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The centrosymmetric to non-centrosymmetric transformation induced by alkaline-earth cations producing infrared nonlinear optical AeMn_(6)Ga_(6)S_(16)(Ae=Ca,Sr)

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Science China Chemistry 2024年第9期67卷 2941-2948页

作者： Yang-Ping Zhang Shao-Min Pei Wen-Fa Chen Bin-Wen Liu Xiao-Ming Jiang guo-cong guo State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China

Non-centrosymmetric(NCS)structure is an indispensable prerequisite for second-order nonlinear optical(NLO)***,the mainstream approach for designing new NCS structures still relies on chemical substitution,necessitating an urgent infusion of fresh *** this work,two isomorphic sulfides AeMn_(6)Ga_(6)S_(16)(Ae=Ca,1;Sr,2)are afforded by modifying the skeleton of centrosymmetric(CS)Mn_(2)Ga_(2)S_(5) via introducing strong electropositive alkaline-earth ***,the incorporation of Ca^(2+)/Sr^(2+)cations allows the elementary[MnGaS_(9)]_(∞)chains to reconfigure into bumpy[MnS_(6)]-[GaS_(4)]layers in a new engagement manner,thus enabling the conversion from CS to NCS *** modifications cause not only strong second-harmonic generation(SHG)responses(~1.5×benchmark AgGaS_(2)@1,700 nm),but also significantly feasible bandgaps(2.60-2.64 e V)compared to the sulfide Mn_(2)Ga_(2)S_(5)(1.36 e V),which ultimately facilitate ultrahigh laser-induced damage thresholds(4.4-6.6×AgGaS_(2)@1,064 nm for compounds 1 and 2).The present study offers an ingenious approach for the transformation of CS to NCS structure.

关键词： second-harmonic generation non-centrosymmetrical structure NLO functional motif solid-state method

Enhancing Electrochemical Reduction of CO_(2) to Formate by Regulating the Support Morphology

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Chinese Journal of Structural Chemistry 2021年第3期40卷 376-382,274页

作者： ZHAO Xiu-Hui ZHUO De-Huang CHEN Qing-Song guo guo-cong College of Chemistry Fuzhou UniversityFuzhou 350116China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Electroreduction of CO_(2) to formic acid has attracted extensive attention,because it is a promising strategy to re-utilize CO_(2) and reduce greenhouse gas emissions that may favor the mitigation of energy and environment *** great efforts have been made to tune the structure and composition of catalysts aiming to improve CO_(2) conversion efficiency,seldom studies have been focused on the support *** this work,ordered,porous TiO_(2) nanotube arrays have been used as model support to study the impact of pore structure for CO_(2) electrochemical *** has been revealed that Pd supported on TiO_(2) nanotube arrays substrate exhibits enhanced performance towards CO_(2) reduction,showing a higher formate Faradaic efficiency of 20%over than Pd supported on TiO_(2) film *** study will shed new light on the design and synthesis of efficient catalysts by tuning the morphology of support for CO_(2) conversion.

关键词： CO_(2)ER morphology electrochemistry formate

Synthesis and Structural Characterization of a New One-dimensional Infinite Chain of Silver(I) Complex with Triphenylphosphine

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Chinese Journal of Structural Chemistry 2004年第6期23卷 547-550页

作者： LIUBing ZHOUguo-Wei FUMing-Lai CAILi-Zhen guoguo-cong HUANGJin-Shun StateKeyLaboratoryofStructuralChemistry FujianInstituteofResearchontheStructureofMatterTheChineseAcademyofSciencesFuzhouFujian350002China GraduateSchooloftheChineseAcademyofSciences Beijing100039China

The reaction of triphenylphosphine with AgNO3 yielded an unusual nitrate anion bridging one-dimensional infinite chain [Ag(PPh3)NO3] in which the silver(I) atom is three-coordinated by one P atom of triphenylphosphine and two O atoms of two bridging nitrate anions to form a scalene triangle. The complex [Ag(PPh3)NO3] crystallizes in the monoclinic system, space group P21/c with a = 10.281(2), b = 18.596(5), c = 9.180(2) , = 90.60(1), V = 1755.1(7) 3, Z = 4, Mr = 432.15, Dc = 1.635 g/cm3, F(000) = 864 and = 1.254 mm-1. The final R = 0.0606 and wR = 0.1400 for 2188 observed reflections with I > 2(I) out of 3057 unique ones (Rint = 0.0539). IR and elemental analysis of the complex are characterized.

