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Metalloporphyrin-based covalent organic frameworks composed of the electron donor-acceptor dyads for visible-light-driven selective CO2 reduction

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Science China Chemistry 2020年第9期63卷 1289-1294页

作者： Haowei Lv Rongjian Sa Pengyue Li daqiang yuan Xinchen Wang Ruihu Wang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Institute of Oceanography Ocean CollegeMinjiang UniversityFuzhou 350108China State Key Laboratory of Photocatalysis on Energy and Environment Fuzhou UniversityFuzhou 350108China

The visible-light-driven photocatalytic CO2 reduction with high efficiency is highly desirable but ***,we present porphyrin-tetraphenylethene-based covalent organic frameworks(MP-TPE-COF,where M=H2,Co and Ni;TPE=4,4′,4″,4?-(ethane-1,1,2,2-tetrayl)tetrabenzaldehyde;COF=covalent organic framework)as ideal platforms for understanding photocatalytic CO2 reduction at molecular *** and theoretical investigations have demonstrated crucial roles of metalloporphyrin units in selective adsorption,activation and conversion of CO2 as well as in the separation of charge carriers and electron transfer,thus allowing for flexible modulation of photocatalytic activity and *** P-TPE-COF exhibits high CO evolution rate of 2,414μmol g-^1 h^-1 with the selectivity of 61%over H2 generation under visible-light irradiation,while Ni P-TPE-COF provides CO evolution rate of 525μmol g^-1 h^-1 and 93%selectivity with superior ***,the photocatalytic system is feasible for the simulated flue gas,which provides CO evolution rate of 386μmol g-1 h-1 and selectivity of 77%.This work provides in-depth insight into the structure-activity relationships toward the activation and photoreduction of CO2.

关键词： covalent organic frameworks photocatalysis porous materials CO2reduction metalloporphyrin

Dimeric Calix[4]resorcinarene-based Porous Organic Cages for CO_(2)/CH_(4) Separation

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Chemical Research in Chinese Universities 2022年第2期38卷 428-432页

作者： YANG Miao WANG Wenjing SU Kongzhao yuan daqiang College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007P.R.China State Key Lab of Structure Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002P.R.China University of the Chinese Academy of Sciences Beijing 100049P.R.China

Investigating gas separation by emerging porous organic cage(POC) solids is still on its initial stage. In this work, two novel [2+4] organic cages with distinguished structures have been prepared based on the Schiff-based condensation reaction between tetraformyl-functionalized calix[4]resorcinarene building blocks and xylylenediamine(XDA) isomers. Specifically, the use of para-position XDA affords lantern-shaped cage(CPOC-105) with a medium cavity of ca. 0.526 nm^(3), while the meta-position produces peanut-shaped structure(CPOC-106) with two small cavities of ca. 0.181 nm^(3). Both CPOC-105 and CPOC-106 exhibit high selectivity capture of CO_(2) over CH4 with calculated selectivity coefficients of 4.5 and 3.1, respectively, under ambient conditions, and are capable of separating CO_(2)/CH_(4) mixtures by fixed-bed column breakthrough experiments.

关键词： Porous organic cage Calixresorcinarene Self-assembly Gas separation Host-guest interaction

Use of breakthrough experiment to evaluate the performance of hydrogen isotope separation for metal-organic frameworks M-MOF-74(M=Co, Ni, Mg, Zn)

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Science China Chemistry 2020年第7期63卷 881-889页

作者： Yanan Si Wenjing Wang El-Sayed M.El-Sayed daqiang yuan State Key Laboratoty of Structural Chemistry Fujian Institute o f Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of the Chinese Academy of Sciences Beijing 100049China Chemical Refining Laboratory Refining DepartmentEgyptian Petroleum Research InstituteNasr CityCairoEgypt

The unique adsorption performance of metal-organic frameworks(MOFs) indicates a new direction for gas separation and purification. The low-temperature distillation, as a traditional technique for hydrogen isotope separation, is limited as it is a high energy-and cost-intensive process. Instead of utilizing such a conventional separation route, we use ordered microporous frameworks based on a physical adsorption mechanism to solve the challenge of hydrogen isotope separation. Herein we analyze M-MOF-74(M=Co, Ni, Mg, Zn), featuring a hexagonal channel about 11 ? and high density of open metal sites, for their ability to separate and purify deuterium from the hydrogen isotope mixture by dynamic column breakthrough experiments. Our results show that the combination of the strength of binding sites, density of coordinatively unsaturated metal sites and hydrogen isotope adsorption capacity of materials renders Co-MOF-74 as an optimal adsorbent for the capture of deuterium from hydrogen isotope mixtures in a simulated industrial process.

