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Self-separation ionic liquid catalyst for the highly effective conversion of H2S by α,β-unsaturated carboxylate esters under mild conditions

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green Energy & Environment 2024年第9期9卷 1440-1448页

作者： Wenjie Xiong Xiaomin Zhang Xingbang Hu Youting Wu Key Laboratory of Mesoscopic chemistry of MOE School of Chemistry and Chemical Engineering Nanjing University The institute of green chemistry and Engineering School of Chemistry and Chemical Engineering Nanjing University

The deep-processing utility of pure hydrogen sulfide （H2S） is a significant direction in natural gas chemical ***,a brand-new strategy of H2S conversion by a,β-unsaturated carboxylate esters into thiols or thioethers using task-specific carboxylate ionic liquids （ILs） as catalyst has been developed,firstly accomplishing the phase separation of product and catalyst without introducing the third *** can be considered as a cascade reaction in which the product selectivity can be controlled by adjusting the molar ratio of H2S to a,β-unsaturated carboxylate ***,the effects of ILs with different anions and cations,intermittent feeding operations,as well as pressure-time kinetic behaviors on cascade reaction were ***,the proposed interaction mechanism of H2S conversion using butyl acrylate catalyzed by[Emim][Ac]was revealed by DFT-based theoretical *** approach enables the self-phase separation promotion of catalyst and product and achieves 99%quantitative conversion under mild conditions in the absence of solvent,making the entire process ecologically ***-efficiency reaction activity can still be maintained after ten cycles of the ***,the good results,combined with its simplicity of operation and the high recyclability of the catalyst,make this green method environmentally friendly and *** is anticipated that this self-separation method mediated by task-specific ILs will provide a feasible strategy for H2S utilization,which will guide its application on an industrial scale.

关键词： Ionic liquid Cascade reaction Self-separation H 2 S conversion Catalysis

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Strong metal-support interaction between AuPd nanoparticles and oxygen-rich defect ZrO_(2) for enhanced catalytic 5-hydroxymethylfurfural oxidation

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Chinese chemical Letters 2024年第2期35卷 507-511页

作者： Yunlei Zhang Yiran Liu Wen Guan Mengxue Cao Yao Chen Pengwei Huo institute of green chemistry and chemical technology School of Chemistry and Chemical EngineeringJiangsu UniversityZhenjiang 212013China School of the Environment and Safety Jiangsu UniversityZhenjiang 212013China

The unique properties of metal oxide surfaces,crystal surfaces and defects play vital roles in biomass upgrading *** this work,hierarchical porous bowl-shaped ZrO_(2)(HB-ZrO_(2))with mixed crystal phase was designed and employed as the support for loading AuPd bimetal with different proportions to synthesize AuPd/HB-ZrO_(2) *** effects of surface chemistry,oxygen defects,bimetal interaction and metal-support interaction of AuPd/HB-ZrO_(2) on catalytic performance for the selective oxidation of 5-hydroxymethylfurfural(HMF)to 2,5-furandicarboxylic acid(FDCA)were systematically *** Au 2 Pd1/HB-ZrO_(2) catalyst afforded a satisfactory FDCA yield of 99.9%from HMF oxidation using O_(2) as the oxidant in water,accompanied with an excellent FDCA productivity at 97.6 mmol g^(−1) h^(−1).This work offers fresh insights into rationally designing efficient catalysts with oxygen-rich defects for the catalytic upgrading of biomass platform chemicals.

