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Chemical Research in Chinese Universities 2018年第6期34卷 1004-1008页

作者： TANG Haodong XIANG Meng XU Bin LI Ying HAN Wenfeng LIU Zongjian Institute of Industrial Catalysis College of Chemical Engineering Zhej'iang University of Technology Hangzhou 300014 P. R. China

Although the hard template method is often employed to prepare N-doped mesoporous carbon（N-MC）, tile removal of the silica template commonly involves the use of highly toxic HF or repeated treatment with NaOH solution. Herein, we reported a polyvinylidene fluoride-assisted one-step method for synthesis of N-MC, namely the silica-free N-MC can be prepared via temperature-programmed thermal treatment of a slurry obtained by dispersing nano-silica into a solution containing sucrose, urea, oxalic acid, polyvinylidene fluoride and dimethylacetamide. The resulting N-MC, which owns 3.47%（mass fraction） nitrogen and a surface area of 929 m^2/g, is a highly suitable support of pd catalyst used in hydrodechlorination of 2,4-dichlorophenol, with its performance being much better than those of MC and activated carbon. The excellent catalytic hydrodeehlorination activity of the pd/N-MC catalyst can be attributed to its strong metal-support interaction, which results in a good pd dispersion and high resistance to the growth of nanosized pd under reaction conditions.

关键词： 2,4-Dichlorophenol Hydrodechlorination N-Doped mesoporous carbon Polyvinylidene fluoride pd catalyst

FeOx Coating on pd/C catalyst by Atomic Layer Deposition Enhances the Catalytic Activity in Dehydrogenation of Formic Acid

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Chinese Journal of Chemical Physics 2017年第3期30卷 319-324,I0002页

作者：李俊杰路军岭中国科学技术大学化学物理系合肥微尺度国家科学实验室能源材料化学协同创新中心中国科学院能量转换材料重点实验室合肥230026

Hydrogen generation from formic acid （FA） has received significant attention. The challenge is to obtain a highly active catalyst under mild conditions for practical applications. Here atomic layer deposition （ALD） of FeOx was performed to deposit an ultrathin oxide coating layer to a pd/C catalyst, therein the FeOx coverage was precisely controlled by ALD cycles. Transmission electron microscopy and powder X-ray diffraction measurements suggest that the FeOx coating layer improved the thermal stability of pd nanoparticles （NPs）. X-ray photoelectron spectroscopy measurement showed that deposition of FeOx on the pd NPs caused a positive shift of pd3d binding energy. In the FA dehydrogenation reaction, the ultrathin FeOx layer on the pd/C could considerably improve the catalytic activity, and pd/C coated with 8 cycles of FeOx showed an optimized activity with turnover frequency being about 2 times higher than the uncoated one. shape as a function of the number of FeOx ALD The improved activities were in a volcanocycles, indicating the coverage of FeOx is critical for the optimized activity. In summary, simultaneous improvements of activity and thermal stability of pd/C catalyst by ultra-thin FeOx overlayer suggest to be an effective way to design active catalysts for the FA dehydrogenation reaction.

关键词： Formic acid Hydrogen generation Atomic layer deposition FeOx coating pd catalyst

A comparison of the catalytic hydrogenation of 2-amylanthraquinone and 2-ethylanthraquinone over a pd/Al2O3 catalyst

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Frontiers of Chemical Science and Engineering 2017年第2期11卷 177-184页

作者： Enxian Yuan Xiangwei Ren Li Wang Wentao Zhao Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and Technology Tianjin University Tianjin 300072 China Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Tianjin 300072 China School of Science Tianjin University Tianjin 300072 China

The hydrogenation of 2-ethylanthraquinone （eAQ）, 2-tert-amylanthraquinone （taAQ） and their mixtures with molar ratios of 1：1 and 1：2 to the corresponding hydroquinones （eAQH2 and taAQH2） were studied over a pd/Al2O3 catalyst in a semi-batch slurry reactor at 60 ℃ and at 0.3 MPa. Compared to eAQ, TaAQ exhibited a significantly slower hydrogenation rate （about half） but had a higher maximum yield of H2O2 and a smaller amount of degradation products. This can be ascribed to the longer and branched side chain in taAQ, which limits its accessibility to the pd surface and its diffusion through the pores of the catalyst. Density functional theory calculations showed that it is more difficult for taAQ to adsorb onto a pd （111） surface than for eAQ. The hydrogenation of the eAQ/taAQ mixtures had the slowest rates, lowest H2O2 yields and the highest amounts of degradation products.

