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Gradual or Hysteretic Transition:anion effects on Cobalt(II)Spin Crossover Complexes

Chinese Journal of Chemistry 2024年第19期42卷 2381-2390页

作者： Yu-Chen Sun Ying-Lian Li Cheng-Cheng Zhang Feng-Li Chen Dong Shao Yue Zhao Hai-Yan Wei Xin-Yi Wang State Key Laboratory of Coordination Chemistry Collaborative Innovation Center of Advanced MicrostructuresSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjingJiangsu 210023China Jiangsu Key Laboratory of Biofunctional Materials School of Chemistry and Materials ScienceNanjing Normal UniversityNanjingJiangsu 210023China Hubei Key Laboratory of Processing and Application of Catalytic Materials College of Chemistry and Chemical EngineeringHuanggang Normal UniversityHuanggangHubei 438000China

Comprehensive Summary To better understand the impact of different anions on the structures and SCO properties of the CoII SCO complexes,six new complexes[Co(terpy-CH_(2)OH)_(2)]A_(2)·sol(terpy-CH_(2)OH=4′-(hydroxymethyl)-2,2′;6′,2″-terpyridine,A=Br^(–)(1,sol=1.5H_(2)O),I^(–)(2),N_(3)^(–)(3,sol=2H_(2)O),H_(3)BCN^(–)(4),OTf^(–)(5),and TsO^(–)(6,sol=4H_(2)O·CH_(3)CN),have been synthesized and *** six compounds consist of mononuclear[Co(terpy-CH_(2)OH)_(2)]^(2+)cations and charge-balancing anions that differ in size,shape,and hydrogen bonding *** 1,2,3,and 6 displayed incomplete gradual SCO transitions,whereas 4 and 5 exhibited abrupt hysteretic spin transitions with loops of 12 and 16 K(250.0—262.0 K for 4,and 370.0—386.0 K for 5,respectively),closely resembling our previously reported complexes with SCN^(–)and SeCN^(–)*** occurrence of the order-disorder transition of the CH2OH groups and their transition temperatures are determined by the size and hydrogen bonding capability of the ***,the transition temperatures of complexes with H_(3)BCN^(–),SCN^(–),OTf^(–),and SeCN^(–)anions exhibit an upward trend as the size and mass of the anions increase,as confirmed through detailed single crystal structure analyses conducted in both high-spin and low-spin states for all four complexes.

关键词： Cobalt Solid-state structures Magnetic properties Spin crossover anion effect

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Mechanistic investigation of zwitterionic MOF-catalyzed enyne annulation using UNLPF-14-Mn^(Ⅲ) as catalyst

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Chinese Chemical Letters 2022年第9期33卷 4281-4286页

作者： Taotao Liu Ruihong Duan Yanyan Wang Shijun Li Lingbo Qu Jinshuai Song Qiang Liu Yu Lan Green Catalysis Center and College of ChemistryZhengzhou UniversityZhengzhou 450001China Center of Basic Molecular Science(CBMS) Department of ChemistryTsinghua UniversityBeijing 100084China College of Chemistry and Chemical Engineering Henan Institute of Science and TechnologyXinxiang 453000China School of Chemistry and Chemical Engineering and Chongqing Key Laboratory of Theoretical and Computational ChemistryChongqing UniversityChongqing 400030China

Hybrid quantum mechanics/molecular mechanics calculations were performed to elucidate how[Mn^(Ⅲ)porphyrin]^(+X−)-based metal-organic frameworks(MOFs)catalyze the[2+1]cycloisomerization of enynes and why zwitterionic MOFs exhibit strong activity in Lewis acid *** calculations showed that zwitterionic MOFs have a“pure cationic active center”leading to a concerted nucleophilic attack pathway with lower *** contrast,metals with coordinating anions have reduced electrophilicity,resulting in a stepwise radical-type pathway with much higher *** calculations showed the nature of catalysis was strongly depended on the charge on the anion ligand.A good linear relationship between the NPA charge and barrier was found,and verified by 73 anions with small derivations,which presents a universal adaptive character for various coordinated anions.

关键词： ONIOM QM/MM Zwitterionic MOF [Mn^(III)porphyrin]^(+X−) Enyne annulation Mechanism anion effect

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anionic Tuning of Zeolite Crystallization

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CCS Chemistry 2021年第12期3卷 189-198页

作者： Chang Sun Zhiqiang Liu Shuang Wang Hao Pang Risheng Bai Qifei Wang Wei Chen Anmin Zheng Wenfu Yan Jihong Yu State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012 State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics National Center for Magnetic Resonance in WuhanWuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhan 430071 College of Chemistry and Chemical Engineering Henan Province Function-Oriented Porous Materials Key LaboratoryLuoyang Normal UniversityLuoyang 471934 International Center of Future Science Jilin UniversityChangchun 130012

Zeolites are of great industrial relevance as catalysts,adsorbents,and ion-exchangers and typically synthesized under hydrothermal *** regulation of their crystallization process is of great significance for zeolite *** this work,we systematically investigate the role of anions in tuning zeolite crystallization via anion introduction including SO_(4)^(2−),F^(−),Cl^(−),Br^(−),I^(−),and SCN^(−) in the sodium form into the SiO2-TPAOH-H2O[tetrapropylammonium hydroxide(TPAOH)]synthetic system of silicalite-1 zeolite.

关键词： zeolite crystallization Hofmeister series anion effect structure-directing agent

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effect of Competing anions on Arsenate Adsorption onto Maghemite Nanoparticles

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Chinese Journal of Chemical Engineering 2012年第3期20卷 505-514页

作者： T.Tuutijrvi E.Repo R.Vahala M.Sillanp G.Chen Department of Civil and Environmental Engineering School of Science and TechnologyAalto UniversityP.O.Box 15200FI-00076 AaltoFinland Laboratory of Green Chemistry Faculty of TechnologyLappeenranta University of TechnologyPatteristonkatu 1FI-50100 MikkeliFinland Laboratory of Applied Environmental Chemistry Department of Environmental SciencesUniversity of Eastern FinlandPatteristonkatu 1FI-50100 MikkeliFinland Department of Chemical and Biomolecular Engineering the Hong Kong University of Science and TechnologyHong KongChina

This paper reports the effect of several competing anions on arsenate adsorption with maghemite nanoparticles. Sulphate （as SO4）, nitrate （as NO3-N）, phosphate （as PO4-P） ions and silicate-（as SiO2） were-studied in dual solution with arsenate. Moreover, the combined effect of ions and other water characteristics were examined with a natural groundwater sample which was spiked with a certain amount of arsenate. Arsenate batch adsorption experiments were carried out with two different kinds of maghemite-a commercially, available one and a homemade one using the sol-gel orocess. Sulohate （≤250 mg.L-1） and nitrate （≤ 12 mg.L-1） had a neglivible effect onthe arsenate （0.5 mg.L-1） adsorption at pH 3. However, both phosphate （42.9 mg·L-1） and silicate （450 mg.L-j） had an adverse impact on arsenate （43 mg.L-1） adsorption at pH 7. Phosphate （41.5 mg.L-1） showed minimal competition with arsenate （0.5 mg.L-1）, while silicate （410 mg.L-1） inhibition was insignificant for all studied As（V） concentrations at p.H 3. The removal of arsenate from the groundwater sample was as efficient as from labo-ratory water tor 0.3 mgL -1 AS（V） botll at pH3 and pH7.

关键词： anion effect groundwater nitrate phosphate silicate water treatment

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