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Decrypting the Influence of axial coordination on the Electronic Microenvironment of Co-N_(5)Site for Enhanced Electrocatalytic Reaction

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CCS Chemistry 2023年第8期5卷 1876-1887页

作者： Bingyu Huang Senhe Huang Chenbao Lu Longbin Li Judan Chen Ting Hu Dirk Lützenkirchen-Hecht Kai Yuan Xiaodong Zhuang Yiwang Chen Institute of Polymers and Energy Chemistry(IPEC) College of Chemistry and Chemical EngineeringNanchang UniversityNanchang 330031 The meso-Entropy Matter Lab School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240 School of Materials Science and Engineering Nanchang UniversityNanchang 330031 Faculty of Mathematics and Natural Sciences-Physics Department Bergische Universität WuppertalWuppertal D-42119 Institute of Advanced Scientific Research(iASR) Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal UniversityNanchang 330022

Metal porphyrins are star molecules that possess welldefined coordination metal centers for versatile catalytic ***,most previous work has focused on the correlations between in-plane symmetric configuration of metal-N_(4)sites and their catalytic *** the catalytic contribution of additional axial coordination to such symmetric configuration remains a *** calculations revealed that axially anchoring an extra pyridine on the tetra-coordinated cobalt porphyrin(Co-N4)to construct penta-coordinated cobalt porphyrin(Co-N_(5))renders cobalt a higher electron density,thereby favoring the rate-determining O_(2)adsorption/activation and reducing the oxygen electroreduction ***,a well-defined Co-N_(5)site is rationally introduced into the azo-linked polymer framework for a fundamental structure-catalytic performance correlation ***-prepared Co-N_(5)catalyst exhibits a 26 mV positive shift in half-wave potential compared with the pyridine-free Co-N_(4)counterpart,discloses a markedly higher power density(141.4 mW cm^(−2)),and possesses better long-term durability(over 160 h cycles)in a Zn-air ***,such a Co-N_(5)catalyst also showcases potential applications for CO_(2)reduction with high CO_(2)-to-CO conversion faradic efficiency and better selectivity than the Co-N_(4)counterpart because coordination of the fifth pyridine evokes electronic localization that suppresses a competitive side *** work proves the positive electrocatalytic contribution of axial penta-coordination on well-defined metalporphyrin-based catalysts and offers atomic understanding of the structure-performance correlation on single atom catalysts for future catalyst design.

关键词： porphyrin axial coordination pentacoordination structureactivity correlation oxygen reduction reaction

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Advances on axial coordination Design of Single‑Atom Catalysts for Energy Electrocatalysis:A Review

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Nano-Micro Letters 2023年第12期15卷 188-230页

作者： Linjie Zhang Na Jin Yibing Yang Xiao‑Yong Miao Hua Wang Jun Luo Lili Han State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117People’s Republic of China State Key Laboratory of ASIC and System Shanghai Institute of Intelligent Electronics and SystemsSchool of MicroelectronicsFudan UniversityShanghai 200433People’s Republic of China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110People’s Republic of China

Single-atom catalysts(SACs)have garnered increasingly growing attention in renewable energy scenarios,especially in electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure *** intensive efforts towards the rational design and synthesis of SACs with versatile local configurations have significantly accelerated the development of efficient and sustainable electrocatalysts for a wide range of electrochemical *** an emergent coordination avenue,intentionally breaking the planar symmetry of SACs by adding ligands in the axial direction of metal single atoms offers a novel approach for the tuning of both geometric and electronic structures,thereby enhancing electrocatalytic performance at active *** this review,we briefly outline the burgeoning research topic of axially coordinated SACs and provide a comprehensive summary of the recent advances in their synthetic strategies and electrocatalytic ***,the challenges and outlooks in this research field have also been *** present review provides an in-depth and comprehensive understanding of the axial coordination design of SACs,which could bring new perspectives and solutions for fine regulation of the electronic structures of SACs catering to high-performing energy electrocatalysis.