关键词： 5-Hydroxymethylfurfural oxidation 2,5-Furandicarboxylic acid Oxygen-rich defect ZrO_(2) AuPd bimetal Bowl-shaped structure

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Application of surfactant for improving leaching process of weathered crust elution-deposited rare earth ores

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Journal of Rare Earths 2024年第1期42卷 181-190,I0007页

作者： Fang Zhou Lisen Zhang Zhiwei Wang Yixin Zhang Ru'an Chi Xiaoyan Wu Key Laboratory for green chemical Process of Ministry of Education Wuhan Institute of TechnologyWuhan430073China

Weathered crust elution-deposited rare earth ores(WREOs)in China are the main source of medium and heavy rare earths in the *** order to improve the seepage and the mass transfer of traditional ammonium salt leaching process of WREOs,surfactants were added in the ammonium sulfate leaching solution and the ammonium chloride leaching *** leaching kinetics,the mass transfer process,and the adhesion work reduction factor calculated from the interfacial properties were studied to reveal the strengthening mechanism of *** the presence of the tested five surfactants,cetyl trimethyl ammonium bromide(CTAB),dodecyl trimethyl ammonium bromide(DTAB),sodium dodecyl sulfate(SDS),sodium oleate and oleic acid,the permeability of WREOs is improved,the rare earth(RE)leaching efficiency increase and the impurity aluminum(Al)leaching efficiency decrease,indicating its promotional effect on the leaching process of ***,CTAB shows a better leaching enhancement,and the optimal addition dosage is 0.4 g/L for the two ammonium salt leaching agent *** kinetics analysis shows the internal diffusion controls model of RE and Al leaching process,and the leaching kinetics equations of RE and Al related to CTAB concentration were obtained for the two ammonium salt leaching *** to the chromatographic plate theory,the mass transfer efficiency of RE increases with the CTAB concentration increasing until 0.4 g/L,which confirms that the optimal CTAB addition is 0.4 g/*** adhesion work and adhesion work reduction factor indicate more favorable permeation as well as the leaching process.

关键词： Weathered crust elution-deposited rare earth ores Surfactant Kinetics Mass transfer

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A chiral fluorescent probe for molecular recognition of basic amino acids in solutions and cells

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Chinese chemical Letters 2024年第10期35卷 390-395页

作者： Chuan-Zhi Ni Ruo-Ming Li Fang-Qi Zhang Qu-Ao-Wei Li Yuan-Yuan Zhu Jie Zeng Shuang-Xi Gu School of chemistry and Environmental Engineering School of Chemical Engineering & Pharmacy Pharmaceutical Research Institute Hubei Key Laboratory of Novel Reactor and Green Chemical Technology Wuhan Institute of Technology Nanjing Pusheng Biomedical Co. Ltd.

A novel and readily available binaphthyl-based fluorescent probe（S）-1 was designed and synthesized.（S）-1 can be used to not only chemoselectively discriminate 3 basic amino acids out of common amino acids, but also enantioselectively recognize histidine. Encouragingly, enantioselective imaging of histidine in cells was achieved for the first time by the probe（S）-1. These performances endowed it potential application in the chiral analysis of basic amino acids in asymmetric synthesis and cell imaging for diagnosis of diseases caused by racemization of histidine. Nuclear magnetic resonance（NMR） and mass spectrometry investigations suggested that different reaction extent of（S）-1 with L/D-histidine and different product structures generated the observed enantioselective fluorescent response. The molecular structures and thermodynamic stability of the complexes, formed from（S）-1 + Zn2+and enantiomers of histidine, were calculated by Gaussian 16 based on density functional theory（DFT） to validate the above action mechanism.

关键词： Basic amino acids Cell imaging Chemoselectivity Chiral recognition Enantioselectivity Fluorescent probe

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Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol

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Chinese Journal of chemical Engineering 2024年第1期65卷 19-28页

作者： Xiaojing Liu Ruohan Zhao Hao Zhao Zhimiao Wang Fang Li Wei Xue Yanji Wang Hebei Provincial Key Laboratory of green chemical technology and High Efficient Energy Saving School of Chemical Engineering and TechnologyHebei University of TechnologyTianjin 300130China Tianjin Key Laboratory of chemical Process Safety Tianjin 300130China Hebei Industrial technology Research institute of green chemical Industry Huanghua 061100China

Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and ***,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticles(NPs)on nitrogen-doped carbon;synthesized by using F127 as a stabilizer,as well as chitosan as a carbon and nitrogen *** Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate,exhibiting higher stability than Pd/NC prepared without F127 *** hydrogen bond between chitosan(CTS)and F127 was enhanced by F127,which anchored the N in the free amino group,increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd *** process helped to improve metal *** increased metal-support interaction,which limits the leaching and coarsening of Pd NPs,improves the stability of the Pd/NCF ***,density functional theory calculations indicated that pyridine N stabilized the Pd^(2+)species,significantly inhibiting the loss of Pd^(2+)in Pd/NCF during the reaction *** work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts.

