Subtle Modifications in Interface Configurations of Iron/Cobalt Phthalocyanine-Based Electrocatalysts Determine Molecular CO2 Reduction Activities
Yinger Xin
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorCharles B. Musgrave III
Materials and Process Simulation Center, California Institute of Technology, Pasadena, CA, 91125 United States
Search for more papers by this authorCorresponding Author
Jianjun Su
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorJiangtong Li
Department of Applied Physics, Hong Kong Polytechnic University, 11 Yuk Choi Rd, Hung Hom, Hong Kong, SAR, 999077 P. R. China
Search for more papers by this authorPei Xiong
Department of Applied Physics, Hong Kong Polytechnic University, 11 Yuk Choi Rd, Hung Hom, Hong Kong, SAR, 999077 P. R. China
Search for more papers by this authorCorresponding Author
Molly Meng-Jung Li
Department of Applied Physics, Hong Kong Polytechnic University, 11 Yuk Choi Rd, Hung Hom, Hong Kong, SAR, 999077 P. R. China
Search for more papers by this authorYun Song
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorQianfeng Gu
Department of Materials Science and Engineering, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorQiang Zhang
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorYong Liu
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorWeihua Guo
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorLe Cheng
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorXuefeng Tan
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorQiu Jiang
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, Sichuan, 611731 P. R. China
Contribution: Formal analysis (supporting)
Search for more papers by this authorChuan Xia
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, Sichuan, 611731 P. R. China
Contribution: Formal analysis (supporting)
Search for more papers by this authorCorresponding Author
Prof. Ben Zhong Tang
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 Clear Water Bay, Hong Kong, SAR, 999077 P. R. China
School of Science and Engineering, Shenzhen Institute of Aggregate Science and Technology, The Chinese University of Hong Kong, Shenzhen, Shenzhen, Guangdong, 518172 P. R. China
Search for more papers by this authorCorresponding Author
William A. Goddard III
Materials and Process Simulation Center, California Institute of Technology, Pasadena, CA, 91125 United States
Search for more papers by this authorCorresponding Author
Prof. Ruquan Ye
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
City University of Hong Kong Shenzhen Research Institute, Shenzhen, Guangdong, 518057 P. R. China
Search for more papers by this authorYinger Xin
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorCharles B. Musgrave III
Materials and Process Simulation Center, California Institute of Technology, Pasadena, CA, 91125 United States
Search for more papers by this authorCorresponding Author
Jianjun Su
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorJiangtong Li
Department of Applied Physics, Hong Kong Polytechnic University, 11 Yuk Choi Rd, Hung Hom, Hong Kong, SAR, 999077 P. R. China
Search for more papers by this authorPei Xiong
Department of Applied Physics, Hong Kong Polytechnic University, 11 Yuk Choi Rd, Hung Hom, Hong Kong, SAR, 999077 P. R. China
Search for more papers by this authorCorresponding Author
Molly Meng-Jung Li
Department of Applied Physics, Hong Kong Polytechnic University, 11 Yuk Choi Rd, Hung Hom, Hong Kong, SAR, 999077 P. R. China
Search for more papers by this authorYun Song
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorQianfeng Gu
Department of Materials Science and Engineering, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorQiang Zhang
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorYong Liu
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorWeihua Guo
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorLe Cheng
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorXuefeng Tan
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
Search for more papers by this authorQiu Jiang
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, Sichuan, 611731 P. R. China
Contribution: Formal analysis (supporting)
Search for more papers by this authorChuan Xia
School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, Sichuan, 611731 P. R. China
Contribution: Formal analysis (supporting)
Search for more papers by this authorCorresponding Author
Prof. Ben Zhong Tang
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 Clear Water Bay, Hong Kong, SAR, 999077 P. R. China
School of Science and Engineering, Shenzhen Institute of Aggregate Science and Technology, The Chinese University of Hong Kong, Shenzhen, Shenzhen, Guangdong, 518172 P. R. China
Search for more papers by this authorCorresponding Author
William A. Goddard III
Materials and Process Simulation Center, California Institute of Technology, Pasadena, CA, 91125 United States
Search for more papers by this authorCorresponding Author
Prof. Ruquan Ye
Department of Chemistry, State Key Laboratory of Marine Pollution, City University of Hong Kong, Tat Chee Avenue 83, Kowloon, Hong Kong SAR, 999077 P. R. China
City University of Hong Kong Shenzhen Research Institute, Shenzhen, Guangdong, 518057 P. R. China
Search for more papers by this authorAbstract
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 CO2 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 TOFCO by >50 % at −0.5 VRHE 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.
Conflict of Interests
The authors declare no conflict of interest.
Open Research
Data Availability Statement
The data that support the findings of this study are available from the corresponding author upon reasonable request.
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