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Journal of Energy Chemistry 2020年第2期29卷 79-86页

作者： Yongcheng Ma Guojun Lan Wenzhao Fu Ying Lai Wenfeng Han Haodong Tang Huazhang Liu Ying Li Institute of Industrial Catalysis Zhejiang University of TechnologyChaowang Road 18Hangzhou 310014ZhejiangChina State Key Laboratory of Chemical Engineering East China University of Science and Technology130 Meilong RoadShanghai 200237China

Carbon nanotubes(CNTs) with abundant surface defects are prepared by a liquid oxidation and thermal annealing method. The defective CNTs-D supported Ba–Ru/CNTs-D catalysts exhibit superior catalytic performance in ammonia synthesis with a TOF be increased up to 0.30 s-1, which is 2.5 times of oxidized CNTs-O supported Ba–Ru/CNTs-O catalysts and 5 times of the Ba–Ru/CNTs. The characterizations by CO chemisorption, transmission electron microscope, Raman, and X-ray photoelectron spectroscopy revealed that the uniformly well dispersed Ru NPs can be stabilized on the defective sites of CNTs-D. The great improvement of the catalytic performance and stability of the Ba–Ru/CNTs-D is contributed to the strong interaction between Ru NPs and surface defect of the CNTs.

关键词： Carbon nanotubes Ruthenium catalyst Defective carbon Ammonia synthesis

Recent advances in carbonized non-noble metal–organic frameworks for electrochemical catalyst of oxygen reduction reaction

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Rare Metals 2021年第10期40卷 2657-2689页

作者： Chan Li Dao-Hui Zhao Hua-Li Long Ming Li Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials Ministry-of-Education Key Laboratory for the Synthesis and Application of Organic Functional MoleculesHubei Key Laboratory of Polymer MaterialsCollege of Chemistry and Chemical EngineeringHubei UniversityWuhan 430062China

The non-noble metal oxygen reduction reaction(ORR) catalysts prepared by carbonization of metal–organic framework(MOF) have attracted more and more attentions in the fields of fuel cells and metal-air batteries due to their unique intrinsic advantages such as high catalytic activity, low price, simple synthesis and good adaptability. Different from the study of traditional high active noble metal catalysts, this review systematically summarizes recent developments on non-noble metal(Fe,Co, Cu, Ni, Mn and Mo) ORR catalysts prepared by various MOFs carbonization in different metal centers. The effects of synthesis strategies and pyrolysis conditions on the catalyst properties are discussed. Meanwhile, the key parameters of catalytic performances(including active sites, dispersed state and specific surface area) are discussed and the prospect is presented. It is expected that this review will provide effective guidance for future studies on carbonized non-noble MOFs for ORR electrochemical catalyst.

关键词： Non-noble metal MOF Pyrolysis catalyst ORR

Highly efficient production of 2,5-dihydroxymethylfuran from biomass-derived 5-hydroxymethylfurfural over an amorphous and mesoporous zirconium phosphonate catalyst

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Journal of Energy Chemistry 2019年第10期28卷 82-92页

作者： Lei Hu Ning Li Xiaoli Dai Yuqi Guo Yetao Jiang Aiyong He Jiaxing Xu Jiangsu Key Laboratory for Biomass-Based Energy and Enzyme Technology Jiangsu Collaborative Innovation Center of Regional Modern Agriculture &Environmental Protection School of Chemistry and Chemical Engineering Huaiyin Normal University

The development of high-efficiency and low-cost catalysts is very crucial for the MeerweinPonndorf-Verley (MPV) reduction of biomass-derived 5-hydroxymethylfurfural (HMF) into 2,5-dihydroxymethylfuran (DHMF). In this work, an amorphous and mesoporous zirconium phosphonate catalyst (Zr-DTMP), which is a zirconium-containing organic-inorganic nanohybrid, was successfully designed and synthesized by the simple assembly of zirconium tetrachloride (ZrCl4) and diethylene triaminepenta(methylene phosphonic acid)(DTMP). Satisfactorily, when Zr-DTMP was employed for the MPV reduction of HMF in the presence of 2-butanol (secBuOH), DHMF yield could be achieved as 96.5% in 3 h under a relatively mild reaction temperature of 140℃. Systematic investigations indicated that this high catalytic activity should be mainly due to the cooperative role of enhancive Lewis acid site (Zr4+) and Lewis base site (O2-) in activating the carbonyl group of HMF and dissociating the hydroxyl group of secBuOH, respectively. Additionally, Zr-DTMP showed excellent catalytic stability, when it was successively used 5 recycles, its surface characteristics and textural properties still remained almost unchanged, and so, the catalytic activity was not obviously affected. More interestingly, Zr-DTMP could also be applied for the selective reduction of other biomass-derived carbonyl compounds, such as 5-methylfurfural (MF), furfural (FF), levulinic acid (LA), ethyl levulinate (EL) and cyclohexanone (CHN), into the corresponding products with high yields, which is beneficial to the effective synthesis of various valuable bio-based chemicals.

