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Pd3 cluster catalysis: Compelling evidence from in operando spectroscopic, kinetic, and density functional theory studies

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Nano Research 2016年第9期9卷 2544-2550页

作者： Chunlin Lv Hao Cheng Wei He Muhammad Ishaq Ali Shah Congqiao Xu Xiangjian Meng Lei Jiao Shiqiang Wei Jun Li Lei Liu Yadong Li Department of Chemistry and Collaborative Innovation Center for Nanomaterial Science and Engineering Tsinghua UniversityBeijing 100084China Tsinghua-Peking Center for Life Sciences Tsinghua UniversityBeijing 100084China National Synchrotron Radiation Laboratory and Collaborative Innovation Center for Nanomaterial Science and Engineering University of Science and Technology of ChinaHefei 230029China

Identification of metal cluster catalysis is a topic that is being investigated since a long time. Here, we report a Pd3 metal cluster catalytic reaction investigated by means of operando studies. We discovered that atomically defined tri-nuclear palladium (Pd3) is a surprisingly active catalyst for the cycloisomerization of 2-phenylethynylaniline. operando1H NMR spectroscopy and X-ray extended absorption fine structure (EXAFS) measurements have indicated that the structural integrity of such a catalyst remains intact throughout the reaction, which has also been confirmed by an ex situ X-ray photoelectron spectroscopy (XPS) study and catalyst recycling experiments. Kinetic data derived from operando IR spectroscopy measurements have shown that Pd3is the active catalytic species. Density functional theory calculations have revealed a reaction pathway consistent with the kinetic data, further supported by NMR titration and X-ray crystal structure studies. Overall, the present study presents a clear example of metal cluster catalysis. [Figure not available: see fulltext.] © 2016, Tsinghua University Press and Springer-Verlag Berlin Heidelberg.

关键词： metal cluster catalysis operando studies active species cycloisomerization palladium

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Characterization of porous cobalt hexacyanoferrate and activated carbon electrodes under dynamic polarization conditions in a sodium-ion pseudocapacitor

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Journal of Energy Chemistry 2021年第3期30卷 53-62页

作者： Bruno Morandi Pires Willian Goncalves Nunes Bruno Guilherme Freitas Francisca Elenice Rodrigues Oliveira Vera Katic Cristiane Barbieri Rodella Leonardo Morais Da Silva Hudson Zanin Advanced Energy Storage Division Manufacturing CroupCarbon Sci-Tech LabsCenter for Innovation on New EnergiesUniversity of CampinasCampinas 13083-852SPBrazil Brazilian Synchrotron Light Laboratory(LNLS/Brazilian Center of Energy and Materiab(CNPEM)) Campinas 13083-970SPBrazil Department of Chemistry Laboratory of Fundamental and Applied ElectrochemistryFederal University of Jequitinhonha and Mucuri's VatleyAlto dajacuba 39100-000Diamantina-MGBrazil

We report here the activated carbon and cobalt hexacyanoferrate composite,which is applied as the electrode materials in symmetric supercapacitors containing a 1.0 M Na_(2)SO_(4) aqueous *** novel material combines high specific surface area and electrochemical stability of activated carbon with the redox properties of cobalt hexacyanoferrate,resulting in maximum specific capacitance of 329 F g^(-1) with large voltage working window of 2.0 *** studies indicated that cobalt hexacyanoferrate introduces important pseudocapacitive properties accounting for the overall charge-storage process,especially when I<0.5 A g^(-1).At lower gravimetric currents(e.g.,0.05 A g^(-1))and up to 1.0 V,the presence of cobalt hexacyanoferrate improves the specific energy for more than 300%.In addition,to better understanding the energy storage process we also provided a careful investigation of the electrode materials under dynamic polarization conditions using the in situ Raman spectroscopy and synchrotron light Xray diffraction *** complementary findings were obtained in these *** believe that this novel electrode material is promising for applications regarding the energy-storage process in pseudocapacitors with long lifespan properties.

关键词： operando studies Raman XRD synchrotron light Cobalt hexacyanoferrate Activated carbon High specific capacitance

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