关键词： Supported Pd catalyst N-doped carbon Amphiphilic triblock copolymer Pyridinic nitrogen Stability

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Activity promotion of Rh_(1)Ca_(x)/Al_(2)O_(3) single-atom catalyst in 1-octene hydroformylation:a volcano curve exists between Ca adding ratio and catalytic activity

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Science China chemistry 2024年第4期67卷 1187-1192页

作者： Hao Zhang Xingcong Zhang Xilun Wang Qingdi Sun Hao Liu Hongbing Ji Xiaohui He Key Laboratory of Bioinorganic and Synthetic chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou 510275China Huizhou Research institute Sun Yat-sen UniversityHuizhou 516081China State Key Laboratory Breeding Base of green-chemical Synthesis technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous *** conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and ***,a volcano curve between Ca addition ratio and catalytic activity is *** Ca significantly increases activity by decreasing the energy barrier,but excessive Ca decreases activity due to hindering substrate adsorption and reaction.

关键词： hydroformylation bimetallic single-atom catalysts rhodium heterogeneous catalyst

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Highly selective electrosynthesis of 3,4-dihydroisoquinoline accompanied with hydrogen production over three-dimensional hollow CoNi-based microarray electrocatalysts

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Nano Research 2024年第4期17卷 2509-2519页

作者： Yu Xin Liyu Chen Yingwei Li Kui Shen Guangdong Provincial Key Lab for green chemical Product technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China State Key Laboratory of Pulp and Paper Engineering School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

Electrocatalytic oxidation reaction of biomass-based derivatives is an excellent candidate to replace water oxidation for obtaining both value-added products and hydrogen(H_(2)),but the exploration of competent electrocatalysts is still highly ***,two new types of three-dimensional self-supported hollow microarrays containing CoNi layered double hydroxide(CoNi-LDH)and N-doped carbon nanosheets decorated with CoNi alloyed nanoparticles(CoNi-NC)on carbon cloth(CC)are prepared,which are further used as efficient electrocatalysts for tetrahydroisoquinoline(THIQ)electrooxidation and hydrogen evolution reaction(HER),*** demonstrate that the Co-modulated electronic environment for Ni(II)/Ni(Ⅲ)redox-looping in CoNi-LDH is the main factor to boost the selectivity of 3,4-dihydroisoquinoline(DHIQ)for the indirect electrooxidation process of *** functional theory(DFT)calculations reveal that the Ni(Ⅲ)/Co(Ⅲ)dual sites of CoNi-LDH exhibit enhanced adsorption for THIQ but poorer adsorption for DHIQ compared to pure Co(Ⅲ)or Ni(Ⅲ).Therefore,the Ni(Ⅲ)/Co(Ⅲ)dual sites can effectively inhibit the peroxidation of DHIQ to isoquinoline(IQ)over CoNi-LDH,thus improving the selectivity of DHIQ to nearly 100%,much higher than that of its pure Ni ***,CC@CoNi-NC can deliver high HER activity with low overpotential(40 mV@10 mA·cm^(-2))and high exchange current density(3.08 mA·cm^(-2)).Impressively,the assembled flow-cell device with CC@CoNi-LDH anode and CC@CoNi-NC cathode only requires low cell voltage and electricity consumption of 1.6 V and 3.50 kWh per cubic meter of H_(2)(@25 mA·cm^(-2)).

