Meng Ge1, Yanzhi Wang2, Francesco Carraro3, Weibin Liang4, Morteza Roostaeinia5, Samira Siahrostami5, Davide M Proserpio6,7, Christian Doonan4, Paolo Falcaro3, Haoquan Zheng2, Xiaodong Zou1, Zhehao Huang1. 1. Department of Materials and Environmental Chemistry, Stockholm University, 10691, Stockholm, Sweden. 2. Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an, 710119, China. 3. Institute of Physical and Theoretical Chemistry, Graz University of Technology, Stremayrgasse 9, 8010, Graz, Austria. 4. Department of Chemistry and the Centre for Advanced Nanomaterials, The University of Adelaide, Adelaide, 5005, South Australia, Australia. 5. Department of Chemistry, University of Calgary, 2500 University Drive NW, Calgary, Alberta, T2N1N4, Canada. 6. Dipartimento di Chimica, Università degli Studi di Milano, 20133, Milano, Italy. 7. Samara Center for Theoretical Materials Science (SCTMS), Samara State Technical University, Samara, 443100, Russia.
Abstract
Metal-organic frameworks (MOFs) are known for their versatile combination of inorganic building units and organic linkers, which offers immense opportunities in a wide range of applications. However, many MOFs are typically synthesized as multiphasic polycrystalline powders, which are challenging for studies by X-ray diffraction. Therefore, developing new structural characterization techniques is highly desired in order to accelerate discoveries of new materials. Here, we report a high-throughput approach for structural analysis of MOF nano- and sub-microcrystals by three-dimensional electron diffraction (3DED). A new zeolitic-imidazolate framework (ZIF), denoted ZIF-EC1, was first discovered in a trace amount during the study of a known ZIF-CO3 -1 material by 3DED. The structures of both ZIFs were solved and refined using 3DED data. ZIF-EC1 has a dense 3D framework structure, which is built by linking mono- and bi-nuclear Zn clusters and 2-methylimidazolates (mIm- ). With a composition of Zn3 (mIm)5 (OH), ZIF-EC1 exhibits high N and Zn densities. We show that the N-doped carbon material derived from ZIF-EC1 is a promising electrocatalyst for oxygen reduction reaction (ORR). The discovery of this new MOF and its conversion to an efficient electrocatalyst highlights the power of 3DED in developing new materials and their applications.
Metal-organic frameworks (MOFs) are known for their versatile n class="Chemical">combination of inorganic building units and organic linkers, which offers immense opportunities in a wide range of applications. However, many MOFs are typically synthesized as multiphasic polycrystalline powders, which are challenging for studies by X-ray diffraction. Therefore, developing new structural characterization techniques is highly desired in order to accelerate discoveries of new materials. Here, we report a high-throughput approach for structural analysis of MOF nano- and sub-microcrystals by three-dimensional electron diffraction (3DED). A new zeolitic-imidazolate framework (ZIF), denoted ZIF-EC1, was first discovered in a trace amount during the study of a known ZIF-CO3 -1 material by 3DED. The structures of both ZIFs were solved and refined using 3DED data. ZIF-EC1 has a dense 3D framework structure, which is built by linking mono- and bi-nuclear Zn clusters and 2-methylimidazolates (mIm- ). With a composition of Zn3 (mIm)5 (OH), ZIF-EC1 exhibits high N and Zn densities. We show that the N-doped carbon material derived from ZIF-EC1 is a promising electrocatalyst for oxygen reduction reaction (ORR). The discovery of this new MOF and its conversion to an efficient electrocatalyst highlights the power of 3DED in developing new materials and their applications.
Keywords:
continuous rotation electron diffraction; electrocatalysis; high throughput structural analysis; metal-organic frameworks; three-dimensional electron diffraction
Authors: Julian T C Wennmacher; Soheil Mahmoudi; Przemyslaw Rzepka; Sung Sik Lee; Tim Gruene; Vladimir Paunović; Jeroen A van Bokhoven Journal: Angew Chem Int Ed Engl Date: 2022-05-25 Impact factor: 16.823