关键词： silver triphenylphosphine infinite chain organic hybrid crystal structure

Paired-Pd(Ⅱ) centers embedded in HKUST-1 framework: Tuning the selectivity from dimethyl carbonate to dimethyl oxalate

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Journal of Energy Chemistry 2022年第4期31卷 233-240页

作者： Hong-Zi Tan Zhe-Ning Chen Kai-Qiang Jing Jing Sun Yu-Ping Xu Ning-Ning Zhang Zhong-Ning Xu guo-cong guo State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina School of Chemistry&Chemical Engineering Shandong University of TechnologyZibo 255049ShandongChina School of Chemistry and Chemical Engineering Liaocheng UniversityLiaocheng 252000ShandongChina

CO oxidative coupling to dimethyl oxalate(DMO) is the most crucial step in coal to ethylene glycol. Pdbased supported catalysts have been verified effective for generating DMO, but concomitant generation of dimethyl carbonate(DMC) is always unavoidable. It is generally accepted that Pd(0) is the active species for producing DMO, while Pd(II) for DMC. However, density functional theory calculations have proposed that the selectivity to DMO or DMC highly depends on the space state of Pd species rather than its oxidative state. It is thus urgently desired to develop high-efficient catalysts with well-defined structure,and further to elucidate the structure-performance relationship. In this work, HKUST-1 with unique structure of paired-Cu(Ⅱ) centers was chosen as ideal support to construct the catalysts with respective paired-Pd(Ⅱ) centers and isolated-Pd(Ⅱ) centers via in situ Pd species doping. In despite of featuring Pdδ+(δ≈2) oxidation state, the synthesized paired-Pd(Ⅱ)/HKUST-1 catalyst still exhibited DMO as dominant product(90.8% of DMO selectivity). For isolated-Pd(Ⅱ)/HKUST-1 catalyst, however, the main product was DMC(84.8% of DMC selectivity). Based on catalyst characterizations, the structures of paired-Pd(Ⅱ) centers and isolated-Pd(Ⅱ) centers were determined. DMO was generated from the coupling of adjacent *COOCH;intermediates adsorbed on paired-Pd(Ⅱ) centers, while DMC was produced from the reaction between methyl nitrite and the *COOCH;intermediates formed on isolated-Pd(Ⅱ) centers. Current work is the first MOFs-based catalyst with well-defined structure being applied in CO oxidative coupling reaction, which not only sheds light on the structure-performance relationship, but also inspires the potential of using MOFs as tunable platform to design high-efficient catalysts in heterogeneous catalysis.

关键词： CO Methyl nitrite Oxidative coupling Dimethyl oxalate Paired-Pd(Ⅱ)centers HKUST-1

A New 1-D Chain ofγ-Hg_(3)S_(2)Br_(2)Constructed from Hg_(4)S_(4)Squares:Solid-state Synthesis,Structure and Optical Properties

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Chinese Journal of Structural Chemistry 2021年第2期40卷 264-269,148页

作者： DIAO Jian-Feng XIE Zhi-Xin LI Pei-Xin guo guo-cong College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Department of Chemistry Faculty of Arts and ScienceUniversity of TorontoTorontoOntario M5S3H6Canada

A new metal chalcogenide,γ-Hg_(3)S_(2)Br_(2)(1),has been prepared by moderate-temperature solid-state reaction,and its crystal structure was determined by single-crystal X-ray diffraction *** 1 crystallizes in space group Cmmm of orthorhombic system with a=9.1923(18),b=18.2262(5),c=4.6251(7)Å,V=774.9(3)Å^(3)and Z=*** the structure,two Hg(1),two Hg(2)and four S(1)atoms form a near square Hg_(4)S_(4),and such squares are linked by Hg(3)atoms nearly linearly coordinated to two S1 atoms of two parallel Hg_(4)S_(4)squares to form one-dimensional infinite Hg_(6)S_(4)chains along c *** absorption spectra reveal the presence of sharp optical gap of 2.80 eV for *** spectrum,TGA and electric resistivity have been investigated.

关键词： crystal structure metal chalcogenides resistance semiconductor solid-state reaction

Solid State Synthesis and Crystal Structure of K_3SI

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Chinese Journal of Structural Chemistry 2006年第2期25卷 159-162页

作者： ZHAO Zhen-Qian LIU Xi CHEN Wen-Tong LI Yan WUA-Qing ZENG Hui-Yi guo guo-cong HUANG Jin-Shun State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter The Chinese Academy of Sciences Fuzhou Fujian 350002 China Graduate School of the Chinese Academy of Sciences Beijing 100039 China

A new ternary alkali metal chalcogenide halide, K3SI, has been synthesized by solid state reaction method and structurally characterized by X-ray crystallography. The crystal belongs to hexagonal, space group P63cm with a = 11.699（I ）, c = 5.8279（9） A°, Mr = 276.26, V = 690.8（1 ）A°^ 3, Z = 6, D, = 3.985 g/cm^3, F（000） = 756, μ = 9.913 mm^-1, S = 1.004, R = 0.0719 and wR = 0.2204. The title compound is the first example containing S anion in the ternary alkali metal chalcogenide halides family M3QX （M = alkali metal, Q = chalcogenide, X - halide）, which crystallizes in the hexagonal anti-perovskite structure type.

