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Electrochemically Generated Iodine Cations from a Glassy Carbon Electrode for Highly Selective Iodination of Anisole

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Transactions of Tianjin University 2022年第6期28卷 433-439页

作者： Liang Yan haitao lei Pengcheng Yang Wei Zhang Shaanxi Coal Chemical Technology Research Institute Co. LtdXi’an 710100China School of Chemistry and Chemical Engineering Shaanxi Normal UniversityXi’an 710119China

The synthesis of aryl iodides from commercially available raw chemicals by simple,cheap and green strategies is of fundamental signifi *** iodides can undergo a series of homo-/cross-coupling reactions for the synthesis of important industrial chemicals and *** methods require the electrophilic substitution on aromatic compounds by iodine or hypervalent iodine compounds,which suff ers from the use of erosive halogens or hazardous *** the development of green chemistry in the fi eld of electrochemical synthesis,anodic oxidation-derived I^(+)cations have been used for substitution ***,the selectivity of the iodination by these electrochemical methods remains *** believed that the anolyte is contaminated by trace platinum species from the working ***,we report the generation of active I^(+)species from the anodic oxidation of I_(2) in acetonitrile using a glassy carbon *** the presence of H^(+),electrolyte prepared with a glassy carbon anode can react with anisole to selectively form 4-iodoanisole with a yield as high as 97%.On contrast,the electrolytes prepared from Pt and graphite anodes fi nished the reaction with yields of 16%and 60%for 4-iodoanisole,*** electrochemical method also applies to the iodination of toluene,benzonitrile and bromobenzene,delivering the target para-iodination products with 92%,84%,and 73%yields,***,an atom-effi cient and highly selective aryl iodination method was developed without the use of excessive oxidants.

关键词： Iodination Electrochemistry Anodic oxidation Aryl iodides Selectivity

Sliding mode Control for Space Grid Structure with Magnetorheological Dampers 36

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Sliding mode Control for Space Grid Structure with Magnetorh...

Cobalt porphyrins supported on carbon nanotubes as model catalysts of metal-N_(4)/C sites for oxygen electrocatalysis

第36届中国控制会议

作者： Zhijun Li haitao lei Yuanyuan Liu Gang Li School of Civil and Architecture Engineering Xi’an Technological University

ISBN: (纸本)9781538629185

Using sliding mode control algorithm with the exponential reaching law,in this paper,a new semi-active control strategy is presented for space grid structures installed with magnetorheological（MR） *** real semi-active control force is obtained based on the computed control force and the maximum control force of the MR damper.A structural model of one-story space grid structure subjected to different ground motions is provided to testify the effectiveness of the proposed control *** results show that（a） the MR damper is an effective shock absorber and（b） semi-active control strategy based on sliding mode control algorithm is effective for the reduction of vibration response quantities of the space grid structure under different ground ***,the robustness of the proposed controller is verified through 20%reduction of structural stiffness.

关键词： Space grid structure magnetorheological damper sliding mode control semi-active control

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Journal of Energy Chemistry 2021年第2期30卷 77-81,I0003页

作者： Haonan Qin Yanzhi Wang Bin Wang Xiaoguang Duan haitao lei Xuepeng Zhang Haoquan Zheng Wei Zhang Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'an 710119.ShaanxiChina School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaide 5005SAAustralid

Transition-metal based M-N_4/C catalysts are appealing for electrocatalytic oxygen reduction reaction(ORR) and oxygen evolution reaction(OER). Employing model catalysts, which have well-defined molecular structures and coordination environments, to investigate electrocatalytic performance of M-N_4/C sites for ORR and OER is of fundamental significance. Herein, we reported the use of Co tetra(phenyl)porphyrin 1 and Co tetra(pentafluorophenyl)porphyrin 2 as models to probe the role of Co-N_4/C sites for oxygen electrocatalysis. We showed that Co porphyrin 1 is more efficient than its structural analogue 2 for oxygen electrocatalysis in alkaline aqueous solutions, indicating that the electronrich Co-N_4/C site is more favored when noncovalently adsorbed on carbon supports. This work inspires rational design of reaction-oriented catalysts for sustainable energy storage and conversion technologies.

关键词： Molecular electrocatalysis Model catalyst Oxygen evolution reaction Oxygen reduction reaction Porphyrin

Comparing electrocatalytic hydrogen and oxygen evolution activities of first-row transition metal complexes with similar coordination environments

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Journal of Energy Chemistry 2021年第12期30卷 659-666,I0016页

作者： Xiaotong Jin Xialiang Li haitao lei Kai Guo Bin Lv Hongbo Guo Dandan Chen Wei Zhang Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119ShaanxiChina