关键词： 5-Hydroxymethylfurfural 2,5-Dihydroxymethylfuran 2-Butanol Zirconium phosphonate catalyst Meerwein-Ponndorf-Verley reduction

Partial Oxidation of Methane with Sol-Gel Fe/Hf/YSZ catalyst in Dielectric Barrier Discharge: catalyst Activation by Plasma

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Journal of Rare Earths 2006年第5期24卷 513-518页

作者： Antonius Indarto Jae-Wook Choi Hwaung Lee Hyung Keun Song Jelliarko Palgunadi Clean Technology Research Center Korea Institute of Science and Technology KoreaDepartment of Chemical and Biological Engineering Korea University Korea Clean Technology Research Center Korea Institute of Science and Technology Korea Hydrogen Energy Research Center Korea Institute of Science and Technology Korea

A 1% Fe-30% Hf over yttria-stabilized zirconia catalyst in combination with novel plasma-assisted activation techniques for a direct partial oxidation of methane to methanol was tested using dielectric barrier discharge plasma at ambient temperature and atmospheric pressure. However, instead of methanol, the reaction products were dominated by HE, CO, CO2, C2, and H2O. A catalytically activated plasma process increased the production of methanol compared with a noncatalytic plasma process. The maximum selectivity of methanol production was achieved using a catalyst that was treated at higher applied power.

关键词： methane oxidation dielectric barrier discharge catalyst plasma activation rare earths

Synthesis,optimization and characterization of biochar based catalyst from sawdust for simultaneous esterification and transesterification

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Chinese Journal of Chemical Engineering 2018年第12期26卷 2654-2663页

作者： Suchith Chellappan Vaishakh Nair Sajith V. Aparna K. Department of Chemical Engineering National Institute of TechnologyCalicut India Institute of Physical Chemistry Polish Academy of Sciences School of Nano Science and Technology National Institute of Technology

The development of a benign environmental catalyst for the generation of biodiesel is an area of importance to reduce the overall usage of fossil fuels. In the current work, biochar was produced by slow pyrolysis of Irul wood sawdust. The optimization for biochar generation was carried out for different reaction temperatures and heating durations. The biochar was used to prepare solid acid catalysts by sulfonation process. The characterization of biochar and the sulfonated catalyst were carried out using Elemental analysis, Fourier Transform Infrared spectroscopy(FTIR), Powder X-ray Diffraction(XRD), Thermo Gravimetric Analysis(TGA), Scanning Electron Microscopy(SEM) and Surface area analyzer(BET). The characterization results showed that sulfonation of biochar resulted in biochar based solid acid catalyst containing various functional acidic groups like weak acidic\\OH groups, strong acidic\\COOH and SO3 H groups. The total acid density and sulfonic acid group density of catalyst were estimated and showed excellent acidic sites concentration which gives a good catalytic activity for biodiesel production through simultaneous esterification and transesterification. The enhanced catalytic activity is due to the high acid density of SO3 H groups and the reactant accessibility towards acidic sites as well as the strong affinity between the hydrophilic reactants and the neutral OH groups which are bonded with the polycyclic aromatic carbon rings. The performance of biochar catalyst for the production of biodiesel was evaluated by comparing the yield obtained. The FTIR and Gas Chromatography–Mass Spectroscopy(GC–MS) were also carried out for the analysis of biodiesel produced.

