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Chinese Journal of Chemical Engineering 2023年第6期58卷 69-75页

作者： Qunfeng Zhang Bingcheng Li Yuan Zhou Deshuo Zhang chunshan lu Feng Feng Jinghui Lv Qingtao Wang Xiaonian Li Institute of Industrial Catalysis of Zhejiang University of Technology State Key Laboratory Breeding Base of Green Chemistry Synthesis TechnologyHangzhou 310014China

The overall performance of metal catalysts can be efficiently adjusted by modifying carbon carriers with different valence sulfur *** wet impregnation technique successfully prepared carbon material carriers doped with varying sources of sulfur(Na_(2)SO_(4),NaHSO_(3),Na_(2)S·9H_(2)O).Palladium carbon catalysts doped with different sulfur precursors had been prepared with the aid of the liquid-phase reduction method of the selective hydrogenation of o-chloronitrobenzene(o-CNB)to o-chloroaniline(o-CAN).The catalyst prepared for Na_(2)S·9H_(2)O as a precursor has excellent performance,and the selectivity for o-CAN is more than 99.9%at 100%*** addition,the characterization results show that with the decrease of S valence,the electronic effect between S and Pd increases,and the outer electron shift of Pd increases,which reduces the adsorption and dissociation ability of Pd to hydrogen,resulting in excellent *** effects provided a good idea for the hydrogenation of o-CNB and a different point of view on sulfur doping in a variety of hydrogenation reactions.

关键词： Catalyst Hydrogenation Selectivity Sulfur doping Electronic effect

Pt-Ni core-shell structure with Pt-skin and electronic effect on catalytic performance

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Chinese Journal of Chemical Engineering 2023年第11期63卷 260-267页

作者： Chong Yao Dandan Ma Jie luo Yixin Chen Min Tian Haoxuan Xie chunshan lu Feng Feng Xiaoliang Xu Qingtao Wang Qunfeng Zhang Xiaonian Li State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

In order to improve the catalytic performance of the nitrobenzene hydrogenation rearrangement to prepare p-aminophenol,a bimetallic Pt-Ni/C(PNC)catalyst was *** advantage of the synergistic effect of Ni and Pt to enhance product selectivity and catalytic performance stability,the electrons in Ni are moved to Pt by the electron effect,which affects the catalyst’s ability to activate H_(2)as well as the amount of hydrogen ***,due to the strong Pt(5d)-Ni(3d)coupling effect,Ni can effectively maintain Pt stability in the acidic system and reduce Pt *** stability of the PNC can be found to be greatly enhanced compared to the Pt/C(PC)catalyst,and p-aminophenol selectivity is greatly enhanced,showing excellent catalytic performance.

关键词： Nitrobenzene p-Aminophenol Pt-Ni/C bimetallic catalyst Electronic effect Pt(5d)-Ni(3d)coupling

Study on Deactivation by Sulfur and Regeneration of Pd/C Catalyst in Hydrogenation of N-（3-nitro-4-methoxyphenyl） Acetamide

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Chinese Journal of Chemical Engineering 2013年第6期21卷 622-626页

作者： ZHANG Qunfeng lu Jinghui MA Lei lu chunshan HIU Wei LI Xiaonian Industrial Catalysis Institute State Key Laboratory Breechng Base ot t.lreen tglaemastry Synthesis lecnnologyZhejiang University of Technology Hangzhou 310032 China

Deactivation of Pd/C catalyst often occurs in liquid hydrogenation using industrial materials. For in-stance, the Pd/C catalyst is deactivated severely in the hydrogenation of N-(3-nitro-4-methoxyphenyl) acetamide. In this study, the chemisorption of sulfur on the surface of deactivated Pd/C was detected by energy dispersive spec-trometer and X-ray photoelectron spectroscopy. Sulfur compounds poison the Pd/C catalyst and increase the forma-tion of azo deposit, reducing the activity of catalyst. We report a mild method to regenerate the Pd/C catalyst: wash the deposit by N,N-dimethylformamide and oxidize the chemisorbed sulfur by hot air. The regenerated Pd/C cata-lyst can be reused at least ten runs with stable activity.