关键词： hydrogenation hydrogen peroxide anthraquinone pd catalyst AO process

Enhancing both selectivity and coking-resistance of a single-atom pd1/C3N4 catalyst for acetylene hydrogenation

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Nano Research 2017年第4期10卷 1302-1312页

作者： Xiaohui Huang Yujia Xia Yuanjie Cao Xusheng Zheng Haibin Pan Junfa Zhu Chao Ma Hengwei Wang Junjie Li Rui You Shiqiang Wei Weixin Huang Junling Lu Department of Chemical Physics iChEM CAS Key Laboratory of Materials for Energy Conversion University of Science and Technology of China Hefei 230026 China National Synchrotron Radiation Laboratory University of Science and Technology of China Hefei 230029 China Hefei National Laboratory for Physical Sciences at the Microscale University of Science and Technology of China Hefei 230026 China

Selective hydrogenation is an important industrial catalytic process in chemical upgrading, where pd-based catalysts are widely used because of their high hydrogenation activities. However, poor selectivity and short catalyst lifetime because of heavy coke formation have been major concerns. In this work, atomically dispersed pd atoms were successfully synthesized on graphitic carbon nitride （g-C3N4） using atomic layer deposition. Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy （HAADF-STEM） confirmed the dominant presence of isolated pd atoms without pd nanoparticle （NP） formation. During selective hydrogenation of acetylene in excess ethylene, the g-C3N4-supported pd NP catalysts had strikingly higher ethylene selectivities than the conventional pd/Al2O3 and pd/SiO2 catalysts. In-situ X-ray photoemission spectroscopy revealed that the considerable charge transfer from the pd NPs to g-C3N4 likely plays an important role in the catalytic performance enhancement. More impressively, the single-atom pd1/C3N4 catalyst exhibited both higher ethylene selectivity and higher coking resistance. Our work demonstrates that the single-atom pd catalyst is a promising candidate for improving both selectivity and coking-resistance in hydrogenation reactions.

关键词： single-atom catalyst pd catalyst atomic layer deposition acetylene hydrogenation C3N4 selectivity coke formation support effect

A sulfur-tolerant pd/CeO_2 catalyst for methanol synthesis from syngas

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Journal of Natural Gas Chemistry 2008年第4期17卷 387-390页

作者： Yuchun Ma Qingjie Ge Wenzhao Li Hengyong Xu Laboratory of Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 Liaoning China

The catalytic activity of ceria-supported pd for selective hydrogenation of CO is well preserved in the presence of 30 ppm H2S due to the parallel oxidation of sulfur by CeO2 under standard methanol synthesis conditions. The bifunctional nature of this catalyst opens a route for the conversion of sulfur-contaminated gas streams such as the integrated gasification combined cycle syngas or biogas into liquid fuels if desulfurization by conventional means is not practical.

关键词： sulfur-tolerant catalysis pd catalyst methanol synthesis

Agglomerated pd catalysts and Their Applications in Hydrogen Production from Formic Acid Decomposition at Room Temperature

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Chemical Research in Chinese Universities 2016年第2期32卷 272-277页

作者： LIU Jun LAN Lixin WU Chao LI Rong LIU Xuanyan Department of Pharmaceutical and Biological Engineering Hunan Chemical Vocational Technology College Zhuzhou 412004 P. R. China

Agglomerated pd catalysts with the nano-porous structure were simply prepared by one-step reduction reaction without using any stabilizer. The pd catalysts show a high catalytic activity for the decomposition of formic acid at room temperature. Among all the pd catalysts tested, the pdug catalyst exhibits the highest catalytic activity. Moreover, the breakthrough of the advanced catalysts is that the above agglomerated pd catalysts can be easily separated from the liquid system to control the catalytic reaction at any time, which may further promote the practical application of formic acid as a H2 storage material.

