检索结果-南通市图书馆

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

在线全文

学校读者我要写书评

暂无评论

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

Nickel Complexes with Non-innocent Ligands as Highly Active Electrocatalysts for Hydrogen Evolution

在线全文

学校读者我要写书评

暂无评论

Chinese Journal of Chemistry 2018年第12期36卷 1161-1164页

作者： Zhixin Chen Tao Wang Tingting Sun Zhiyong Chen Tian Sheng Yu-Hao Hong Zi-Ang Nan Jun Zhu Zhi-You Zhou Haiping Xia Shi-Gang Sun Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory for Physical Chemistry of Solid SurfacesCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamenFujian 361005China

Rational design of a molecular catalyst for a hydrogen evolution reaction (HER) with both high rates and low overpotential remains a challenge. Here we report a series of Ni‐based catalysts incorporating non‐innocent ligands and aimed at reduction of the overpotential by reserving electrons in the ligand, which could decouple the correlation between metal center reduction and metal hydride formation. The third‐order rate constant of our catalysts can be increased by 2 orders of magnitude without increase of overpotential by altering the substituents in the imide since the electronic effect of substituents can change the kinetics of metal hydride formation dramatically. Furthermore, constructing a proton shuttle in the ligand further improves the activity. The catalyst with both of these features can catalyze HER at a turnover frequency of 2572 s –1 with low concentrations of acid and an extremely high third‐order rate constant of 2.7×10 6 M –2 ·s –1 at a low overpotential.

关键词： hydrogen evolution molecular electrocatalysis non‐innocent ligand electrochemistry homogeneous catalysis N ligands

Electropolymerization of cobalt porphyrins and corroles for the oxygen evolution reaction

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

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

在线全文

学校读者我要写书评

暂无评论

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

在线全文

学校读者我要写书评

暂无评论

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

Bioinspired iron porphyrins with appended poly-pyridine/amine units for boosted electrocatalytic CO_(2) reduction reaction

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

eScience 2022年第6期2卷 623-631页

作者： Jinxiu Han Ni Wang Xialiang Li Haitao Lei Yabo Wang Hongbo Guo Xiaotong Jin Qingxin Zhang Xinyang Peng Xue-Peng Zhang 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'an710119China Ruhr-Universität Bochum Fakultät für Chemie und BiochemieAnorganische Chemie I Universitätsstrasse 15044801BochumGermany Fraunhofer UMSICHT Department for Electrosynthesis46047OberhausenGermany

Developing highly efficient electrocatalysts for the CO_(2) reduction reaction(CO_(2)RR)has attracted increasing interest in the past ***,we report on the design and synthesis of Fe porphyrin 1 with an appended N,N-di(2-picolyl)ethylenediamine(DPEN)unit that boosts electrocatalytic activity for CO_(2)-to-CO conversion in acetonitrile with water as the proton *** mimicking carbon monoxide dehydrogenase(CODH),1 has poly-pyridine/amine units located at the active site to form hydrogen-bonded water-containing networks that enable fast proton *** protonated and positively charged DPEN unit can also stabilize CO_(2) reduction intermediates through electrostatic and hydrogen-bonding *** factors make 1 a highly active electrocatalyst for the CO_(2)RR by achieving a TOFmax of 5.0×10^(4)s^(−1) with water providing the *** critical roles of the DPEN unit in the CO_(2)RR are further supported by theoretical *** work is significant to highlight the benefits of using molecular catalysts to elucidate structural effects.

关键词： CO_(2)reduction reaction Fe porphyrin molecular electrocatalysis Structural effect Water network

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

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

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

Iron porphyrin with appended guanidyl group for significantly improved electrocatalytic carbon dioxide reduction activity and selectivity in aqueous solutions

在线全文

维普期刊数据库

学校读者我要写书评

暂无评论

Chinese Journal of Catalysis 2022年第12期43卷 3089-3094页

作者： Hongbo Guo Zuozhong Liang Kai Guo Haitao Lei Yabo Wang Wei Zhang Rui Cao Key Laboratory of Applied Surface and Colloid Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119ShaanxiChina

Iron porphyrins have high activity and selectivity for electrocatalytic CO_(2)reduction reaction(CO_(2)RR)in nonaqueous solutions,but they usually display poor or moderate selectivity for CO_(2)RR in aqueous solutions because of the competitive hydrogen evolution *** water as the electrocatalytic reaction solvent is more favored because not only it is cheap,green and abundant but also it can sufficiently provide protons required for CO_(2)***,developing Fe porphyrins as electrocatalysts for efficient and selective CO_(2)RR in aqueous solutions is of both fundamental and practical ***,we report the design and synthesis of Fe porphyrin 1 with an appended guanidyl group and its electrocatalytic features for CO_(2)RR in both nonaqueous and aqueous *** acetonitrile,Fe porphyrin 1 and its guanidyl-free analogue,tetrakis(3,4,5-trimethoxyphenyl)porphyrin 2,are both efficient for electrocatalytic CO_(2)-to-CO conversion,but the turnover frequency with 1(3.9´10^(5)s^(-1))is one order of magnitude larger than that with 2(1.7´10^(4)s^(-1)),showing the critical role of the appended guanidyl group in improving electrocatalytic CO_(2)RR *** importantly,in 0.1 mol L^(-1)KHCO_(3)aqueous solutions,1 showed very high selectivity for electrocatalytic CO_(2)-to-CO conversion with a Faradaic efficiency of 96%,while 2 displayed a Faradaic efficiency of 65%for the CO_(2)-to-CO *** work is of significance to show the effect of appended guanidyl group on improving both activity and selectivity of Fe porphyrins for CO_(2)RR electrocatalysis.

关键词： CO_(2)reduction molecular electrocatalysis Iron porphyrin Electrostatic interaction Proton relay

O-O bond formation mechanisms during the oxygen evolution reaction over synthetic molecular catalysts

在线全文

学校读者我要写书评

暂无评论

Chinese Journal of Catalysis 2021年第8期42卷 1253-1268页

作者： Xue-Peng Zhang Hong-Yan Wang 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 710119ShaanxiChina

Water oxidation is one of the most important reactions in natural and artificial energy conversion *** nature,solar energy is converted to chemical energy via water oxidation at the oxygen-evolving center of photosystem II to generate dioxygen,protons,and *** artificial energy schemes,water oxidation is one of the half reactions of water splitting,which is an appealing strategy for energy conversion via photocatalytic,electrocatalytic,or photoelectrocatalytic *** it is thermodynamically unfavorable and kinetically slow,water oxidation is the bottleneck for achieving large-scale water ***,developing highly efficient water oxidation catalysts has attracted the interests of researchers in the past *** formation of O-O bonds is typically the rate-determining step of the water oxidation catalytic ***,better understanding this key step is critical for the rational design of more efficient *** review focuses on elucidating the evolution of metal-oxygen species during transition metal-catalyzed water oxidation,and more importantly,on discussing the feasible O-O bond formation mechanisms during the oxygen evolution reaction over synthetic molecular catalysts.

关键词： Oxygen evolution reaction Water oxidation O-O bond formation Transition metal complex molecular electrocatalysis Reaction mechanism