Developing cheap and efficient electrocatalysts for water splitting is required for energy conversion *** first-row transition metal complexes have been shown to be active for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Metal ions play crucial roles in these catalytic processes,but the activity dependence on the nature of metal ions has been rarely studied due to the difficulty to compare metal complexes with different coordination *** herein reported the synthesis of a series of metal complexes of azido-substituted porphyrin(1),in which metal ions have very similar coordination *** grafting 1-M(M=Mn,Fe,Co,Ni,and Cu)onto alkynefunctionalized carbon nanotubes(CNTs)through the same covalent connection,the resulted hybrids 1-M@CNT were all active and robust for both electrocatalytic HER and OER in alkaline aqueous *** these hybrids,1-Fe@CNT displayed the highest electrocatalytic activity for HER,while 1-Co@CNT was the most active one for ***,a two-electrode water electrolysis cell assembled with 1-Fe@CNT as the cathode and 1-Co@CNT as the anode required smaller applied bias potential by210 mV to get 10 mA/cm^(2)current density as compared to that assembled with Pt/C and Ir/C with the same amount of metal *** work is significant to correlate HER and OER activity with the nature of first-row transition metal ions and to highlight promising potential applications of molecular electrocatalysis in water splitting.

关键词： Metal porphyrins Molecular electrocatalysis Hydrogen evolution Oxygen evolution Water splitting

Substituent position effect of Co porphyrin on oxygen electrocatalysis

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Chinese Chemical Letters 2021年第9期32卷 2841-2845页

作者： Haoyuan Lv Hongbo Guo Kai Guo haitao lei Wei Zhang Haoquan Zheng Zuozhong Liang Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119China

Substituent effect of metal porphyrin molecular catalysts plays a crucial role in determining the catalytic activity of oxygen ***,substituent position effect of Co porphyrins on oxygen electrocatalysis,including the oxygen reduction reaction(ORR)and the oxygen evolution reaction(OER),was *** Co porphyrins,namely 2,4,6-OMe-CoP and 3,4,5-OMe-CoP,were selected as the research *** ORR and OER performance was evaluated by drop-coating molecular catalysts on carbon nanotubes(CNTs).The resulted 3,4,5-OMe-CoP/CNT exhibited high bifunctional electrocatalytic activities and better long-term stability for both ORR and OER than 2,4,6-OMe-CoP/***,when applied in the Zn-air battery,3,4,5-OMe-CoP/CNT exhibited comparable performance to that with precious metal-based *** enhanced catalytic activity may be attributed to the improved charge transfer rate,mass transfer and *** work provides an effective strategy to further enhance catalytic activity by introducing substituent position effect,which is of great importance for developing more efficient energy-related electrocatalysts.

关键词： Oxygen electrocatalysis Oxygen reduction reaction Oxygen evolution reaction Co porphyrin Substituent effect

Electropolymerization of cobalt porphyrins and corroles for the oxygen evolution reaction

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Chinese Chemical Letters 2021年第12期32卷 3807-3810页

作者： Qingxin Zhang Yabo Wang Yanzhi Wang Shujiao Yang Xuan Wu Bin Lv Ni Wang Yimei Gao Xiaoran Xu haitao lei Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi'an 710119China

Developing large-scale electrocatalysts using molecular complexes for the oxygen evolution reaction(OER)is of great importance. Herein, four cobalt porphyrins and corroles are deposited on electrode substrates using a simple and fast electropolymerization method. Our results showed that Co-1-P@CC, formed by electropolymerizing Co tetrakis(p-N-pyrrolylphenyl)porphyrin(Co-1-P) on carbon cloth(CC), is the most active OER catalyst in the examined Co porphyrins and corroles in alkaline aqueous solutions by displaying an onset overpotential of 380 m V. Long-term electrolysis tests confirmed the stability of these electropolymerized films by functioning as OER electrocatalysts.

关键词： Cobalt corroles Cobalt porphyrins Electropolymerization Molecular electrocatalysis Oxygen evolution

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

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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

A Cobalt(Ⅲ)Corrole with a Tethered Imidazole for Boosted Electrocatalytic Oxygen Reduction Reaction

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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

Tuning Electronic Structures of Covalent Co Porphyrin Polymers for Electrocatalytic CO_(2) Reduction in Aqueous Solutions

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CCS Chemistry 2022年第9期4卷 2959-2967页

作者： Yabo Wang Xue-Peng Zhang haitao lei Kai Guo Gelun Xu Lisi Xie Xialiang Li Wei Zhang Ulf-Peter Apfel Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119 Fakultät für Chemie und Biochemie Ruhr-Universität Bochum44801 Bochum Fraunhofer UMSICHT 46047 Oberhausen

Improving the selectivity of the electrocatalytic CO_(2) reduction reaction(CO_(2)RR)over hydrogen evolution in aqueous solutions is required but challenging because the two reactions occur at close thermodynamic potentials and compete with each ***,we report on the selective CO_(2)RR in aqueous solutions utilizing covalent Co porphyrin polymers with fine-tuned electronic structures.

关键词： carbon dioxide reduction molecular electrocatalysis covalent porphyrin polymer electronic structure selectivity