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[WS_(3)Cu_(2)]簇基超分子框的组装、结构及其三阶非线性光学响应

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无机化学学报 2024年第1期40卷 71-78页

作者：余蕙敏王志康李洁宋瑛林杜明浩郎建平苏州大学材料与化学化工学部苏州市资源分子精准转化重点实验室苏州215123

将二(4-吡啶)硫烷(L_(1))、4,4'-二(4-吡啶)二苯甲酮(L_(2))分别与(Et_(4)N)(Tp*WS_(3))(A)(Tp*=三(3,5-二甲基吡唑)氢合硼酸根)和[Cu(Me CN)_(4)]PF_(6)进行反应,得到2个W/Cu/S簇基超分子化合物[Tp*WS_(3)Cu_(2)(L_(1))]_(2)(PF_(6))_(2)·2Me CN·2CHCl_(3)(1·2Me CN·2CHCl_(3))和[Tp*WS_(3)Cu_(2)(L_(2))(Me CN)]_(2)(PF_(6))_(2)·4Me CN (2·4Me CN)。对配合物1·2Me CN·2CHCl_(3)和2·4Me CN分别进行了单晶X射线衍射、核磁、质谱、红外、紫外可见和元素分析表征。单晶X射线衍射分析表明,它们是由2个L_(1)/L_(2)配体连接2个[Tp*WS_(3)Cu_(2)]~+簇核形成的阳离子型簇基超分子框。核磁氢谱和高分辨电喷雾离子化质谱(HRESI-MS)证明它们在溶液中具有一定的稳定性。并利用Z扫描技术测试了超分子化合物1·2Me CN·2CHCl_(3)和2·4MeCN溶液的三阶非线性光学特性,测试结果表明它们的三阶非线性光学响应强于前驱体A。

关键词： W/Cu/S簇超分子框三阶非线性光学性质

Two Cluster-Based Coordination Polymers Derived from [Et_(4)N][Tp*WS_(3)(CuBr)_(3)] and CuCN: Isolation, Structures and Amplified Third-Order Nonlinear Optical Responses

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Chinese Journal of Chemistry 2014年第10期32卷 1065-1071页

作者： Quan Liu Wenhua Zhang Zhenrong Sun jianping lang College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China College of Chemistry and Chemical Engineering Nantong UniversityNantongJiangsu 226019China Department of Physics East China Normal UniversityShanghai 200062China

Treatment of a W/Cu/S precursor[Et_(4)N][Tp*WS_(3)(CuBr)_(3)](1)with three *** CuCN in DMF/MeCN/benzonitrile(or α-tolunitrile)yielded two[Tp*WS_(3)Cu_(3)(μ_(3)-DMF)]-based coordination polymers,[Tp*WS_(3)Cu_(3)(μ_(3)-DMF)(CN)_(3)Cu]_(2)•2DMF(2•2DMF)and[Tp*WS_(3)Cu_(3)(μ_(3)-DMF)(CN)_(3)Cu(α-tolunitrile)]_(2)•3MeCN(3•3MeCN),*** analysis revealed that 2 adopts a 2D network with a 4.8^(2) topology while 3 has a 1D ladder-type *** third-order nonlinear optical responses of 2 and 3 in DMF were 10 times enhanced compared to those of the precursor cluster 1.

关键词： W/Cu/S clusters CuCN coordination polymers crystal structures third-order NLO responses

Butterfly and Nest-Shaped Tp*-W-Cu-S Cluster Monomers and Dimers with Hexamethylenetetramine as Ligand:Anion-Dependent Structures and Nonlinear Optical Properties

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Chinese Journal of Chemistry 2021年第3期39卷 647-654页

作者： Quan Liu Mingie Lu Lice Yu Yinglin Song jianping lang College of Chemistry and Chemical Engineering Nantong UniversityNantongJiangsu 226019China College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhouJiangsu 215123China School of Physical Science and Technology Soochow UniversitySuzhouJiangsu 215006China

Main observation and conclusion The assembly of[Et4N][Tp*WS3](1)with CuX(Tp*=hydridotris(3,5-dimethylpyrazol-1-yl)borate;X=Cl,Br,andI)or[Cu(MeCN)][PF6]in the presence of tetratopic ligand hexamethylenetetramine(HMT)afforded an array of four cluster-based compounds,which are either neutral or *** compounds include[Tp*WSzCu3Cl2(HMT)](2,monomer,neutral),[Tp*WSzCugBr2(HMT)](3,monomer,neutral),[Tp*WSzCu3l1 s(HMT)21(4,dimer,anionic),and[Tp*WSzCu2(HMT)]2(PFc)2(5,dimer,anionic).The size of the halogen is found to dictate the structures(2/3 versus 4),and the presence/absence of halogen also affects the utiliation of coordinate site of HMT(4 versus 5)by creating more available CuOite in the case of *** structures of 2-5 are also characterized using elemental analysis,Fourier-transform infrared(FT-IR)spectra,and ultraviolet-visible(UV-Vis)spectroscopy,with the dimeric structure of 5 also selected for the third-order nonlinear optical(NLO)property *** NLO measurement results suggest that the hyperpola rizability value(v)of 5,reflecting its NLO properties as a neat material,features 2.12×10^(-30)esu,and it is comparable to other W/Cu/S clus-terbased molecular entities,rendering 5 a promising NLO-active material.

