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A cobalt(Ⅲ)corrole with a Tethered Imidazole for Boosted Electrocatalytic Oxygen Reduction Reaction

Chinese Journal of Chemistry 2023年第21期41卷 2866-2872页

作者： Yimei Gao Benxing Mei Yizhen Wu Qian Zhao Zijia Bao Haonan Qin Yuhan Xu Haoyuan Lv Xinyang Peng Yan He Ting Luo Ran Yao Wei Zhang Haitao Lei Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'anShaanxi710119 China Beihang School Beihang UniversityBeijing100191 China

Developing electrocatalysts with high activity and selectivity for the oxygen reduction reaction(ORR)is vital to promote the performance of the next-generation energy technologies,which depend on the efficiency of the catalytic reduction of *** the structure of cytochrome c oxidases(CcOs),a histidine imidazole residue binding to the axial position of Fe plays a crucial role in facilitating the selective reduction of O_(2)to *** by nature,we herein report on the synthesis of CoIII corrole 1 tethered with an imidazole ligand as well as its electrocatalytic ORR and O_(2)binding *** compared to the imidazolium-free analogue,complex 1 displayed remarkably boosted activity for the selective four-electron/four-proton(4e-/4H+)ORR with a half-wave potential of E1/2=0.82 V versus reversible hydrogen electrode(RHE)in 0.1 mol/L KOH ***,we demonstrate that the tethered axial imidazole ligand improves the O_(2)binding ability of 1 thermodynamically and dynamically,which is crucial to boost electrocatalytic ORR *** work presents an example to improve electrocatalytic ORR activity and selectivity of Co corroles by introducing an axial imidazole ligand to enhance the O_(2)binding and activation.

关键词： Molecular electrocatalysis cobalt corrole Axial ligand effect Oxygen reduction reaction O_(2)binding

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cobalt‐N_(4) macrocyclic complexes for heterogeneous electrocatalysis of the CO_(2) reduction reaction

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Chinese Journal of Catalysis 2022年第1期43卷 104-109页

作者： Zhichao Lin Zhan Jiang Yubo Yuan Huan Li Hongxuan Wang Yirong Tang Chunchen Liu Yongye Liang Department of Materials Science and Engineering Southern University of Science and Technology of ChinaShenzhen 518055GuangdongChina Guangdong Provincial Key Laboratory of Energy Materials for Electric Power Southern University of Science and TechnologyShenzhen 518055GuangdongChina

Metal-N_(4)(M-N_(4))macrocyclic complexes are interesting electrocatalysts due to their well-defined structures and rich molecular *** them,metal phthalocyanines have been widely studied for the carbon dioxide reduction reaction(CO_(2)RR)in heterogeneous systems and demonstrated good electrocatalytic ***,other complexes like metal corroles and metal porphyrins are much less explored,and often show inferior *** this study,three cobalt macrocyclic complexes,cobalt phthalocyanine,cobalt meso-tetraphenylporphyrin,and cobalt meso-triphenylcorrole(CoPc,CoTPP and CoTPC)are investigated in heterogeneous electrocatalysis of CO_(2)*** CoPc/carbon nanotube(CNT)hybrid exhibits high electrocatalytic activity,CNT hybridization does not work for CoTPC and CoTPP that hold weak interactions with *** the drop-dry method with a high molecular loading of 5.4×10^(–7) mol cm^(–2),CoTPC and CoTPP could deliver appreciable electrode ***(4-vinylpyridine)(PVP)introduction is further demonstrated as a facile method to afford enhanced activities for CoTPP at low molecular loadings through enhancing molecule-substrate *** partial current density of carbon monoxide for CoTPP+CNT/PVP is around 8 times higher than the sample without PVP at–0.67 V versus reversible hydrogen *** work provides solutions to enhance the electrode activities of molecular electrocatalysts with weak substrate interactions in heterogeneous systems.

关键词： CO_(2)reduction cobalt phthalocyanine cobalt corrole cobalt porphyrin Heterogeneous electrocatalysis

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