关键词： hydrogen isotope separation breakthrough experiment MOF-74

3D metal-organic frameworks based on lanthanide-seamed dimeric pyrogallol[4]arene nanocapsules

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Science China Chemistry 2018年第6期61卷 664-669页

作者： Kongzhao Su Mingyan Wu Wenjing Wang Mi Zhou daqiang yuan Maochun Hong State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou 350002 China University of the Chinese Academy of Sciences Beijing 100049 China

Two novel 3D metal-organic frameworks(MOFs)with cds network,{[Me NH_3]_7[Ln_8(Pg C_2)_2(H_2O)_y(HCOO)_7]}_n·x(Solvent)(FJI-Y4,FJI=Fujian Institute,Ln=Gd,y=12;FJI-Y5,Ln=Dy,y=11;Pg C_2=C-ethylpyrogallol[4]arene),based on unprecedented dimeric pyrogallol[4]arene-based Ln_8metal-organic nanocapsule(MONC)supramolecular building blocks and formate linkers,have been prepared under solvothermal *** our best of knowledge,they present not only the first two examples of 3D hierarchical structures constructed from MONCs in metal-pyrogallol[4]arene system,but also the first two examples of MOFs based on lanthanide ***,the inner cavity volume of the Ln_8capsule in FJI-Y4 and FJI-Y5 is approximately151?~3,which is larger than those found in previous transition metal-seamed dimeric Pg C_n-based *** investigation on FJI-Y4 suggests a significant magnetocaloric effect(23.97 J kg^(-1)K^(-1),ΔH=7 T,2.5 K),while FJI-Y5 exhibits slow relaxation of the magnetization.

关键词： lanthanide pyrogallolarene metal-organic frameworks(MOFs) magnetic propeties

Highly effective H_(2)/D_(2)separation in a stable Cu-based metalorganic framework

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Nano Research 2021年第2期14卷 518-525页

作者： Yanan Si Xiang He Jie Jiang Zhiming Duan Wenjing Wang daqiang yuan State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Department of Chemistry College of SciencesShanghai UniversityShanghai 200444China University of the Chinese Academy of Sciences Beijing 100049China

A three-dimensional copper metal-organic framework with the rare chabazite(CHA)topology namely FJI-Y11 has been constructed with flexibly carboxylic ligand 5,5'-[(1,4-phenylenebis(methylene))bis(oxy)]diisophthalic acid(H_(4)L).FJI-Y11 exhibits high water stability with the pH range from 2 to 12 at temperature as high as 373 ***,FJI-Y11 also shows high efficiency of hydrogen isotope separation using dynamic column breakthrough experiments under atmospheric pressure at 77 *** to its excellent structural stability,FJI-Y11 possesses good regenerated performance and maintains high separation efficiency after three cycles of breakthrough experiments.

关键词： metal-organic framework(MOFs) hydrogen isotope separation breakthrough experiments

Synthesis and Characterization of Two Isostructural Lantha- nide-Containing Metal-Organic Frameworks Constructed from an Unprecedented [Ln7（μ3-OH）8]^13＋ Cluster

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Chinese Journal of Chemistry 2016年第2期34卷 210-214页

作者： Lianchao Liu Chaojun Shen Fangfang Dong Wenjing Wang daqiang yuan College of Chemistry Fuzhou University Fuzhou Fujian 350002 China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 China

Two isostructural metal-organic frameworks formulated as [Gd7（L）4（μ3-OH）8（HCOO）（DMF）6（H20）].DMF·H2O （1） and [Tbv（L）4（P3-OH）8（HCOO）（DMF）5（HzO）]·DMFoH2O （2）（H3L=3,5-di（4＇-carboxylphenyl）benzoic acid） have been synthesized and structurally characterized. The building blocks of the structures are the heptanuclear lanthanide clusters of the dicubane-like type [Lnv7（μ3-OH）s]13＋（Ln=Gd, Tb） which are formally assembled into porous three-dimensional networks through the linkage of L. Variable temperature magnetic studies down to 2 K reveal antiferromagnetic interactions in complex 1. Furthermore, the fluorescence property of 2 was also studied.