关键词： Single-atom catalyst axial coordination Synthetic strategy Electrocatalytic application

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Cobalt porphyrin immobilized on the TiO_(2) nanotube electrode for CO2 electroreduction in aqueous solution

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Journal of Energy Chemistry 2021年第4期30卷 219-227页

作者： Shengshen Gu Aleksei N.Marianov Yuxiang Zhu Yijiao Jiang School of Engineering Macquarie UniversitySydneyNSW 2109Australia

Herein we report CO_(2) electrochemical reduction reaction(CO_(2) ERR)on the cobalt tetraphenylporphyrin(Co TPP)modified TiO_(2) nanotube(TNT)*** was found the axial coordination of drop-casting solvent to Co TPP and the porphyrin structure are the major factors that have significant effects on the catalytic performance of the *** confirmed by spectrophotometric titration,pyridine has a stronger coordination bond to Co TPP than DMF and THF thus leading to the highest efficiency among the dropcasting solvents tested in the *** on the spectrophotometric analysis,possible coordination mechanism between drop-casting solvents and Co TPP is put *** the other hand,introduction of-COOMe substituents in phenyl rings of Co TPP weakens the coordination bond between pyridine and Co TPP as clearly evidenced by deuterium NMR spectra,resulting in a detrimental effect on CO_(2) ***,the manipulation of the coordination environment around the metal center of immobilized catalyst is crucial in designing an efficient electrocatalytic system.

关键词： CO_(2)electroreduction Co porphyrins Immobilization Drop-casting solvent axial coordination

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Single-molecule imaging of dinitrogen molecule adsorption on individual iron phthalocyanine

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Nano Research 2020年第9期13卷 2393-2398页

作者： Chengding Gu Jia Lin Zhang Jian Qiang Zhong Qian Shen Xiong Zhou Kaidi Yuan Shuo Sun Xu Lian Zhirui Ma Wei Chen Department of Chemistry National University of SingaporeSingapore 117543Singapore Department of Physics National University of SingaporeSingapore 117542Singapore Department of Interface Science Fritz-Haber-Institut der Max-Planck-GesellschaftBerlin 14195Germany Institute of Advanced Materials Nanjing Tech UniversityNanjing 210009China BNLMS College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China School of Physical Science and Technology Shanghai Tech UniversityShanghai 200031China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou 350207China National University of Singapore(Suzhou)Research Institute Suzhou 215123China

Nitrogen fixation is a vital process for both nature and *** the nitrogenase can reduce nitrogen in ambient environment in nature,the industrialized Haber-Bosch process is a high temperature and high-pressure *** the discovery of the first dinitrogen complex in 1965,many dinitrogen complexes are prepared in a homogeneous solution to mimic the nitrogenase enzyme in ***,studies of the heterogeneous process on surface are rarely ***,molecular scale characterization for such dinitrogen complex is ***,we present a simple model system to investigate,at the single-molecule level,the binding of dinitrogen on a surface confined iron phthalocyanine(FePc)monolayer through the combination of in-situ low-temperature scanning tunneling microscopy(LT-STM)and X-ray photoelectron spectroscopy(XPS)*** iron center in FePc molecule deposited on Au(111)and highly oriented pyrolytic graphite(HOPG)surface can adsorb dinitrogen molecule at room temperature and low pressure.A comparative study reveals that the adsorption behaviors of FePc on these two different substrates are *** bond is formed between the dinitrogen and the Fe atom in the FePc molecule,which greatly modifies the electronic structure of *** bonding is reversible and can be manipulated by applying bias using a STM tip or by thermal annealing.

关键词： single-molecule dinitrogen iron phthalocyanine axial coordination

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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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ZnTPP axially Coordinated with a Novel Dipyridylamine Ligand:Hydrothermal Synthesis and Crystal Structure

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Chinese Journal of Structural Chemistry 2010年第8期29卷 1197-1200页

作者：王全国伍锡荣朱为宏解永树 Key Laboratory for Advanced Materials and Institute of Fine Chemicals East China University of Science & Technology Department of Chemistry University of Malaya

A novel complex ZnTPPL1·3DMF 1（TPP = tetraphenylporphyrin,L1 = N-（4-（9-carbazolyl） phenyl）-N,N-di（4-pyridyl）amine） was prepared by a hydrothermal method and characterized by elemental analysis,IR,and single-crystal X-ray diffraction *** 1 crystallizes in triclinic,space group P1 with a = 13.3082（2）,b = 14.3276（2）,c = 18.6120（3） ,α = 109.853（1）,β = 95.054（1）,γ = 98.832（1）°,V = 3260.57（9） 3,Z = 2,Dc = 1.334 g/cm3,C81H69N11O3Zn,Mr = 1309.84,μ（MoKα） = 0.438 mm-1,F（000） = 1372,GOF = 1.159,the final R = 0.0482 and wR = 0.1479 for 12091 observed reflections（Ⅰ 〉 2σ（Ⅰ））.Crystal structure analyses revealed that L1 utilizes one pyridyl N atom to bind Zn via axial coordination,affording a 1：1 *** binding constant was estimated to be 1.74（7） × 10^4 M^-1 from electronic spectra measurements.

关键词： zinc porphyrin axial coordination crystal structure hydrothermal synthesis

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