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Unraveling the Dynamic Structural Evolution of Phthalocyanine Catalysts during CO2 Electroreduction
Jianing Mao, Bingbao Mei*, Ji Li, Shuai Yang, Fanfei Sun, Siyu Lu, Wei Chen, Fei Song* and Zheng Jiang*

Phthalocyanine catalysts have well-defined active site structures that allow reaction-based mechanism exploration. In this regard, the actual behaviors of metal ions in the phthalocyanine catalysts have aroused considerable attention. Operando high-energy resolution fluorescence detected X-ray absorption (HERFD-XANES) can be employed in the practical situation of electrocatalysis to realize the interfacial interaction between metal ions and the reactants, offering a unique insight into the active site geometry and structural evolution during CO2 reduction. In this work, the CO2RR to CO dominates over the HER with Faradaic efficiency reaching the maximum value of 89% at 0.85 V versus RHE. The results demonstrate the atomically dispersed, low-valent Ni(I) centres with high intrinsic CO2 reduction activity.

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In-Situ HP-STM and Operando EC-STM Studies of Heterogeneous Catalysis at Interfaces

Lei Xie*, Chaoqin Huang, Zhaofeng Liang, Hongbing Wang, Zheng Jiang and Fei Song*

Chin. J. Struct. Chem. 2022, 41, 2210029-2210044  DOI: 10.14102/j.cnki.0254-5861.2022-0136

October 25, 2022

HP-STM, EC-STM, heterogeneous catalysis, in-situ, operando, interfaces

ABSTRACT

Heterogeneous catalysis taking place at solid interfaces plays a crucial role not only in industrial chemical production, energy conversion but also in fundamental research. The dynamic evolution of surface morphology and composition requires full understanding especially under realistic reaction conditions. To this end, conventional scanning tunneling microscopy (STM) has been integrated with high pressure cell and electrochemical cell, forming high pressure (HP) STM and electrochemical (EC) STM for the in-situ/operando characterization at solid-gas and solid-liquid interfaces with atomic resolution, respectively. In this review, we attempt to give a brief introduction to the development and working principle of these two techniques and subsequently summarize several representative progresses in recent days. The dynamic changes in active sites, surface reconstruction, absorbates alteration and products formation are directly characterized in a combination with other surface sensitive technologies. The correlation between surface structures and catalytic performance as well as the underlying mechanism can thus be unraveled, which provides insights into the rational design and optimization of catalysts.

                     


                                  



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