关键词：催化剂失活甲氧基苯基硫化合物再生方法乙酰胺 Pd 硝基 X-射线光电子能谱

High halogenated nitrobenzene hydrogenation selectivity over nano Ir particles

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Chinese Journal of Chemical Engineering 2017年第3期25卷 306-312页

作者： Lei Ma Jianguo Wang Hanbing Wang Qunfeng Zhang chunshan lu Xiaobo He Xiaonian Li Industrial Catalysis Institute of Zhejiang University of Technology State Key Laboratory Breeding Base of Green Chemistry Synthesis TechnologyHangzhou 310032China

The selective hydrogenation of halogenated nitrobenzene over noble metal catalysts(Pd, Pt, and Ir) has attracted much attention owing to its high efficiency and environmental friendliness. However, the effect of size on the catalytic performance varies among different metal catalysts. In this study, sub-nano(<3 nm) Ir and Pd particles were prepared, and their catalytic properties for hydrogenation of halogenated nitrobenzene were *** show that high selectivity(N 99%) was achieved over small Ir nanoparticles, in which the selectivity over the Pd with same size was much lower than that on Ir nanoparticles. Meanwhile, Ir and Pd have different hydrogen consumption rates and reaction rates. Density functional theory calculations showed that p-chloronitrobenzene(CNB) has different adsorption properties on Ir and Pd. The distance between oxygen(cholorine) and Ir is much shorter(longer) than that between oxygen and Pd. The reaction barriers of dechlorination of p-CNB and p-chloroaniline over different Ir models are much larger than those on Pd. Especially,lower coordination of Ir leads to larger barriers of dechlorination reaction. These theoretical results explain the difference between Ir and Pd on hydrogenation of halogenated nitrobenzene.

关键词：卤代硝基苯纳米微粒苯加氢卤化贵金属催化剂对氯硝基苯密度泛函理论加氢反应

Experimental investigation on coal pore-fracture variation and fractal characteristics synergistically affected by solvents for improving clean gas extraction

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International Journal of Mining Science and Technology 2024年第3期34卷 413-425页

作者： Feilin Han Sheng Xue chunshan Zheng Zhongwei Chen Guofu Li Bingyou Jiang Key Laboratory of Safe and Effective Coal Mining of Ministry of Education Anhui University of Science and TechnologyHuainan 232001China School of Safety Science and Engineering Anhui University of Science and TechnologyHuainan 232001China School of Mechanical and Mining Engineering University of QueenslandQLD 4072Australia State Key Laboratory of Coal and Coalbed Methane Co-Mining Jincheng 048012China

Chemical solvents instead of pure water being as hydraulic fracturing fluid could effectively increase permeability and improve clean methane extraction ***,pore-fracture variation features of lean coal synergistically affected by solvents have not been fully *** testing,nuclear magnetic resonance analysis,liquid phase mass spectrometry was adopted to comprehensively analyze pore-fracture change characteristics of lean coal treated by combined solvent(NMP and CS_(2)).Meanwhile,quantitative characterization of above changing properties was conducted using geometric fractal *** model between permeability,fractal dimension and porosity were *** indicate that the end face fractures of coal are well developed after CS2and combined solvent treatments,of which,end face box-counting fractal dimensions range from 1.1227 to *** decreases in ultrasonic longitudinal wave velocity of coal affected by NMP,CS_(2)and combined solvent are 2.700%,20.521%,22.454%,*** treatments could lead to increasing amount of both mesopores and *** ratio of fractal dimension Dsis 0.259%–2.159%,while permeability increases ratio of NMR ranges from 0.1904 to ***,combined solvent could dissolve coal polar and non-polar small molecules and expand flow *** could provide reference for solvent selection and parameter optimization of permeability-enhancement technology.

关键词： Clean gas extraction Chemical solvent Experimental investigation Fractal characteristics Pore fracture

A Novel Retrograde AAV Variant for Functional Manipulation of Cortical Projection Neurons in Mice and Monkeys

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Neuroscience Bulletin 2024年第1期40卷 90-102页

作者： Yefei Chen Jingyi Wang Jing Liu Jianbang Lin Yunping Lin Jinyao Nie Qi Yue chunshan Deng Xiaofei Qi Yuantao Li Ji Dai Zhonghua lu Department of Anesthesiology Shenzhen Maternity and Child Healthcare HospitalThe First School of Clinical MedicineSouthern Medical UniversityShenzhen 518027China Shenzhen Technological Research Center for Primate Translational Medicine Shenzhen Key Laboratory for Molecular Biology of Neural DevelopmentShenzhen-Hong Kong Institute of Brain ScienceShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China University of Chinese Academy of Sciences Beijing 100049China CAS Key Laboratory of Brain Connectome and Manipulation the Brain Cognition and Brain Disease InstituteShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China Guangdong Provincial Key Laboratory of Brain Connectome and Behavior the Brain Cognition and Brain Disease InstituteShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China Biomedical Research Institute Hubei University of MedicineShiyan 442000China Faculty of Life and Health Sciences Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China

