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Highly Efficient Au/TiO_(2) Catalyst for One-pot Conversion of Nitrobenzene to p-Aminophenol in Water Media

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Chinese Journal of Chemistry 2014年第3期32卷 257-262页

作者： Luyao Zou Yuanyuan Cui Weilin Dai Department of Chemistry and Shanghai Key Laboratory of Molecular catalysis and innovative Materials Fudan UniversityShanghai 200433China

Au/TiO_(2) catalyst is firstly reported to be efficient in the hydrogenation of nitrobenzene to produce p-aminophenol with a high PAP selectivity of 81%and overall yield more than 63%.The catalyst is also quite stable... 详细信息

关键词： nitrobenzene p-aminophenol Au/TiO_(2)catalyst hydrogenation

Remarkably reducing carbon loss and H2 consumption on Ni–Ga intermetallic compounds in deoxygenation of methyl esters to hydrocarbons

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Journal of Energy Chemistry 2020年第2期29卷 194-208页

作者： Ning Zhao Ying Zheng Jixiang Chen Tianjin Key Laboratory of Applied catalysis science and Technology Department of Catalysis Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China

Ni–Ga alloy(Ni/Ga atomic ratio of 8),Ni3Ga and Ni5Ga3 intermetallic compounds(IMCs)catalysts were prepared from Ni–Mg-Al-Ga layered double hydroxides(LDHs)for the deoxygenation of methyl esters to *** the alloy and IMCs,the presence of Ga reduced the surface Ni atom density,and the charge transfer from Ga to Ni increased the electron density of *** the deoxygenation of methyl laurate,the Ni catalyst gave a complete hydrogenolysis of methyl laurate to CH4at 330°C and 3.0 MPa,while the presence of Ga promoted the HDO pathway and suppressed C–C bond hydrogenolysis and *** Ni5Ga3 catalyst exhibited the best desired *** at 400°C,it gave the yield of C11 and C12 hydrocarbons of ~99%,and the selectivity to CH4(SCH4) was only 2.4%.In the deoxygenation of methyl octanoate and methyl palmitate,the Ni5Ga3 catalyst also gave the yield of hydrocarbons above95%.Reactivity evaluation and methyl propionate-TPD and TPSR results indicate that the C–OCH3 bond instead of the O–CH3 one was cleaved on both Ni and bimetallic Ni–Ga *** is highlighted that methanol,derived from the C–OCH3 bond hydrogenolysis,mainly decomposed to CO and H2 on IMCs,while it was converted to methane on metallic Ni and *** is of great significance that H2 could be yielded from the methyl ester *** short,the utilization of Ni–Ga IMCs can effectively reduce carbon loss and H2 consumption,all of which are ascribed to the geometric and electronic effects of Ga.

关键词： Ni–Ga intermetallic compounds Methyl ester Decarbonylation/decarboxylation Hydrodeoxygenation C–C bond hydrogenolysis Methanation

Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated Ni–Sn intermetallic compounds with methanol as hydrogen donor

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Frontiers of Chemical science and Engineering 2023年第2期17卷 139-155页

作者： Haonan Shi Xiaoyu Gu Yinteng Shi Dandan Wang Sihao Shu Zhongze Wang Jixiang Chen Tianjin Key Laboratory of Applied catalysis science and Technology Department of Catalysis Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China

Porous carbon-encapsulated Ni and Ni-Sn intermetallic compound catalysts were prepared by the one-pot extended Stöber method followed by carbonization and tested for in-situ hydrothermal deoxygenation of methyl palmitate with methanol as the hydrogen *** the catalyst preparation,Sn doping reduces the size of carbon spheres,and the formation of Ni-Sn intermetallic compounds restrain the graphitization,contributing to larger pore volume and pore ***,a more facile mass transfer occurs in carbon-encapsulated Ni-Sn intermetallic compound catalysts than in carbonencapsulated Ni *** the in-situ hydrothermal deoxygenation,the synergism between Ni and Sn favors palmitic acid hydrogenation to a highly reactive hexadecanal that easily either decarbonylate to n-pentadecane or is hydrogenated to *** high reaction temperature,hexadecanol undergoes dehydrogenation-decarbonylation,generating ***,the C-C bond hydrolysis and methanation are suppressed on Ni-Sn intermetallic compounds,favorable for increasing the carbon yield and reducing the H_(2) *** npentadecane and n-hexadecane yields reached 88.1%and 92.8%on carbon-encapsulated Ni_(3) Sn_(2) intermetallic compound at 330℃.After washing and H_(2) reduction,the carbon-encapsulated Ni_(3) Sn_(2) intermetallic compound remains stable during three recycling *** is ascribed to the carbon confinement that effectively suppresses the sintering and loss of metal particles under harsh hydrothermal conditions.