关键词： crystal structure solid state synthesis ternary alkali metal chalcogenide halide

Phase Matching Achieved by Bandgap Widening in Infrared Nonlinear Optical Materials[ABa_(3)Cl_(2)][Ga_(5)S_(10)](A=K,Rb,and Cs)

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CCS Chemistry 2021年第3期3卷 964-973页

作者： Bin-Wen Liu Hui-Yi Zeng Xiao-Ming Jiang guo-cong guo State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002

Large nonlinear optical(NLO)coefficient(d_(ij)),high laser damage threshold(LDT),and phase matching(PM)are crucial for the practical applications of IR NLO crystals.A great number of IR NLO materials with high dij have been explored,but many of them suffer from non-PM,which dramatically decreases their ultimate NLO output *** settle this problem,we have developed a new strategy involving modulating normal dispersion via bandgap(E_(g))widening to achieve PM in this *** synthesized successfully three new wide E_(g)(∼4.0 eV)IR NLO salt-inclusion sulfides[ABa_(3)Cl_(2)][Ga_(5)S_(10)](A=K,1;Rb,2;and Cs,3)with PM behaviors,mainly ascribed to the PM cut-off wavelength blue shift that originated from the wide Eg values,with less contribution from birefringence *** the compounds possessed large second-harmonic-generation(SHG)efficiency(∼1×AgGaS_(2))and hitherto the highest LDTs(188–200 MW/cm^(2),at 1.06μm,10 ns pulse width)for known chalcogenides with SHG efficiencies comparable to that of commercial silver gallium sulfide(AgGaS_(2))crystal.

关键词： chalcogenide infrared nonlinear optic phase matching second-harmonic generation laser damage threshold

Light-Responsive Proton Conductor:Record High Gain of Proton Conductivity Achieved by Photoinduced Electron-Transfer Strategy

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CCS Chemistry 2021年第11期3卷 50-57页

作者： Xiu-Shuang Xing Cai Sun Lu Liu Ming-Sheng Wang guo-cong guo State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 Henan Key Laboratory of New Optoelectronic Functional Materials College of Chemistry and Chemical EngineeringAnyang Normal UniversityAnyang 455000 State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhouFujian 350108 Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian 350108

Light-responsive proton conductors might find applications in both traditional fields(fuel cells,chemical sensors,bio-ionic functions,etc.)and modern high-speed switchable smart systems(Internet of things,robotics,etc... 详细信息

关键词： photochromism photoinduced electron transfer proton conduction smart material viologen

Double Free:A Promising Route toward Moisture-Stable Hypotoxic Hybrid Perovskites

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CCS Chemistry 2022年第4期4卷 1273-1283页

作者： Guang-Ning Liu Ruo-Yu Zhao Rang-Dong Xu Cuncheng Li guo-cong guo School of Chemistry and Chemical Engineering University of JinanJinanShandong 250022 State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002

The moisture instability and toxicity of lead have hindered the development of lead organometal halide perovskites(Pb-OHPs).Similar to Pb-OHPs,OHPs based on Pb-free elements,including Group VA metals Bi and Sb(denoted as M),exhibit optoelectronic properties due to their isoelectronic configuration and close chemistry of the lone-pair ns^(2) ***,M-OHPs are mostly based on hydrophilic protonated organic countercations and possess low structural dimensionalities,which affect the moisture stability and disrupt continuous carrier transport,***,we demonstrate a“double-free”strategy to realize the rational synthesis of moisture-stable hypotoxic hybrid perovskites.A hydrogen-bond-free alkylated countercation was assembled with Pb-free OHP bearing an extended structure in one *** a proof of concept,two double-free M-OHPs are synthesized,which show greatly improved moisture and photostability compared to their corresponding hydrogen-bond OHPs and the extensively studied MA_(3)M_(2)X_(9)(MA=CH_(3)NH_(3)^(+)).The photoconduction behaviors of both double-free OHPs display short rise and decay recovery time and exhibit excellent photocurrent ***,(1-methyl-4-phenylpyridin-1-ium)BiI_(4)(Me4ppi-BiI_(4))displays a comparable switching on/off ratio with MA_(3)Bi_(2)I_(9),and can endure 75% relative humidity(RH)for at least 243 *** photophysical property measurements and theoretical calculations show that this remarkable photoconversion performance results from the relatively low exciton binding energy and greatly improved carrier mobility and concentration.

关键词： bismuth halide crystal structure hydrogen-bond-free inorganic-organic hybrid photoconductor