关键词： highly selective electrosynthesis dihydroisoquinolines hydrogen evolution reaction metal-organic frameworks hollow microarrays

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Interface engineering enabled sintering-resistant metal nanocatalysts via reverse Ostwald ripening

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Science China chemistry 2024年第9期67卷 2789-2791页

作者： Ying Sun Wenhui Fang Jieshan Qiu institute of Clean Energy chemistry Key Laboratory for Green Synthesis and Preparative Chemistry of Advanced Materials of Liaoning ProvinceCollege of ChemistryLiaoning UniversityShenyang 110036China State Key Laboratory of chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029China

The design and fabrication of advanced nanocatalysts with the high activity,selectivity,and superior durability remains a big challenge in industrial catalysis[1,2].The sintering of nanocatalysts under the thermally and/or chemically triggered conditions is a bottle-neck issue,which seriously decreases the amount of the exposed active sites and changes the original electronic structure of catalysts,resulting in the irreversible catalyst deactivation and high capital and time cost in industrial operation[3].

关键词： durability irreversible catalysis

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Compositional evolution for mixed aerosols containing gluconic acid and typical nitrate and the effect of multiply factors on hygroscopicity

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Journal of Environmental Sciences 2024年第5期139卷 206-216页

作者： Yue Zhu Shufeng Pang Yunhong Zhang School of chemistry and chemical Engineering Beijing Institute of TechnologyBeijing 100081China

The aging process of atmospheric aerosols usually leads to a mixture of inorganic salts and organic compounds of anthropogenic *** organic compounds,polyhydroxy organic acids are important components,however,the study on composition and hygroscopic properties of the mixture containing inorganics and polyhydroxy organic acids is *** this study,gluconic acid,the proxy of polyhydroxy organic acids,is mixed with the representative nitrate(Mg(NO_(3))_(2),Ca(NO_(3))_(2))to form ***-FTIR and optical microscopy are employed to study the component changes and hygroscopicity as a function of relative *** relative humidity fluctuates,the FTIR-ATR spectra display that the internal mixed gluconic acid(CH_(2)(CH)_(4)(OH)_(5)COOH)and nitrate can react to release acidic gases,forming relevant gluconate and further affecting the *** specific presentation is particles cannot be recovered to their original size after the dehydration-hydration process and there will be some disparities in GF for mixed *** the gluconic acid-Ca(NO_(3))_(2)/Mg(NO_(3))_(2)mixtures with molar ratios of 1:1,higher degree of reaction resulting in the production of large amounts of gluconate should be responsible to the lower hygroscopicity compared to ZSR *** 1:2 gluconic acid-nitrate mixed systems(with higher nitrate content),the hygroscopicity of mixtures are higher than the ZSR prediction.A possible reason could be‘salt-promoting effect’on the organic fractions of the surplus inorganic salt in the *** data can improve the chemical composition list evaluation,in turn hygroscopic properties and phase state of atmospheric aerosol,and then the climate effect.

关键词： Hygroscopicity Gluconic acid Reaction ZSR simulation Size growth factors

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Role of methoxy and C_(α)-based substituents in electrochemical oxidation mechanisms and bond cleavage selectivity of β-O-4 lignin model compounds

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green Energy & Environment 2024年第1期9卷 114-125页

作者： Yang Zhou Qiang Zeng Hongyan He Kejia Wu Fuqiao Liu Xuehui Li School of chemistry and chemical Engineering The Guangdong Provincial Key Laboratory of Green Chemical Product TechnologyState Key Laboratory of Pulp and Paper EngineeringSouth China University of TechnologyGuangzhouGuangdong510640China CAS Key Laboratory of green Process and Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing100190China

In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para-methoxy(on the aryl ring closing to Cα) and Cα-OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the Cα-Cβbond cleavage induced by electrochemical oxidations.

关键词： Lignin model compounds β-O-4 dimers Electrochemical oxidation Oxidation mechanisms Substituent effect

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