Subtle Modifications in Interface Configurations of Iron/Cobalt Phthalocyanine‐Based Electrocatalysts Determine Molecular CO<sub>2</sub> Reduction Activities

Abstract Strain engineering has emerged as a powerful approach in steering material properties. However, the mechanism and potential limitations remain poorly understood. Here we report that subtle changes in molecular configurations can profoundly affect, conducively or adversely, the catalytic selectivity and product turnover frequencies (TOFs) of CO 2 reduction reaction. Specifically, introducing molecular curvature in cobalt tetraaminophthalocyanine improves the multielectron reduction activity by favorable *CO hydrogenation, attaining methanol Faradaic efficiency up to 52 %. In stark contrast, strained iron phthalocyanine exacerbates *CO poisoning, leading to decreased TOF CO by &gt;50 % at −0.5 V RHE and a rapid current decay. The uniform dispersion is crucial for optimizing electron transfer, while activity is distinctly sensitive to the local atomic environment around the active sites. Specifically, local strain either enhances binding to intermediates or poisons the catalytic sites. Our comprehensive analysis elucidates the intricate relationship between molecular structure and activities, offering insights into designing efficient heterogeneous molecular interfaces.

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Publication Details

Journal
Angewandte Chemie
Published
2024-11-25
DOI
https://doi.org/10.1002/ange.202420286
Citations
12
Primary Topic
CO2 Reduction Techniques and Catalysts
Type
article
Field-Weighted Citation Impact
1.23
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article

Subtle Modifications in Interface Configurations of Iron/Cobalt Phthalocyanine‐Based Electrocatalysts Determine Molecular CO2 Reduction Activities

Ruquan Ye, Xuefeng Tan, Chuan Xia, Yinger Xin et al.
12 citations
Angewandte Chemie
CO2 Reduction Techniques and Catalysts
1.23
article

Subtle Modifications in Interface Configurations of Iron/Cobalt Phthalocyanine‐Based Electrocatalysts Determine Molecular CO2 Reduction Activities

Ruquan Ye, Xuefeng Tan, Chuan Xia, Yinger Xin, Molly Meng‐Jung Li, William A. Goddard, Yun Mi Song, Qianfeng Gu, Jianjun Su, Qiu Jiang, Charles B. Musgrave, Ben Zhong Tang, Yong Liu, Qiang Zhang, Pei Xiong, Le Cheng, Weihua Guo, Jiangtong Li
article en
12 citations

Abstract

Abstract Strain engineering has emerged as a powerful approach in steering material properties. However, the mechanism and potential limitations remain poorly understood. Here we report that subtle changes in molecular configurations can profoundly affect, conducively or adversely, the catalytic selectivity and product turnover frequencies (TOFs) of CO 2 reduction reaction. Specifically, introducing molecular curvature in cobalt tetraaminophthalocyanine improves the multielectron reduction activity by favorable *CO hydrogenation, attaining methanol Faradaic efficiency up to 52 %. In stark contrast, strained iron phthalocyanine exacerbates *CO poisoning, leading to decreased TOF CO by &gt;50 % at −0.5 V RHE and a rapid current decay. The uniform dispersion is crucial for optimizing electron transfer, while activity is distinctly sensitive to the local atomic environment around the active sites. Specifically, local strain either enhances binding to intermediates or poisons the catalytic sites. Our comprehensive analysis elucidates the intricate relationship between molecular structure and activities, offering insights into designing efficient heterogeneous molecular interfaces.

Angewandte ChemieVol. 137(8)
California Institute of Technology (US), Hong Kong Polytechnic University (HK), University of Electronic Science and Technology of China (CN), City University of Hong Kong (HK), Hong Kong University of Science and Technology (HK), City University of Hong Kong, Shenzhen Research Institute (CN), Chinese University of Hong Kong, Shenzhen (CN)
Responsible consumption and production
Openalex Percentile: Top 23%
CO2 Reduction Techniques and Catalysts
1.23
DOIOpen Access PDFOpenAlex
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