关键词： W/Cu/S cluster Hexamethylenetetramine Halogens Crystal growth Nonlinear optics

Coordination Polymers with Bipyridyl Diene and Triene Ligands:Synthesis,Structures and Luminescent Properties

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Chemical Research in Chinese Universities 2022年第1期38卷 209-216页

作者： HUA Chen YI Pin LIU Wencong WANG Mengfan NIU Zheng lang jianping College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123P.R.China

Solvothermal reactions of cadmium salts with bipyridyl diene and triene ligands[1,3-bis((E)-2-(pyridin-4-yl)vinyl)benzene-(1,3-bpeb) and 1,6-bis(4-pyridyl)-1,3,5-hexatriene(bphte)] and one bipyridyl triene ligand[1,6-bis(4-pyridyl)-1,3,5-hexatriene-(bphte)] in the presence of auxiliary carboxylic acids including 2,6-dichlorobenzoic acid(2,6-HDCBA) and 2-naphthal-enecarboxylic acid(2-HNCA) gave rise to four coordination polymers[Cd(bphte)(2,6-DCBA)2]n(1), {[Cd(bphte)(2-NCA)2]·5.8H2O}n(2),[Cd2(1,3-bpeb)2(2,6-DCBA)4]n(3) and {[Cd4(1,3-bpeb)4(2-NCA)7(HCOO)]·2-HNCA·H2O}n(4), respectively. Compounds 1-4 were structurally characterized by elemental analysis, IR, 1H NMR, powder X-ray diffraction, thermogravimetric analysis and single-crystal X-ray diffraction. They possess one-dimensional linear(1, 2) and zigzag(3, 4) chain structures. Their luminescent properties were explored while the representative sample 4 exhibited good luminescent performance in sensing Fe(III) in water.

关键词： Coordination polymer Bipyridyl olefinic ligand Crystal structure Luminescent property

Multiple structural defects in ultrathin NiFe-LDH nanosheets synergistically and remarkably boost water oxidation reaction

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Nano Research 2022年第1期15卷 310-316页

作者： Zhongyin Zhao Qi Shao Jiangyan Xue Bolong Huang Zheng Niu Hongwei Gu Xiaoqing Huang jianping lang College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HornKowloonHong Kong SARChina

Modifying electrocatalysts nanostructures and tuning their electronic properties through defects-oriented synthetic strategies are:essential to improve the oxygen evolution reaction(OER)performance of *** synthetic strategies *** mainly target the single or double structural defects,while the researches about the synergistic effect of multiple'structural defects are *** this work,the ultrathin NiFe layered double hydroxide nanosheets with a holey structure,oxygen;vacancies and Ni^(3+)defects on nickel foam(NiFe-LDH-NSs/NF)are prepared by employing a simple and green H202-assisted etching 1 *** synergistic effect ofthe above three defects leads to the exposure *** active sites and significant improvement of:the intrinsic *** optimized catalyst exhibits an excellent OER performance with an extraordinarily low overpotential of 170 mV;at to mA·cm^(-2) and a small Tafel slope of 39.3 mV·dec^(-1) in 1 M KOH *** functional theory calculations reveal this OER;performance arises from pseudo re-oxidized metal-stable Ni^(3+)near oxygen vacancies(O_(vac)),which suppresses 3d-e_(g) of Ni-site and!elevates d-band center towards the competitively low *** work provides a new insight to fabricate advanced electrocatalysts for renewable energy conversion technologies.

关键词： layered double hydroxide holey structures oxygen vacancies Ni3+defects oxygen evolution reaction

One-pot pyrolysis synthesis of highly active Ru/RuOx nanoclusters for water splitting

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Nano Research 2022年第2期15卷 1020-1026页

作者： Fengyuan Zhu Jiangyan Xue Lingjian Zeng Jingrui Shang Shuanglong Lu Xueqin Cao Brendan F.Abrahams Hongwei Gu jianping lang College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China School of Chemical and Material Engineering Jiangnan UniversityWuxi 214122China School of Chemistry University of MelbourneVictoria 3010Australia

