An Sufeng, Zhang Guanghui, Wang Tingwen, Zhang Wenna, Li Keyan, Song Chunshan, Miller Jeffrey T, Miao Shu, Wang Junhu, Guo Xinwen
State Key Laboratory of Fine Chemicals, PSU-DUT Joint Center for Energy Research, School of Chemical Engineering , Dalian University of Technology , Dalian 116024 , PR China.
Davidson School of Chemical Engineering , Purdue University , West Lafayette , Indiana 47907 , United States.
ACS Nano. 2018 Sep 25;12(9):9441-9450. doi: 10.1021/acsnano.8b04693. Epub 2018 Sep 10.
Ultra-small metal clusters have attracted great attention owing to their superior catalytic performance and extensive application in heterogeneous catalysis. However, the synthesis of high-density metal clusters is very challenging due to their facile aggregation. Herein, one-step pyrolysis was used to synthesize ultra-small clusters and single-atom Fe sites embedded in graphitic carbon nitride with high density (iron loading up to 18.2 wt %), evidenced by high-angle annular dark field-scanning transmission electron microscopy, X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and Fe Mössbauer spectroscopy. The catalysts exhibit enhanced activity and stability in degrading various organic samples in advanced oxidation processes. The drastically increased metal site density and stability provide useful insights into the design and synthesis of cluster catalysts for practical application in catalytic oxidation reactions.
超小金属簇因其优异的催化性能和在多相催化中的广泛应用而备受关注。然而，由于其易于聚集，合成高密度金属簇极具挑战性。在此，采用一步热解法合成了嵌入石墨相氮化碳中的高密度超小簇和单原子铁位点（铁负载量高达18.2 wt%），这通过高角度环形暗场扫描透射电子显微镜、X射线吸收光谱、X射线光电子能谱和Fe穆斯堡尔谱得到证实。这些催化剂在高级氧化过程中降解各种有机样品时表现出增强的活性和稳定性。金属位点密度和稳定性的大幅提高为用于催化氧化反应实际应用的簇催化剂的设计和合成提供了有用的见解。
