DataVXAdvanced MaterialsPaper
journal article·2024-04

Ultrathin, Cationic Covalent Organic Nanosheets for Enhanced CO2 Electroreduction to Methanol

Yun Song, Peng Guo, Tinghao Ma, Jianjun Su, Libei Huang, Weihua Guo, Yong Liu, Geng Li, Yinger Xin, Qiang Zhang, Siwei Zhang, Hanchen Shen, Xing Feng, Dengtao Yang, Jia Tian, Sai Kishore Ravi, Ben Zhong Tang, Ruquan Ye

Advanced Materials· Volume 36· Issue 17
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Source abstract

Abstract

Abstract Metalloporphyrins and metallophthalocyanines emerge as popular building blocks to develop covalent organic nanosheets (CONs) for CO2 reduction reaction (CO2RR). However, existing CONs predominantly yield CO, posing a challenge in achieving efficient methanol production through multielectron reduction. Here, ultrathin, cationic, and cobalt‐phthalocyanine‐based CONs (iminium‐CONs) are reported for electrochemical CO2‐to‐CH3OH conversion. The integration of quaternary iminium groups enables the formation of ultrathin morphology with uniformly anchored cobalt active sites, which are pivotal for facilitating rapid multielectron transfer. Moreover, the cationic iminium‐CONs exhibit a lower activity for hydrogen evolution side reaction. Consequently, iminium‐CONs manifest significantly enhanced selectivity for methanol production, as evidenced by a remarkable 711% and 270% improvement in methanol partial current density (jCH3OH) compared to pristine CoTAPc and neutral imine‐CONs, respectively. Under optimized conditions, iminium‐CONs deliver a high jCH3OH of 91.7 mA cm−2 at −0.78 V in a flow cell. Further, iminium‐CONs achieve a global methanol Faradaic efficiency (FECH3OH) of 54% in a tandem device. Thanks to the single‐site feature, the methanol is produced without the concurrent generation of other liquid byproducts. This work underscores the potential of cationic covalent organic nanosheets as a compelling platform for electrochemical six‐electron reduction of CO2 to methanol.
Source: crossref · Quality: baseline

Research context

Nanomaterials

OpenAlex topics: CO2 Reduction Techniques and Catalysts · Ionic liquids properties and applications · Covalent Organic Framework Applications

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

Affiliations

Department of Chemistry and State Key Laboratory of Marine Pollution City University of Hong Kong Hong Kong 999077 China

City University of Hong Kong Shenzhen Research Institute Shenzhen 518057 China

Key Laboratory of Synthetic and Self‐Assembly Chemistry for Organic Functional Molecules Center for Excellence in Molecular Synthesis Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences Chinese Academy of Sciences 345 Lingling Road Shanghai 200032 China

School of Chemistry and Chemical Engineering Northwestern Polytechnical University Xi'an 710072 China

Shenzhen Institute of Molecular Aggregate Science and Engineering School of Science and Engineering The Chinese University of Hong Kong Longgang District Shenzhen 518172 China

Department of Chemistry and the Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction The Hong Kong University of Science and Technology Hong Kong 999077 China

Guangdong Provincial Key Laboratory of Information Photonics Technology School of Material and Energy Guangdong University of Technology Guangzhou 510006 P. R. China

School of Energy and Environment City University of Hong Kong Hong Kong 999077 China

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