Using simple methods to obtain efficient catalysts has been a long-standing goal for *** this work,the employment of a one-pot pyrolysis reaction to achieve molecular confinement,has led to the preparation of ruthenium(Ru)-based nanoclusters in a carbon matrix.A unique feature of the synthetic approach employed is that solvent and substrates were calcined *** solvent evaporates,during calcination,the substrates form a dense solid which has the effect of limiting the aggregation of Ru centers during the carbonization *** catalyst prepared in this simple manner showed an impressively high activity with respect to the hydrogen/oxygen evolution reaction(HER/OER).The Ru nanoclusters(Ru NCs),as the hydrogen evolution reaction(HER)catalysts,require ultralow overpotentials of 5 mV and 5.1 mV at-10 mA·cm^(-2) in 1.0 M KOH,and 0.5 M H_(2)SO_(4),***,the catalyst prepared by the one-pot method has higher crystallinity,a higher Ru content and an ultrafine cluster size,which contributes to its exceptional electrochemical ***,the RuO_(x) nanoclusters(RuO_(x) NCs),obtained by oxidizing the aforementioned Ru NCs,exhibited good oxygen evolution reaction(OER)performance with an overpotential of 266 mV at 10 mA·cm^(-2).When applied to overall water splitting,Ru/RuO_(x) nanoclusters as the cathode and anode catalysts can reach 10 mA·cm^(-2) at cell voltages of only 1.49 V in 1 M KOH.

关键词： pyrolysis ruthenium nanoclusters ruthenium dioxide nanoclusters hydrogen evolution reaction oxygen evolution reaction overall water splitting

Pore-Directed Solid-State Selective Photoinduced E–Z Isomerization and Dimerization within Metal–Organic Frameworks

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CCS Chemistry 2023年第5期5卷 1225-1232页

作者： Shu-Li Chen Yan Mi Fei-Long Hu David James Young jianping lang Key Laboratory of Chemistry and Engineering of Forest Products State Ethnic Affairs CommissionGuangxi Minzu UniversityNanning 530006Guangxi College of Chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123Jiangsu College of Engineering IT and EnvironmentCharles Darwin UniversityDarwin 0909Northern Territory

Design and construction of suitable pore microenvironments for selective catalytic reactions of small guest molecules is a major goal for ***,we report control of competitive E–Z photoisomerization and photodimerization within porous metal–organic frameworks(MOFs)by fine-tuning the pore microenvironments using different dicarboxylate *** with small pores((E)-X_(MOF_(1))and(E)-X_(MOF_(1))′)favor the photoinduced E–Z isomerization of one encapsulated diaryl alkene substrate while those with large pores(((E)-X)_(2MOF_(2)))prefer the photodimerization of two encapsulated alkene *** reactions show broad functional group compatibility and proceed stereospecifically in good yields under mild *** local concentration of diaryl alkene ligands and their preorientation within pores facilitate stereoselective *** pore engineering strategy is applicable to control and create pore microenvironemnts for other photoinduced organic reactions within porous MOFs.

关键词： pore engineering E–Z photoisomerization photodimerization metal–organic frameworks solid-state reaction

Construction of [Cu_nI_n]-based coordination polymers via flexible benzimidazolyl-based ligands

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Science China Chemistry 2010年第10期53卷 2083-2090页

作者： LI LingLing, REN ZhiGang, Lü Xue, WANG HeMing, CHANG YuJie, LI HongXi, WU Bing & lang jianping College of Chemistry, Chemical Engineering and Materials Science, Suzhou University, Suzhou 215123, China College of Chemistry Chemical Engineering and Materials Science Suzhou University Suzhou China

Four new [CunIn]-based coordination polymers, [{Cu4(μ3-I)4(mbbm)2}·2DMF]n (1), [(CuI)2(mbbm)2]n (2), [{Cu2(μ-I)2-(ebbm)2}·2MeCN]n (3), and [Cu2(μ-I)2(prbbm)2]n (4), were prepared from solvothermal reactions of CuI with three flexible ligands [(bzim)(CH2)n(bzim)] (bzim = benzimidazole; n = 1, mbbm; n = 2, ebbm; n = 3, prbbm). These compounds were characterized by elemental analysis, IR and X-ray crystallography. 1 consists of cubanelike [Cu4(μ3-I)4] fragments that link the neighboring ones via mbbm bridges to form a 1D ladder-type chain. 2 contains mononuclear [CuI] fragments that are bridged by mbbm ligands to yield a 1D zigzag chain. 3 or 4 contains a [Cu2(μ-I)2] dimeric fragment, which works as a four-connecting node to link its four equivalent ones to form a 2D (4,4) network (3) or acts as a two-connecting node to connect its two equivalent ones via two pairs of prbbm bridges to form a 1D double chain (4). The photoluminescent properties of 1-4 in the solid state at ambient temperature were investigated.

关键词： coordination polymers assembly flexible ligands solvothermal reactions photoluminescent properties

Syntheses of Secondary Amines and Imines via Acceptorless Dehydrogenation Reactions Catalyzed by Ru NPs on N-doped Carbon

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Syntheses of Secondary Amines and Imines via Acceptorless De...