journal article·2024-06

Constructing Asymmetric Charge Polarized NiCo Prussian Blue Analogue for Promoted Electrocatalytic Methanol to Formate Conversion

Yunxiang Lin, Yan‐ge Wang, Xiaoyu Li, Jiahui Zhao, Hengjie Liu, Chuanqiang Wu, Li Yang, Guang Li, Zeming Qi, Lei Shan, Yong Jiang, Li Song

Small· Volume 20· Issue 23
Publisher page

Abstract

Abstract The highly selective electrochemical conversion of methanol to formate is of great significance for various clean energy devices, but understanding the structure‐to‐property relationship remains unclear. Here, the asymmetric charge polarized NiCo prussian blue analogue (NiCo PBA‐100) is reported to exhibit remarkable catalytic performance with high current density (210 mA cm−2 @1.65 V vs RHE) and Faraday efficiency (over 90%). Meanwhile, the hybrid water splitting and Zinc–methanol‐battery assembled by NiCo PBA‐100 display the promoted performance with decent stability. X‐ray absorption spectroscopy (XAS) and operando Raman spectroscopy indicate that the asymmetric charge polarization in NiCo PBA leads to more unoccupied states of Ni and occupied states of Co, thereby facilitating the rapid transformation of the high‐active catalytic centers. Density functional theory calculations combining operando Fourier transform infrared spectroscopy demonstrate that the final reconstructed catalyst derived by NiCo PBA‐100 exhibits rearranged d band properties along with a lowered energy barrier of the rate‐determining step and favors the desired formate production.
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Research context

OpenAlex topics: Electrocatalysts for Energy Conversion · CO2 Reduction Techniques and Catalysts · Ammonia Synthesis and Nitrogen Reduction

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institutes of Physical Science and Information Technology School of Materials Science and Engineering Leibniz International Joint Research Center of Materials Sciences of Anhui Province Center of High Magnetic Fields and Free Electron Lasers Information Meterials and Intelligent Sensing Laboratory of Anhui Province Anhui University Hefei 230601 China

National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230029 China

Helmholtz‐Zentrum Dresden‐Rossendorf Bautzner Landstrasse 400 01328 Dresden Germany

School of Materials Science and Engineering University of Science and Technology Beijing Beijing 100083 China

School of Electronic and Information Engineering Tiangong University Tianjin 300387 China

Zhejiang Institute of Photonelectronics Jinhua Zhejiang 321004 China

Funding

National Key Research and Development Program of China · National Natural Science Foundation of China · Fundamental Research Funds for the Central Universities · Natural Science Foundation of Anhui Province

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