子分辨的高角度环形暗场-扫描透射电子显微镜(high angle annular dark field scanning transmission electron microscope,HAADF-STEM)成像技术表征了合金不同时效阶段形成的析出结构,并结合第一性原理计算的方法分析了它们的稳定性.结果表明,相关的β_(F)'、β_(M)和β″相主要在β'相粗化过程的早期形成,它们的形成与β'相相界面周围存在较高的错配应变场密切相关;随着β'相粗化过程的进行,β_(M)和β″相的尺寸和数量逐渐减少,而由β'与β_(F)'相交替组成的竹节状析出物增多,成为合金基体中主要的析出结构;当错配应变足够大时,β_(F)'相内部出现位错,β相在位错处可以形核,并逐渐长大成为基体中主要的平衡析出结构.展开更多
Atomically dispersed catalysts have attracted attention in energy conversion applications because their efficiency and chemoselectivity for special catalysis are superior to those of traditional catalysts. However, th...Atomically dispersed catalysts have attracted attention in energy conversion applications because their efficiency and chemoselectivity for special catalysis are superior to those of traditional catalysts. However, they have limitations owing to the extremely low metal-loading content on supports, difficulty in the precise control of the metal location and amount as well as low stability at high temperatures. We prepared a highly doped single metal atom hybrid via a single-step thermal pyrolysis of glucose, dicyandiamide, and inorganic metal salts. High-angle annular dark field-scanning transmission electron microscopy （HAADF-STEM） and X-ray absorption fine structure spectroscopy （XAFS） revealed that nitrogen atoms doped into the graphene matrix were pivotal for metal atom stabilization by generating a metal-Nx coordination structure. Due to the strong anchoring effect of the graphene matrix, the metal loading content was over 4 wt.% in the isolated atomic hybrid （the Pt content was as high as 9.26 wt.% in the Pt-doped hybrid）. Furthermore, the single iron-doped hybrid （Fe@N-doped graphene） showed a remarkable electrocatalytic performance for the oxygen reduction reaction. The peak power density was - 199 mW·cm-2 at a current density of 310 mA·cm-2 and superior to that of a commercial Pt/C catalyst when it was used as a cathode catalyst in assembled zinc-air batteries. This work offered a feasible approach to design and fabricate highly doped single metal atoms （SMAs） catalysts for potential energy applications.展开更多
基金supported by the National Basic Research Program of China(Grant No.2014CB921002)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB07030200)the National Natural Science Foundation of China(Grant Nos.51522212,51421002,and 51672307)
文摘Scanning transmission electron microscopy（STEM） has been shown as powerful tools for material characterization,especially after the appearance of aberration-corrector which greatly enhances the resolution of STEM. High angle annular dark field（HAADF） and annular bright field（ABF） imaging of the aberration-corrected STEM are widely used due to their high-resolution capabilities and easily interpretable image contrasts. However, HAADF mode of the STEM is still limited in detecting light elements due to the weak electron-scattering power. ABF mode of the STEM could detect light and heavy elements simultaneously, providing unprecedented opportunities for probing unknown structures of materials. Atomiclevel structure investigation of materials has been achieved by means of these imaging modes, which is invaluable in many fields for either improving properties of materials or developing new materials. This paper aims to provide a introduction of HAADF and ABF imaging techniques and reviews their applications in characterization of cathode materials, study of electrochemical reaction mechanisms, and exploring the effective design of lithium-ion batteries（LIBs）. The future prospects of the STEM are also discussed.
文摘为了研究Mg_(97)Gd_(2)Y_(1)合金中β'相的粗化过程以及相关析出结构的形成和演变机制,使用原子分辨的高角度环形暗场-扫描透射电子显微镜(high angle annular dark field scanning transmission electron microscope,HAADF-STEM)成像技术表征了合金不同时效阶段形成的析出结构,并结合第一性原理计算的方法分析了它们的稳定性.结果表明,相关的β_(F)'、β_(M)和β″相主要在β'相粗化过程的早期形成,它们的形成与β'相相界面周围存在较高的错配应变场密切相关;随着β'相粗化过程的进行,β_(M)和β″相的尺寸和数量逐渐减少,而由β'与β_(F)'相交替组成的竹节状析出物增多,成为合金基体中主要的析出结构;当错配应变足够大时,β_(F)'相内部出现位错,β相在位错处可以形核,并逐渐长大成为基体中主要的平衡析出结构.
基金This work is financially supported partly by Ministry of Science and Technology （MOST） （Nos. 2017YFA0303500 and 2014CB848900）, the National Natural Science Foundation of China （NSFC） （Nos. U1532112, 11574280 and 11605201 ）, CAS Interdisciplinary Innovation Team and CAS Key Research Program of Frontier Sciences （No. QYZDB-SSW-SLH018）. L. S. acknowledges the recruitment program of global experts, the CAS Hundred Talent Program and Key Laboratory of Advanced Energy Materials Chemistry （Ministry of Education） Nankai University. We thank the Shanghai Synchrotron Radiation Facility （14W1, SSRF）, the Beijing Synchrotron Radiation Facility （1W1B and soft-X-ray endstation, BSRF）, the Hefei Synchrotron Radiation Facility （Photoemission, MCD and Catalysis/ Surface Science Endstations, NSRL）, and the USTC Center for Micro and Nanoscale Research and Fabrication for helps in characterizations.
文摘Atomically dispersed catalysts have attracted attention in energy conversion applications because their efficiency and chemoselectivity for special catalysis are superior to those of traditional catalysts. However, they have limitations owing to the extremely low metal-loading content on supports, difficulty in the precise control of the metal location and amount as well as low stability at high temperatures. We prepared a highly doped single metal atom hybrid via a single-step thermal pyrolysis of glucose, dicyandiamide, and inorganic metal salts. High-angle annular dark field-scanning transmission electron microscopy （HAADF-STEM） and X-ray absorption fine structure spectroscopy （XAFS） revealed that nitrogen atoms doped into the graphene matrix were pivotal for metal atom stabilization by generating a metal-Nx coordination structure. Due to the strong anchoring effect of the graphene matrix, the metal loading content was over 4 wt.% in the isolated atomic hybrid （the Pt content was as high as 9.26 wt.% in the Pt-doped hybrid）. Furthermore, the single iron-doped hybrid （Fe@N-doped graphene） showed a remarkable electrocatalytic performance for the oxygen reduction reaction. The peak power density was - 199 mW·cm-2 at a current density of 310 mA·cm-2 and superior to that of a commercial Pt/C catalyst when it was used as a cathode catalyst in assembled zinc-air batteries. This work offered a feasible approach to design and fabricate highly doped single metal atoms （SMAs） catalysts for potential energy applications.
