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Effect of TiO_(2) support on immobilization of cobalt porphyrin for electrochemical CO_(2) reduction

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Journal of Materials Science & Technology 2021年第21期80卷 20-27页

作者： Shengshen Gu Aleksei N.Marianov Haimei Xu Yijiao Jiang School of Engineering Macquarie UniversitySydneyNSW2109Australia

Electrochemical reduction of CO_(2) is a promising strategy to manage the global carbon balance by transforming CO_(2) into chemicals. The efficiency of CO_(2) electroreduction is largely dependent on the design of hybrid electrode where both support and catalyst govern the performance of the electrolyzer. In this work,TiO_(2) calcined at different temperatures, was used as a support for immobilization of cobalt tetraphenyl porphyrin(CoTPP) and its effect on CO_(2) reduction was studied. It is demonstrated that the crystalline phase of TiO_(2) and doping of TiO_(2) apparently affecting CO_(2) electroreduction. It is found that anatase phase exhibits higher activity and selectivity compared to rutile due to the enhanced conductivity which in turn enables faster electron transfer between the support and CoTPP. As for dopants, the carbon doping in anatase TiO_(2) is proven to further enhance its conductivity, consequently resulting in the enhanced performance. This study implies that the rational design of supports is important for the performance of the hybrid electrode towards electrochemical CO_(2) reduction.

关键词： CO_(2)electroreduction cobalt porphyrin Immobilization TiO_(2)support Carbon doping

Synthesis of Axially Coordinated cobalt porphyrin/graphene Oxide Nanocomposite for Enhanced Electrocatalytic CO_(2) Reduction to CO

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Chinese Journal of Structural Chemistry 2022年第3期41卷 1-11,I0007页

作者： YOU Wei-Feng XU Xiao CAO Ai-Hui TAO Zhi-Jie KANG Long-Tian Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China University of Chinese Academy of Sciences Chinese Academy of SciencesBeijing 100049China

The electrocatalysts containing cobalt-pyrrolic nitrogen-carbon(Co-N_(4)-C)moiety for CO_(2)reduction reaction(CO_(2)RR)have caught much ***;the effects of Co valence state and its synergy with gra-phene substrate are not clear *** this work;cobalt porphyrin(CoTPP)molecule with the intrinsic Co-N_(4)-C moiety is successfully combined with graphene oxide(GO)via three kinds of liquid-phase *** ratio of CoTPP to GO and the valence state of Co atom are studied to explore their catalysis for CO_(2)RR to *** is found that axial-ly-coordinated Co(III)TPPCl/GO nanocomposites synthesized via a chemical method exhibit better ability for CO_(2)RR;as compared with Co(II)TPP+GO and/or Co(III)TPPCl+GO nanocomposites obtained via a physically mixing *** optimizing the ratio of CoTPP to GO;the Faradaic efficiency(FE)is more than 90%for CO_(2)RR to CO between−0.7 and−0.8 V *** hydrogen electrode(RHE)in Co(III)TPPCl/*** synergy be-tween CoTPP and GO and the effect of Co valence state are systematically investigated;indicating that their strong interaction plays the key role in electrocatalytic CO_(2)RR.

关键词： cobalt porphyrin graphene oxide axial coordination carbon dioxide reduction synergistic catalysis

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Molecular Insights into the Structure-Activity Relationship in cobalt porphyrin Catalyzed Oxygen Reduction Reaction

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CCS Chemistry 2023年第11期5卷 2628-2637页

作者： Xiang Wang Ya-Chen Feng Yu-Qi Wang Zhen-Yu Yi Jun-Jie Duan Hui-Juan Yan Dong Wang Li-Jun Wan CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Science(BNLMS)Institute of ChemistryChinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100049

We present a microscopic investigation on the structure-activity relationship of the Co-N4 site in the oxygen reduction reaction(ORR)by electrochemical scanning tunneling microscopy(ECSTM)at the molecular *** cobalt porphyrins with various substituents(CoTPPX_(4),X=Cl,H,OCH_(3))that delicately regulate the electronic structure of the active site were investigatedasmodel *** measurements evidenced that the CoTPPCl_(4)exhibits better activity,higher product selectivity for H_(2)O,and lower *** CoTPPX_(4)-O_(2)complex with higher contrast can be observed in the STM images and the proportion of the CoTPPCl_(4)-O_(2)is appreciably larger than that of CoTPP-O_(2)and CoTPP(OCH_(3))4-O_(2).Theoretical simulations of the model catalysts and the reaction processes of the ORR reveal the relationship between the electronic structure and the catalytic behavior of the model *** transformation of the CoTPPX_(4)-O_(2)and CoTPPX_(4)in the electrocatalytic reaction was monitored by in situ ECSTM *** structure-activity relationship clarified by experimental and theoretical investigations in this work should help to guide the rational design and optimization of high-performance catalysts.

