期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 307, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121164
关键词
in-situ liquid phase TEM; Transformation mechanism; MOFs-based derivative; CO2 reduction reaction
资金
- National Natural Science Foundation of China [91934303, 21991151, 21991150, 21673198]
- National Key Research and Development Program of China [2017YFA0206500]
The nanoscale transformation processes of MOFs derivatives were directly observed using in-situ liquid phase TEM, revealing the unexpected nanobubble stability controlled mechanism of ZIF-67 transition to Co-TMH. This study provides new insights and methods for the synthesis and catalytic performance of porous Co-TMH.
Materials derived from MOFs have great potentials in energy conversion. However, the nanoscale transformation processes of MOFs derivatives remain unknown. Herein, by using in-situ liquid phase TEM, we directly visualize the MOFs etching processes. For the first time, unexpected nanobubble stability controlled transformation mechanism of ZIF-67 to porous or layered cobalt transition metal hydroxide (Co-TMH) is identified. Voids in MOFs migrate and merge to form nanobubbles due to structural collapse. Under slow diffusion conditions, nanobubbles move slowly and Co-TMH clusters generate on the nanobubble interface, further favoring the formation of internal nanocages and porous structures. On the other hand, a fast diffusion leads to rapid nanobubbles generation, aggregation and reshaping, inducing layered structure formation. Inspired by in-situ observation, we further synthesize porous Co-TMH at -80 degrees C under inhibited diffusion conditions, which exhibits excellent catalytic performance on CO2 reduction reaction.
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