Retrograde adeno-associated viruses(AAVs)are capable of infecting the axons of projection neurons and serve as a powerful tool for the anatomical and functional characterization of neural ***,few retro-grade AAV capsids have been shown to offer access to cor-tical projection neurons across different species and enable the manipulation of neural function in non-human primates(NHPs).Here,we report the development of a novel retro-grade AAV capsid,AAV-DJ8R,which efficiently labeled cortical projection neurons after local administration into the striatum of mice and *** addition,intrastriatally injected AAV-DJ8R mediated opsin expression in the mouse motor cortex and induced robust behavioral ***,AAV-DJ8R markedly increased motor cortical neuron firing upon optogenetic light stimulation after viral delivery into the macaque *** data demonstrate the usefulness of AAV-DJ8R as an efficient retrograde tracer for cortical projection neurons in rodents and NHPs and indicate its suitability for use in conducting functional interrogations.

关键词： Retrograde AAV Capsid variant Cortical projection neuron Optogenetics Monkey

One pot synthesis of N-ethylaniline from nitrobenzene and ethanol

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Science China Chemistry 2008年第3期51卷 248-256页

作者： LI XiaoNian ZHANG JunHua XIANG YiZhi MA Lei ZHANG QunFeng lu chunshan WANG Hong BAI Ying Resources&Environment Catalysis Institute of Zhejiang University of Technology State Key Laboratory Breeding Base of Green Chemistry Synthesis TechnologyHangzhou 310032China

A novel method for the one pot synthesis of N-alkyl arylamines from nitro aromatic compounds and alcohols is proposed through the combination of the aqueous-phase reforming of alcohol for hydrogen production, the reduction of nitro aromatic compounds for the synthesis of aromatic amine and the N-alkylation of aromatic amine for the production of N-alkyl arylamine over an identical catalyst under the same conditions of temperature and pressure in a single reactor. In this process, hydrogen generated from the aqueous-phase reforming of alcohols was used in-situ for the hydrogenation of nitro aromatic compounds for aromatic amine synthesis, followed by N-alkylation of aromatic amine with alcohols to form the corresponding N-alkyl arylamines at a low partial pressure of hydrogen. For the system composed of nitrobenzene and ethanol, under the conditions of 413 K and PN2 = 1 MPa, the conversion degrees of nitrobenzene and aniline were 100%, the selectivity to N-ethylaniline and N, N-diethylaniline were 85.9% and 0%-4%, respectivity, after reaction for 8 h at the volumetric ratio of nitrobenzene:ethanol:water = 10:60:0. The selectivity for N, N-diethylaniline production is much lower than that through the traditional method. In this process, hydrogen and aromatic amines generated from the aqueous-phase reforming of alcohols and hydrogenation of nitro aromatic compounds, respectively, could be promptly removed from the surface of the catalyst due to the occurrence of in-situ hydrogenation and N-alkylation reactions. Thus, this may be a potential approach to increase the selectivity to N-alkyl arylamine.

关键词： nitrobenzene ethanol one pot N-ethylaniline combination N-alkylation Raney Ni

A resource recycling technique of hydrogen production from the catalytic degradation of organics in wastewater

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Science China Chemistry 2008年第11期51卷 1118-1126页

作者： LI XiaoNian KONG LingNiao XIANG YiZhi JU YaoMing WU XiaoQiong FENG Feng YUAN JunFeng MA Lei lu chunshan ZHANG QunFeng State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology Resources and Environment Catalysis InstituteZhejiang University of TechnologyHangzhou 310032China

A resource recycling technique of hydrogen production from the catalytic degradation of organics in wastewater by aqueous phase reforming (APR) has been proposed. It is worthy of noting that this technique may be a potential way for the purification of refractory and highly toxic organics in water for hydrogen production. Hazardous organics (such as phenol, aniline, nitrobenzene, tetrahydrofuran (THF), toluene, N,N-dimethylformamide (DMF) and cyclohexanol) in water could be completely de-graded into H2 and CO2 with high selectivity over Raney Ni, and Sn-modified Raney Ni (Sn-Raney-Ni) or Pd/C catalyst under mild conditions. The experimental results operated in tubular and autoclave reactors, indicated that the degradation degree of organics and H2 selectivity could reach 100% under the optimal reaction conditions. The Sn-Raney-Ni (Sn/Ni=0.06) and Pd/C catalysts show better catalytic performances than the Raney Ni catalyst for the degradation of organics in water into H2 and CO2 by the aqueous phase reforming process.