关键词： extended Stöber method carbon encapsulated Ni-Sn intermetallic compounds confinement in-situ hydrothermal deoxygenation hydrogenation decarbonylation

Carbon-coated Ni-Co alloy catalysts:preparation and performance for in-situ aqueous phase hydrodeoxygenation of methyl palmitate to hydrocarbons using methanol as the hydrogen donor

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Frontiers of Chemical science and Engineering 2022年第4期16卷 443-460页

作者： Yinteng Shi Lin Ai Haonan Shi Xiaoyu Gu Yujun Han Jixiang Chen Tianjin Key Laboratory of Applied catalysis science and Technology Department of Catalysis Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China

Carbon-coated Ni,Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber *** was found that the introduction of Co remarkably reduced the carbon microsphere *** metallic Ni,Co,and Ni-Co alloy particles(mainly 10-12 nm)were uniformly distributed in carbon microspheres.A charge transfer from Ni to Co appeared in the Ni-Co *** with those of metallic Ni and Co,the d-band center of the Ni-Co alloy shifted away from and toward the Fermi level,*** the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330℃,the decarbonylation/decarboxylation pathway dominated on all *** Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts,and the yields of n-pentadecane and n-C6-n-C16 reached 71.6%and 92.6%,*** excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon *** to the confinement effect of carbon,the metal particles showed high resistance to sintering under harsh hydrothermal *** deactivation is due to the carbonaceous deposition,and the regeneration with CO_(2) recovered the catalyst reactivity.

关键词： Stöber method carbon-coated Ni-Co alloy in-situ hydrodeoxygenation methyl palmitate decarbonylation decarboxylation

Effect of Fluorination on the Crystal Structure,Stability and Gas Adsorption Property in Zinc (Ⅱ) Metal-organic Frameworks

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Chinese Journal of Structural Chemistry 2022年第2期41卷 49-56,I0008页

作者： ZHANG Xin CHEN Zhen-Xia YANG Yong-Tai DENG Ming-Li WENG Lin-Hong Shanghai Key Laboratory of Molecular catalysis and innovative Materials Department of ChemistryFudan UniversityShanghai 200433China

Three zinc(Ⅱ) metal-organic frameworks (x F-MAC-3) have been synthesized by using Zn(Ⅱ) salts,3,5-dimethyl-1H-1,2,4-triazole (Hdmtrz) and different fluorination degree carboxylate ligands,which are analogic structures and can be described as (6,6)-connected pcu-b *** find that the fluorine atoms have structural regulation effect on x F-MAC-3,which can not only enlarge the torsion angle φ of carboxylate ligands but also elevate the space group of ***,the CO_(2)-273 K uptake increased from 23.21 cm^(3)·g^(-1) (MAC-3) to36.13 cm^(3)·g^(-1) (4F-MAC-3) and H_(2)-77 K uptake increased from 24.33 cm^(3)·g^(-1) (MAC-3) to 59.79 cm^(3)·g^(-1)(4F-MAC-3),which means fluorination can enhance the gas adsorption uptake of x F-MAC-3 ***,the results of fluorination in x F-MAC-3 analogues offer a potential way to study the ligand pre-functionalization effect on the structures and properties of MOFs analogues.

关键词： metal-organic frameworks fluorine functionalization X-ray crystallography gas adsorption

Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO2 in CO2 electroreduction

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Journal of Energy Chemistry 2025年第1期100卷 66-76页

作者： Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng Inner Mongolia Key Laboratory of Chemistry and Physics of Rare Earth Materials School of Chemistry and Chemical Engineering Inner Mongolia University State Key Laboratory of Coal Conversion Institute of Coal Chemistry Chinese Academy of Sciences Institute of catalysis Department of Chemistry Zhejiang University National Key Laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization Baotou Research Institute of Rare Earths

Conversion of CO2back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as ***,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based ***,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO2nanorods were effectively created,with adjustable vacancy/Cu *** resulting optimum catalyst shows up to 79% catalytic current density to hydrocarbons （excluding CO）,with 49% faradaic efficiency to *** and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to *** findings may spur new insights for designing and developing more controllable chemical process relevant to CO2utilization.