关键词： Biochar Biochar based catalyst Pyrolysis Biomass Sulfonation

Influence of Different Subsistence States of CeO_2^-ZrO_2 Mixed Oxides in catalyst Coating on Catalytic Properties

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Journal of Rare Earths 2006年第1期24卷 54-59页

作者：陈建军冯长根舒柏崇樊俊 School of Mechanic-Electronic Engineering Beijing Institute of Technology Beijing 100081 China School of Mechanic-Electronic Engineering Beijing Institute of Technology Beijing 100081 Chin Guilin REEcat Environment Industry Co. Guilin 541004 China Department of Materials Science and Engineering Tsinghua University Beijing 100084 China

The metallic substrate-catalysts with different subsistence states of CeO2-ZrO2 mixed oxides were prepared and the catalytic properties were investigated. The studies on CeO2-ZrO2-V2O5-CuO mixed oxides which were prepared by coprecipitation, show that the doping of V^5＋ and Cu^2＋ in CeO2-ZrO2 mixed oxides can enhance the catalytic activity and thermal stability of coating materials. Moreover, different additives were doped in slurries of γ-Al2O3 to investigate the influence of additives on oxidation activity of catalysts. The mixture of ceria-zirconia, alkali metals and other rare earths acting as additives exhibits promotion effect on oxidation activity by optimizing the distribution of oxygen on the surface and in the bulk of ceria species. This mentioned mixture was mixed with γ-Al2O3 and a newly proposed active component to prepare a new catalyst. Afterward, the influence of thermal treatment on the new catalyst were investigated by calcinations at 500, 650, 750, 800, 850 and 900 ℃ for 2 h. The light-off curves of CO and HC show that after being treated at 650 - 750 ℃, catalysts present the best activity. XRD patterns show that ceria and zirconia species in the newly proposed active component form a phase of extra CeO2-ZrO2 mixed oxides on the surface of catalysts after the thermal treatment at 750 ℃, which has practical value for improving the preparation process and promoting the catalytic properties. Moreover, XPS resuits imply the existence of Ce1-xPdxO2-σ and Ce1- xPtxO2-σ on the surface of these treated samples, which may show influence on the catalytic activities.

关键词： catalyst metallic substrate ceria-zirconia dopant subsistent form coating technology rare earths

Cathode catalyst prepared from bacterial cellulose for ethanol fermentation stillage treatment in microbial fuel cell

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Chinese Journal of Chemical Engineering 2021年第12期34卷 256-261页

作者： Huiyu Li Ming Gao Pan Wang Hongzhi Ma Ting Liu Jin Ni Qunhui Wang Tien-Chin Chang Department of Environmental Engineering University of Science and Technology BeijingBeijing Key Laboratory of Resource-oriented Treatment of Industrial PollutantsBeijing 100083China Key Laboratory of Cleaner Production and Integrated Resource Utilization of China National Light Industry Beijing Technology and Business UniversityBeijing 100048China Institute of Environmental Engineering and Management National Taipei University of TechnologyTaipei 106China

Bacterial cellulose doped with P and Cu was used as a catalyst for a microbial fuel cell(MFC) cathode,which was then used to treat ethanol fermentation stillage from food *** output power,coulombic efficiency(CE),and biological toxicity were *** a series of characterization experiments,the addition of the cathode catalyst was found to improve catalytic activity and accelerate the consumption of the *** resulting maximum output power was 572.16 mW·m^(-2).CE and the removal rate of chemical oxygen demand(COD) in the fermentation stillage by P-Cu-BC reached 26% and 64.5%,*** rate of biotoxicity removal by MFC treatment reached 84.7%.The aim of this study was apply a novel catalyst for MFC and optimize the treatment efficiency of fermentation stillage.

关键词： Microbial fuel cell Oxygen reduction reaction Fermentation catalyst Biomass Biotoxicity

Selective hydrogenolysis of 5-hydroxymethylfurfural to 2,5-dimethylfuran over Co_3O_4 catalyst by controlled reduction

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Journal of Energy Chemistry 2019年第3期28卷 34-41页

作者： Dan Li Qiying Liu Changhui Zhu Haiyong Wang Chunhua Cui Chenguang Wang Longlong Ma Nano Science and Technology Institute University of Science and Technology of China Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development CAS Key Laboratory of Renewable Energy Guangzhou Institute of Energy Conversion Chinese Academy of Sciences University of Chinese Academy of Sciences