关键词： organic wastewater catalytic degradation hydrogen production resource recycling aqueous phase reforming

Influence of Ni-electrodeposited Pretreatment on Galvanized Coatings of Reactive Steels

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Journal of Wuhan University of Technology(Materials Science) 2007年第2期22卷 221-224页

作者：车淳山 College of Materials Science and Engineering South China University of Technology

Four types of steel sheets containing 0.04%, 0.09%, 0. 14% and 0.36% Si, respectively, were electrodeposited with a nickel layer of 3 tam in thickness and then galvanized in molten Zn at 450℃ for various periods of time. The formation and growth of intermetallic compound layers on the surface of the samples were investigated by SEM and EDS. The experimental results show that the method of Ni-electrodeposited pretreatment can distinctively restrain the over-growth of the galvanized coatings of reactive steels and get eligible coatings with a proper thickness, bright appearance and strong adherence. EDS results indicate that a series of Ni-Zn intermetallic compounds γ′, γ and δ, are first formed on the surface of the samples. With a prolonged immersion time, the F2-Fe-Zn-Ni and δ-Fe-Zn are formed accompanied by the gradual disappearance of γ′, γ and δ2 layer. After a longer immersion time, the lumpy ζ- Fe-Zn occurs between δ and liquid Zn and the F-Fe-Zn does between steel substrate and δ. Subsequently, ζ is in the form of a continuous and compact layer. The method of Ni-electrodeposited pretreatment changes the formation of Fe-Zn intermetallic compounds, which delay the growth of lumpy （and promote the growth of compact δ. Consequently, the abnormal growth of reactive steels is eliminated.

关键词： hot-dip galvanizing electrodepositing Ni reactive steel intermetallic compound

Triple the steady-state reaction rate by decorating the In_(2)O_(3)surface with SiO_(x)for CO_(2)hydrogenation

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Journal of Energy Chemistry 2024年第8期95卷 96-105,I0003页

作者： Hao Wang Chun Yang Xiaoyan Yu Mingrui Wang Runze Yang Xiaowa Nie Ben Hang Yin Alex C.K.Yip chunshan Song Guanghui Zhang Xinwen Guo State Key Laboratory of Fine Chemicals Frontier Science Center for Smart MaterialsPSU-DUT Joint Center for Energy ResearchSchool of Chemical EngineeringDalian University of TechnologyDalian 116024LiaoningChina Department of Chemistry the Chinese University of Hong KongHong Kong 999077China Paihau-Robinson Research Institute the MacDiarmid Institute for Advanced Materials and NanotechnologyVictoria University of WellingtonWellington 6012New Zealand Department of Chemical and Process Engineering The University of CanterburyChristchurch 8041New Zealand

Indium oxide(In_(2)O_(3)),as a promising candidate for CO_(2)hydrogenation to C_(1) products,often suffers from sintering and activity decline,closely related to the undesirable structural evolution under reaction *** on the comprehension of the dynamic evolution,this study presents an efficient strategy to alleviate the agglomeration of In_(2)O_(3)nanoparticles by the surface decoration with highly dispersed silica species(SiO_(x)).Various structural characterizations combined with density functional theory calculations demonstrated that the sintering resulted from the over-reduction,while the enhanced stability originated from the anchoring effect of highly stable In-OSi bonds,which hinders the substantial formation of metallic In(In^(0))and the subsequent agglomeration.0.6Si/In_(2)O_(3)exhibited CO_(2)conversion rate of10.0 mmol g^(-1)h^(-1)at steady state vs.3.5 mmol g^(-1)h^(-1)on In_(2)O_(3)in CO_(2)*** steady-state activity was also achieved on Pd-modified *** to the traditional Pd/In_(2)O_(3)catalyst,the methanol production rate of Pd catalyst supported on 0.6Si/In_(2)O_(3)was enhanced by 23%,showing the potential of In_(2)O_(3)modified by SiO_(x)in serving as a platform *** work provides a promising method to design new In_(2)O_(3)-based catalysts with improved activity and stability in CO_(2)hydrogenation.

关键词： CO_(2)hydrogenation In_(2)O_(3)sintering Dynamic structural evolution Surface SiO_(x)modification DFT simulations