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Conductive Metal/Covalent Organic Frameworks for CO_(2) Electroreduction

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Chinese Journal of Structural Chemistry 2022年第5期41卷 1-14页

作者： Chang-Pu Wan Jun-Dong Yi Rong Cao yuan-biao huang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100049China School of Chemistry and Materials Science Collaborative Innovation Center of Chemistry for Energy Materials(iChEM)University of Science and Technology of ChinaHefei 230026China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Porous crystalline metal-organic frameworks(MOFs)and covalent organic frameworks(COFs)are promising platforms for electrocatalytic reduction of CO_(2)(CO_(2)RR)due to their large CO_(2)adsorption uptakes and periodically arranged single active ***,the applications in CO_(2)RR of the traditional MOFs and COFs are greatly limited by their low electron *** recent years,numerous types of MOFs and COFs with high intrinsic conductivity have been rationally designed and successfully constructed,and some of them have been applied in CO_(2)*** this review,the applications of conductive MOFs and COFs in CO_(2)RR have been *** conductive MOFs and COFs can be categorized according to the methods,in which the conductivity is enhanced,such as constructing fullyπ-conjugated backbones,donor-acceptor heterojunction,enhancing theπ-πstacking interactions between organic moieties and/or the introduction of guest molecules.

关键词： metal-organic frameworks covalent organic frameworks CO_(2)electroreduction reaction conductive frameworks

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Conductive phthalocyanine-based metal-organic framework as a highly efficient electrocatalyst for carbon dioxide reduction reaction

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Science China Chemistry 2021年第8期64卷 1332-1339页

作者： Meng-Di Zhang Duan-Hui Si Jun-Dong Yi Qi Yin yuan-biao huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of Chinese Academy of Sciences Beijing100049China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou350007China Fujian College University of Chinese Academy of SciencesFuzhou350002China

Porous crystalline metal-organic frameworks(MOFs)are one class of promising electrode materials for CO_(2)electroreduction reaction(CO_(2)RR)by virtue of their large CO_(2)adsorption capacities and abundant tunable active sites,but their insulating nature usually leads to low current ***,a two-dimensional(2D)Ni-phthalocyanine-based MOF(NiPc-Ni(NH)4)constructed by 2,3,9,10,16,17,23,24-octaaminophthalocyaninato nickel(II)(NiPc-(NH_(2))_(8))and nickel(II)ions attained high electrical conductivity due to the high overlap of d-πconjugation orbitals between the nickel node and the Ni-phthalocyanine-substituted *** CO_(2)RR,the NiPc-Ni(NH)4 nanosheets achieved a high CO Faradaic efficiency of 96.4%at−0.7 V and a large CO partial current density of 24.8 mA cm^(−2)at−1.1 V,which surpassed all the reported two-dimensional MOF electrocatalysts evaluated in an *** control experiments and density functional theory(DFT)calculations suggested that the Ni-N_(4)units of the phthalocyanine ring are the catalytic active *** work provides a new route to the design of highly efficient porous framework materials for the enhanced electrocatalysis via improving electrical conductivity.

关键词： metal-organic frameworks electroreduction conductive CO_(2) CO

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Highly efficient electroreduction of CO_(2) by defect single-atomic Ni-N_(3) sites anchored on ordered micro-macroporous carbons

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Science China Chemistry 2022年第8期65卷 1584-1593页

作者： Qiu-Xia Li Duan-Hui Si Wan Lin Yao-Bing Wang Hong-Jing Zhu yuan-biao huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry Fuzhou UniversityFuzhou 350108China University of the Chinese Academy of Sciences Beijing 100049China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Microporous supports typically fail to fully expose active sites for electrolytes and CO_(2) molecules,and this usually results in low current density for the electrocatalytic CO_(2) reduction reaction(CO_(2)RR).To overcome the biggest obstacle and facilitate commercial applications,defective single-atomic Ni-N_(3) sites anchored to ordered micro-macroporous N-doped carbon(Ni-N/OMC)have been prepared by the pyrolysis of the Ni-ZIF-8@PS(ZIF=zeolitic imidazolate framework)and are intended to provide enhanced CO_(2)RR with a current density at an industrial *** Ni-ZIF-8@PS is constructed of nickel-based ZIF-8 embedded in the three-dimensional(3D)highly ordered polystyrene spheres(PS).The 3D ordered micro-macroporous architecture of Ni-N/OMC could facilitate the mass transfer of substrates to the accessible defective single-atomic Ni-N_(3) sites through micropores(0.6 nm)and macropores(~200 nm)interconnected by 50 nm *** a flow cell,Ni-N/OMC exhibits almost 100.0%CO Faraday efficiency(FECO)between−0.2 and−1.1 V *** and an industrial level CO partial current density of 208 mA cm^(−2).It has a turnover frequency of 1.5×10^(5) h^(−1) at−1.1 V *** in 1 M KOH electrolyte,which exceeds that of most reported nickel-based *** excellent CO_(2)RR performance for Ni-N/OMC makes it a state-of-the-art electrocatalyst for CO_(2)*** calculations show that the defective Ni-N_(3) site can lower the energy of*COOH formation compared with that of the Ni-N4 site,thereby accelerating CO_(2)***-N/OMC can also be utilized as a cathodic catalyst in Zn-CO_(2) battery,exhibiting high CO selectivity in the discharge process and excellent *** work paves a pathway to rational design of highly efficient electrocatalysts with 3D hierarchically ordered micro-macroporous architecture for CO_(2)RR towards industrial production and commercial applications.