2,5-dimethyfuran(DMF), which is produced from 5-hydroxymethyfurfural(HMF) by hydrodeoxygenation(HDO), is a high quality fuel due to the high heating value, the high octane number and the suitable boiling point. Selective hydrogenation of HMF into liquid fuel DMF has been widely researched. In this paper, Co_3O_4 catalyst was prepared by co-precipitation and was reduced at different temperatures to form Co–CoO_x catalysts. The characterization of catalysts was tested by XRD, TEM, XPS, TPR, BET and ***–CoO_x possessed a high amount of Co metal and CoO_x acidic sites, wherein Co worked as the active hydrogenation sites and CoO_x acted as the acid promoter to facilitate the selective HDO of HMF to *** synergistic effect of Co–CoO_x is the key for HDO of HMF, obtaining 83.3% of DMF yield at 170 °C, 12 h and the reduction temperature of 400 °C. This method not only saves the catalyst cost, but also promotes the utilization of biomass energy.

关键词： HMF DMF Co3O4 catalyst Hydrogenolysis

Ultralow platinum-loading PtPdRu@PtRuIr/C catalyst with excellent CO tolerance and high performance for the methanol oxidation reaction

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Rare Metals 2014年第3期33卷 337-342页

作者： Yan-Ni Wu Shi-Jun Liao Hai-Fu Guo Xiang-Ying Hao Zhen-Xing Liang School of Chemistry and Chemical Engineering Zhaoqing University School of Chemistry and Chemical Engineering South China University of Technology

Carbon-supported PtPdRuIr, Pd@PtRuIr, PtPd@PtRuIr, and PtPdRu@PtRuIr catalysts were prepared by a colloidal method and their catalytic activities to the methanol oxidation reaction in the acidic media were extensively investigated at room temperature. The catalysts were characterized by transmission electron microscopy and X-ray diffraction techniques, and their electrochemical behavior was evaluated by the cyclic voltammetry. The PtPdRu@PtRuIr/C catalyst is found to yield much higher electrocatalytic activity than the other ones and the commercial catalyst. For example, the Pt metal mass-specific activity of this PtPdRu@PtRuIr/C（Pt content 10 wt%,1.7 mAácm-2ámg-1） electrocatalyst is ＊3-fold higher than that of the commercial JM 40 % Pt/C（0.6 mAácm-2ámg-1）electrocatalysts, and the If/Ib ratio of PtPdRu@PtRuIr/C is1.6, which is higher than that of the JM 40 % Pt/C（0.9）. The improvement may result from the high dispersion of the active metal catalyst and the synergistic effect between the PtRuIr and PtPdRu layers. It is thus concluded that the pseudo-core-shell structure could significantly improve the methanol electro-oxidation activity and CO tolerance of the electrocatalyst.

关键词： catalyst Colloidal approach Methanoloxidation PtPdRu@PtRuIr/C

Dehydrogenation of isobutane to isobutene over a Pt-Cu bimetallic catalyst in the presence of LaAlO_(3) perovskite

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Chinese Journal of Chemical Engineering 2021年第4期34卷 203-211页

作者： Yanyong Li Meng Ge Jiameng Wang Mengquan Guo Fanji Liu Mingxun Han Yanhong Xu Lihong Zhang Department of Catalysis Science and Technology Tianjin Key Laboratory of Applied Catalysis Science&TechnologySchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Department of Materials Engineering Xuzhou College of Industrial TechnologyXuzhou 221140China

In this study,isobutane dehydrogenation to isobutene reaction was carried out in a series of PtCu bimetallic catalysts prepared by coimpregnation *** catalysts were characterized by means of several techniques,including XRD,N_(2) adsorptiondesorption,TEM,XPS,H2TPR and *** results show that the existence of LaAlO_(3) perovskite can enhance the dispersion and sintering resistance of metal nanoparticles and facilitate the transfer of carbon deposits from active sites to the ***,the perovskite nanoparticles can also inhibit the reduction of CuOx and the formation of PtCu alloys,resulting in the suitable interaction between Pt and *** PtCu/LaAlO_(3)/SiO_(2)catalyst exhibits the optimal dehydrogenation performance with an isobutane conversion of 47%and isobutene selectivity of 92%after 310 min reaction,which was ascribed to the unique role of LaAlO_(3) perovskite as well as the appropriate PtCu interaction.

关键词： Isobutane dehydrogenation catalyst Nanoparticles Silica LaAlO_(3)perovskite Pt-Cu interaction