关键词： cobalt porphyrin oxygen reduction reaction electrochemical scanning tunneling microscope structure-activity relationship model catalyst

cobalt porphyrin Catalyzed Carbon-Carbon Bond Transfer Hydrogenation with DMF

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Cobalt Porphyrin Catalyzed Carbon-Carbon Bond Transfer Hydro...

A cobalt(Ⅱ)porphyrin with a tethered imidazole for efficient oxygen reduction and evolution electrocatalysis

中国化学会第四届卟啉与酞菁学术研讨会

作者： Chun Meng Tam Ching Tat To Kin Shing Chan Department of Chemistry The Chinese University of Hong Kong

The Co(ttp) catalyzed carbon-carbon bond transfer hydrogenation of [2.2]paracyclophane(PCP) with DMF was *** investigation suggested that the benzylic carbon-carbon bond of PCP reacts with Co II(ttp) to generate 1,subsequent homolysis of Co-C bond and hydrogen atom abstraction yield 2 and regenerate the Co(ttp) *** mechanism of cobalt porphyrin catalysis is distinctly different from the rhodium and iridium catalyses.1,2

关键词： C-C bond hydrogenation transfer hydrogenation cobalt porphyrin N,N-dimethylformamide

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Journal of Energy Chemistry 2023年第1期76卷 617-621,I0015页

作者： Xialiang Li Ping Li Jindou Yang Lisi Xie Ni Wang Haitao Lei Chaochao Zhang Wei Zhang Yong-Min Lee Weiqiang Zhang Shunichi Fukuzumi Wonwoo Nam Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'an 710119 ShaanxiChina Department of Chemistry and Nano Science Ewha Womans UniversitySeoul 03760Republic of Korea

Electrocatalytic oxygen reduction and evolution reactions are involved in new energy conversion and storage technologies,such as various fuel cells and metal-air batteries and also water splitting devices[1,2].However... 详细信息

关键词： Molecular electrocatalysis cobalt porphyrin Axial ligand effect Oxygen reduction reaction Oxygen evolution reaction

The interaction of a cobalt porphyrin with cancer-associated nitrosamines

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The interaction of a cobalt porphyrin with cancer-associated...

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

中国烟草学会2015年年会

作者： Feiyan Tao Ya Dai Changguo Wang Guanglin Feng Dongliang Li Kuoyan Ma Lijun Zhu Lanlan Tan Xiaoqi Yu Key Laboratory of Green Chemistry and Technology Ministry of Education College of Chemistry Sichuan University Harmful Components and Tar Reduction in Cigarette Sichuan Key Laboratory Technical Research Center Chuanyu Branch of China Tobacco Corporation

A cobalt porphyrin(CY-B) was presented, and its interaction with tobacco-specific nitrosamines(TSNAs)was investigated by UV–Vis spectroscopy and high-resolution mass spectrometry. The results revealed that the stoichiometry of the host–guest interaction was 1:2 and that the binding constant between CY-B and TSNAs was within the range of 0.78 108–7.83 108 M 2. The coordination strength between CY-B and TSNAs decreased in the sequence of NNN > NAB > NAT > NNK based on the binding *** interaction mechanism of CY-B with TSNAs involved a coordination interaction, and the p–p interaction between the porphyrin macrocycle and the aromatic frame of the TSNAs pyridines may also have been a driving force. The measured thermodynamic properties demonstrated that the reaction of CY-B with TSNAs was spontaneous and that the driving force for the interaction was a change in *** reaction was exothermic, and an increasing temperature inhibited the interaction. The IR spectrum of the complex revealed that the ANAN@O group of TSNAs and the metal cobalt of CY-B formed the six-coordinate complex.

关键词： Metalloporphyrin cobalt porphyrin TSNAs Coordination interaction Hemin Association constants

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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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Study on Synthesis and Deplete Harmful Radical of cobalt porphyrins as the Mimic of Enzyme

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Wuhan University Journal of Natural Sciences 2000年第2期5卷 214-214页

作者： LI Zao ying1, ZHANG Yue ning1, LI Cong1, FENG Qing2, XIA Shu zhen2 (1. College of Chemistry and Environment Science, Wuhan University, Wuhan 430072, China 2. Department of Chemistry, Tongji Medical University, Wuhan 430030, China)

The four cobalt porphyrins [Co (3, 4, 5 MeO TPP) (1) ; Co (TTP) (2) ; Co (4 CI TPP) (3);Co (4 HSO 3 TPP) (4)] were synthesized and considered as two mimic of superoxide dismutaes (SOD) and catalase (CAT). The catalytic efficiency of them on deplete the harmful radical have been proved using riboflavin methionine photoreduction method in the concentration range of 10 6 ～10 5 mol/L. The catalytic efficiency of them at decomposing H 2O 2 has been performed by spectrophotometer. The percentage of decomposing H 2O 2 while the increasing the concentration of the imitating compounds. The lipid peroxidationproduced in liver homogenatcd of mice was determined by spectrophotometer detecting the content of MDA.

关键词： cobalt porphyrin synthesis superoxide dismutaes catalase two functional mimic of enzyme