关键词： metal-organic framework hierarchically ordered porous carbon Ni single atom CO_(2)electrocatalysis CO

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Migration-Prevention Strategy to Fabricate Single-Atom Fe Implanted N-Doped Porous Carbons for Efficient Oxygen Reduction

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Research 2019年第1期2019卷 612-623页

作者： Dong-Li Meng Chun-Hui Chen Jun-Dong Yi Qiao Wu Jun Liang yuan-biao huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of the Chinese Academy of Sciences Beijing 100049China

It is highly desired but challenging to achieve highly active single-atom Fe sites from iron-based metal-organic frameworks(MOFs)for efcient oxygen reduction reaction(ORR)due to the easy aggregation of iron species and formation of the inactive Fe-based particles during ***,a facile migration-prevention strategy is developed involving the incorporation of polyaniline(PANI)into the pores of iron porphyrinic-based MOF PCN-224(Fe)and followed by pyrolysis to obtain the single-atom Fe implanted N-doped porous carbons material PANI@PCN-224(Fe)-*** introduced PANI inside the pores of PCN-224(Fe)not only served as protective fences to prevent the aggregation of the iron species during thermal annealing,but also acted as nitrogen sources to increase the nitrogen content and form Fe-Nx-C active *** with the pristine PCN-224(Fe)derived carbonization sample containing Fe-based particles,the carbonaceous material PANI@PCN-224(Fe)-900 without inactive Fe-based particles exhibited superb ORR electrocatalytic activity with a more positive half-wave potential,signifcantly improved stability in both alkaline media,and more challenging acidic *** migration-prevention strategy provides a new way to fabricate atomically dispersed metal active sites via pyrolysis approach for promoting catalysis.

关键词： prevention pyrolysis Oxygen

Hydrophobic perfluoroalkane modified metal‐organic frameworks for the enhanced electrocatalytic reduction of CO_(2)

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SmartMat 2022年第1期3卷 163-172页

作者： Xu Yang Qiu‐Xia Li Shao‐Yi Chi Hong‐Fang Li yuan‐biao huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouChina College of Chemical Engineering Fuzhou UniversityFuzhouChina University of Chinese Academy of Sciences BeijingChina Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China FuzhouChina

The electrochemical reduction of CO_(2) to value‐added chemicals would be an efficient way to utilize CO_(2) and mitigate greenhouse gas ***,the associated competitive hydrogen evolution reaction(HER)in aqueous electrolytes usually leads to poor selectivity for the CO_(2) electroreduction reactions(CO_(2)RR).Due to their high specific surface areas and tunable single active sites,metal‐organic frameworks(MOFs)are considered as promising candidates for CO_(2)***,the Fe‐porphyrin based Zr‐MOF,PCN‐222(Fe),was treated with perfluorocarboxylic acid to afford the hydrophobic Fn‐PCN‐222(Fe)(n=5 and 7,n is the number of fluorine atoms in the perfluoroalkyl chain)for improving the selectivity CO_(2)RR via inhibiting the *** to the single active Fe sites were positioned in a hydrophobic microenvironment,the optimal F5‐PCN‐222(Fe)shows a high Faradic efficiency of 97%toward production of CO at−0.7 V versus reversible hydrogen ***,F5‐PCN‐222(Fe)achieved a high turnover frequency value of 3850 h−1 at−0.8 V,which was almost 3.6 times higher than that of PCN‐222(Fe)and surpassed most of other reported *** study paves a new way to improve the selectivity of the CO_(2)RR via inhibiting the associated HER by increasing the hydrophobicity of the electrocatalysts.