关键词： Nanorods

Synthesis and reaction of 16-electron Cp^tRh halfsandwich complexes containing 1,2- dichalcogenolate carborane ligands

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Chinese science Bulletin 2003年第16期48卷 1733-1736页

作者： KONG Qingan, JIN Guoxin, CAI Shuyi & WENG Linhong Laboratory of Molecular catalysis and innovative Material, Chemistry Department, Fudan University, Shanghai 200433, China Correspondence should be addressed to Jin Guoxin (e-mail: gxjin@ ***) Laboratory of Molecular catalysis and innovative Material Chemistry Department Fudan University Shanghai China

The reactions of [CptRhCl(m-Cl)]2 (1) (Cpt = tBu2C5H3) with Li2E2C2B10H10 (E = S, Se) lead to the green 16-electron dichalcogenolate complexes CptRh(E2C2B10H10) [E = S(2a), Se(2b)]. The 16-electron complexes 2a and 2b can take up two-electron donor ligands such as tert-butyl isoni-trile and carbon monoxide to give the 18-electron dichalco-genolate derivatives Cpt(L)(E2C2B10H10) [L = tBuNC, E = S(3a), Se(3b); L = CO, E = S(4a), Se(4b)]. The molecular structures of complexes 2a and 3a were determined by X-ray crystal structure analysis. The molecular structure of 16- electron complex 2a shows the pseudoaromatic system in IrSe2C2 five numbered ring.

关键词：碳硼烷配合体化合物异腈一氧化物晶体结构分析分子结构有限环

Fluorescent Silk Obtained by Feeding Silkworms with Fluorescent Materials

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Chinese Journal of Chemistry 2023年第16期41卷 2035-2046页

作者： Zhao-Fan Wu Zhao-Nan Sun Huan-Ming Xiong Department of Chemistry and Shanghai Key Laboratory of Molecular catalysis and innovative Materials Fudan UniversityShanghai 200438China

Comprehensive Summary Fluorescent silk has potential application in many fields such as bioimaging,tissue engineering scaffolds,luminescent marks,and dazzling *** the methods to endow natural silk with fluorescent properties,feeding silkworms with fluorescent additives is facile,low-cost and environment friendly,which has the prospect of large-scale *** this paper,we reviewed the research progress for this aim in the past ten years,and summarized the unified characteristics for the substances that can enter the silk gland by digestive tract of *** advantages and disadvantages of various fluorescent materials for this application are compared in *** the future research directions are suggested to overcome the shortcomings of the present research.

关键词： Fluorescent silk Fluorescent materials Feeding silkworms Carbon dots Nanoparticles Nanotechnology Multi-color emission Bioimaging

Synthesis and Crystal Structure of [Cp_2Ln(OC(SEt)NPh )]_2

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Chinese Journal of Structural Chemistry 2006年第2期25卷 131-134页

作者： ZHANG Chun-Mei LIU Rui-Ting ZHOU Xi-Geng Department of Chemistry Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Fudan University Shanghai 200433 China Department of Chemistry East China University of Science and Technology Shanghai 200237 China

Treatment of Cp3Y with EtSH, followed by reaction with an equivalent of PhNCO, yielded the dinuclear complex [Cp2Y（μ-η^1：η^3-OC（SEt）NPh）]2. The structure was characterized by elemental analysis, IR, MS and single-crystal X-ray diffraction analysis. The title compound crystallizes in triclinic, space group P1^- with a = 8.643（3）, b = 10.752（4）, c = 11.161（4）A°, α= 117.840（5）, β = 94.086（5）, γ= 101.008（5）°, V = 884.8（6） A°^3, Z = 1, Mr = 798.66 （C38H40N2O2S2Y2）, λ（MoKα） = 0.710730 .A°, ,μ= 3.417 mm^-1, Dc = 1.499 g/cm^3, F（000） = 408, the final R = 0.0453 and wR = 0.1007 for 3067 unique reflections （Rint = 0.0317） with 2357 observed ones （I 〉 2σ（I））. X-ray analysis reveals an unusual bonding mode of the OC（SEt）NPh ligand and the OCN fragment acts as a both bridging and side-on chelating ligand. Each yttrium atom is coordinated by two η^5-cyclopentadienyl groups, one chelating η^3-OC（SEt）NPh ligand and one bridging O atom from another η^3-OC（SEt）NPh ligand.

关键词： organolanthanide isocyanate insertion structure cyclopentadienyl