关键词： MOFs heptanuclear lanthanide cluster magnetic fluorescent

Linker extension through hard-soft selective metal coordination for the construction of a non-rigid metal-organic framework

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Science China Chemistry 2013年第4期56卷 418-422页

作者： WEI ZhangWen yuan daqiang ZHAO XiaoLiang SUN DaoFeng ZHOU Hong-Cai Department of Chemistry Texas A&M University College Station Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Key Lab of Colloid and Interface Chemistry Ministry of Education School of Chemistry and Chemical Engineering Shandong University

A metal-organic framework （MOF） has been obtained by using a linker extension strategy. Three di-anions of 4-（3,5-dimethyl- 1H-pyrazol-4-yl）-benzoic acid coordinate to three Cu（I） ions forming an extended trigon... 详细信息

关键词： MOF linker extension copper (I)

Highly Stable sp^(2) Carbon-Conjugated Porous Organic Cages

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CCS Chemistry 2024年第1期6卷 149-156页

作者： Fenglei Qiu Xun Chen Wenjing Wang Kongzhao Su daqiang yuan State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 College of Chemistry Fuzhou UniversityFuzhouFujian 350116 University of the Chinese Academy of Sciences Beijing 100049

The high-yield synthesis of ultrastable porous organic cages(POCs)by facile methods is highly desirable but *** by highly stable sp^(2) carbon-conjugated(C=C)covalent organic frameworks,we used rational design and synthesized the first family of sp^(2) carbon-linked POCs(sp^(2)c-POCs)with triangular prism shapes by a one-step Knoevenagel reaction that is a high yield[2+3]condensation *** stability of sp^(2)c-POC was demonstrated under strenuous conditions involving for example concentrated HCl or saturated NaOH ***^(2)c-POC was used as a robust adsorbent for efficient separation of CO_(2)/CH_(4) or CO_(2)/N_(2) *** view of their facile synthesis and unique properties,we expect widespread use of these sp^(2) C=C linkages in the development of POC materials.

关键词： porous organic cages Knoevenagel condensation sp^(2)C=C linkage exceptional chemical stability gas adsorption and separation properties

The competitive and synergistic effect between adsorption enthalpy and capacity in D_(2)/H_(2)separation of M_(2)(m-dobdc)frameworks

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Chinese Chemical Letters 2021年第11期32卷 3562-3565页

作者： Fan Wu Liqiong Li Yanxi Tan El-Sayed M.El-Sayed daqiang yuan 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 College of Chemistry Fuzhou UniversityFuzhou 350108China Chemical Refining Laboratory Refining DepartmentEgyptian Petroleum Research InstituteNasr CityCairo 11727Egypt

Hydrogen isotope separation is a challenging task due to their similar ***,based on the chemical affinity quantum sieve(CAQS)effect,the D_(2)/H_(2)separation performance of M_(2)(m-dobdc)(M=Co,Ni,Mg,Mn;m-dobdc^(4-)=4,6-dioxido-1,3-benzenedicarboxylate),a series of honeycomb-shaped MOFs with high stability and abundant open metal sites,are studied by gases sorption and breakthrough experiments,in which two critical factors,gas uptake and adsorption enthalpy,are taken into *** these MOFs,Co_(2)(m-dobdc)exhibits the longest D_(2)retention time of 180 min/g(H_(2)/D_(2)/Ne:1/1/98)at 77 K because of its second-highest adsorption enthalpy(10.7 kJ/mol for H_(2)and 11.8 kJ/mol for D_(2))and the best sorption capacity(5.22 mmol/g for H_(2)and 5.49 mmol/g for D_(2))under low pressure of 1 kPa and 77 K,which make it a promising material for industrial hydrogen isotope ***,the results indicate that H_(2)and D_(2)capacities under low pressure(about 1 kPa)dominate the final D_(2)/H_(2)separation property of MOFs.

关键词： Breakthrough experiment Open metal sites Hydrogen isotope separation Sorption and separation Chemical affinity quantum sieve