关键词： CO CO_(2)electrocatalysis hydrophobicity metal‐organic framework perfluoroalkyl chain

Boosting Electrocatalytic CO_(2)Reduction with Conjugated Bimetallic Co/Zn Polyphthalocyanine Frameworks

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CCS Chemistry 2023年第5期5卷 1130-1143页

作者： Nan Li Duan-Hui Si Qiu-jin Wu Qiao Wu yuan-biao huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 University of Chinese Academy of Science Beijing 100049 Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian 350108

Development of high-efficiency electrode materials for the electrochemical CO_(2)reduction reaction(CO_(2)RR)with high current density and selectivity compatible with industry is an important but significant ***,we describe a facile strategy to enhance the selectivity and current density by regulating the local electron density of the cobalt site in a series of stable,conjugated,bimetallic Co/Zn polyphthalocyanine frameworks Co_(x)Zn_(y)PPc with an AB stacking model under alkaline aqueous *** adjusting the ratio of Co and Zn to 3:1,the optimal Co3Zn1PPc exhibits an industry-compatible CO partial current density of 212 mA cm^(−2)at−0.9 V versus reversible hydrogen electrode in a flow cell,which is 1.7 and 9.1 times that of the single metal polyphthalocyanine CoPPc and ZnPPc,***_(3)Zn_(1)PPc shows a high CO Faraday efficiency of more than 90%in a wide operating potential window of−0.3 to−0.9 ***-depth experimental and theoretical analysis revealed that introduction of electron-rich Zn atoms modified the electron density of the active Co center,placing Co in the electronrich region and weakening the bonding strength with the reaction intermediate,thereby improving the CO_(2)RR *** results clarify the interaction mechanism of dual metal sites at the atomic level and provide a new avenue for the design of electrocatalysts with potential in industrial applications.

关键词： CO_(2)electrocatalysis flow cell cobalt polyphthalocyanine zinc polyphthalocyanine AB stacking

Ni single-atom sites supported on carbon aerogel for highly efficient electroreduction of carbon dioxide with industrial current densities

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eScience 2022年第3期2卷 295-303页

作者： Hui Guo Duan-Hui Si Hong-Jing Zhu Qiu-Xia Li yuan-biao huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China University of Chinese Academy of Sciences Beijing100049China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian350108China

Finding highly efficient electrocatalysts for the CO_(2)electroreduction reactions(CO_(2)RR)that have high selectivity and appreciable current density to meet commercial application standards remains a *** their reduction potentials are similar to that of the associated competitive hydrogen evolution reaction and the CO_(2)activation kinetics are *** single-atom catalysts(SACs)with high atom efficiency are one class of promising candidates for the CO_(2)RR to produce CO,single-atom active sites supported on microporous carbons are not fully exposed to substrates and thus lead to low current *** aerogels with interconnected channels and macropores can facilitate mass *** few reports describe utilizing them as supports to anchor SACs for efficient ***,N-doped carbon aerogels supporting Ni single atomic catalyst sites(denoted as Ni-NCA-X,X¼10,20)were fabricated by pyrolyzing Ni/Zn bimetallic zeolitic imidazolate framework(Ni/Zn-ZIF-8)/carboxymethylcellulose composite *** to abundant hierarchical micro-,meso-,and macropores and high CO_(2)adsorption,the Ni single active sites in the optimal Ni-NCA-10 were readily accessible for the electrolyte and CO_(2)molecules and thus achieved an industrial-level CO partial current density of 226 mA cm?2,a high CO Faradaic efficiency of 95.6%at?1.0 V *** reversible hydrogen electrode,and a large turnover frequency of 271810 h?1 in a flow-cell reactor at?1.0 *** excellent CO_(2)RR performance makes Ni-NCA-10 a rare state-of-the-art electrocatalyst for CO_(2)-to-CO *** work provides an effective strategy for designing highly efficient electrocatalysts toward the CO_(2)RR to achieve industrial current density via anchoring single-atom sites on carbon aerogels.

关键词： Carbon aerogel ZIF-8 Single-atom catalyst CO_(2)electrocatalysis CO

Multifunctional Gold Nanoparticles@Imidazolium-Based Cationic Covalent Triazine Frameworks for Efficient Tandem Reactions

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CCS Chemistry 2021年第9期3卷 2368-2380页

作者： Chang He Qiu-Jin Wu Min-Jie Mao Yu-huang Zou Bai-Tong Liu yuan-biao huang Rong Cao State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002 University of Chinese Academy of Sciences Beijing 100049 Fujian College University of Chinese Academy of SciencesFuzhou 350002

Tandem catalytic reactions have attracted extensive interest because of their ability to reduce reaction steps,energy consumption,and ***,the construction of highly efficient tandem catalytic systems is still a significant challenge due to the problematic integration of multiple active sites in one reaction system and the incompatibility of different reaction *** metal nanoparticles(MNPs)supported on porous framework materials have shown excellent catalytic performances in various reactions,their cooperative catalysis for tandem reactions is rarely reported.

关键词： tandem reaction imidazolium covalent triazine framework Lewis acid and base gold

Atomically Isolated Metal-Nitrogen Sites Anchored on Porphyrinic Triazine Frameworks for Electroreduction of CO2

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Atomically Isolated Metal-Nitrogen Sites Anchored on Porphyr...