关键词： Hydrogen energy Heterogeneous catalyst Formic acid decomposition pd catalyst Nano-porous structure

Effect of reduction method on the performance of pd catalysts supported on activated carbon for the selective oxidation of glucose

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Science China Chemistry 2010年第7期53卷 1598-1602页

作者： CHEN KangCheng PAN YunXiang LIU ChangJun Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical EngineeringTianjin UniversityTianjin 300072China Shanghai Research Institute of Petrochemical Technology Shanghai 201208China

The effect of the reduction method on the catalytic properties of palladium catalysts supported on activated carbon for the oxidation of D-glucose was *** reduction methods investigated include argon glow discharge plasma reduction at room temperature,reduction by flowing hydrogen at elevated temperature,and reduction by formaldehyde at room *** plasma-reduced catalyst shows the smallest metal particles with a narrow size distribution that leads to a much higher *** catalyst characteristics show that the plasma reduction increases the amount of oxygen-containing functional groups,which significantly enhances the hydrophilic property of the activated carbon and improves the dispersion of the metal.

关键词： reduction method plasma oxidation of glucose pd catalyst activated carbon

Surface interaction between pd and nitrogen derived from hyperbranched polyamide towards highly effective formic acid dehydrogenation

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Journal of Energy Chemistry 2020年第1期29卷 212-216,I0008页

作者： Yancun Yu Xian Wang Changpeng Liu Fateev Vladimir Junjie Ge Wei Xing Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina University of Chinese Academy of Sciences Beijing 100049China Jilin Province Key Laboratory of Low Carbon Chemical Power Sources Changchun 130022JilinChina State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina University of Science and Technology of China(USTC) Hefei 230026AnhuiChina National Research Center Kurchatov Institute Kurchatov sq.1MoscowRussia Laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchaun 130022Jilin.China

Hydrogen production from formic acid decomposition(FAD)is a promising means of hydrogen energy storage and utilization in fuel *** of efficient catalysts for dehydrogenation of formic acid is a challenging *** surface chemical and electronic structure of the active catalysis components is important in formic acid decomposition at ***,the pyrdinic-nitrogen doped catalysts from hyperbranched polyamide were prepared via in situ polymerization reaction process by using activated carbon as a *** of the introduction of the polymer,the particles of the catalysts were stabilized,and the average particle diameter was only 1.64 *** mild conditions,the catalysts activities were evaluated for *** optimized pd-N30/C catalyst exhibited high performance achieving almost full conversion,with a turnover frequency of 3481 h^-1 at 30℃.

关键词： Formic acid decomposition Hydrogen generation Hyperbranched polymer pd catalyst

Enhancing alkyne semi-hydrogenation through engineering metal-support interactions of pd on oxides

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Nano Research 2024年第5期17卷 3707-3713页

作者： Yuefeng Wu Xiaotong Lu Pengfei Cui Wenyu Jia Jun Zhou Yuan Wang Hussain Zahid Yuxin Wu Muhammad Umer Rafique Xiong Yin Baoshan Li Leyu Wang Guolei Xiang State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China College of Chemical Engineering Beijing University of Chemical TechnologyBeijing 100029China

Supported pd catalysts show superior activities for olefin productions from alkynes through semi-hydrogenation reactions,but over-hydrogenation into alkanes highly decreases olefin *** phenylacetylene semi-hydrogenation as a model reaction,here we explore the optimization approaches toward better pd catalysts for alkyne semi-hydrogenation through investigating support effect and metal-support *** results show that the states of pd with supports can be tuned by varying oxide reducibility,loading ratios,and *** our system,0.06 wt.%pd on rutile-TiO_(2) nanorods shows the highest activity owing to the synergistic effects of single-atoms and *** reducibility can change the filling degrees of pd 4d orbitals through varying interfacial bonding strengths,which further affect catalytic activity and selectivity.

关键词： alkyne semi-hydrogenation support effect metal-support interaction pd catalyst single-atom catalyst

Effects of water on CO catalytic oxidation over pd/CeO2

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Journal of Rare Earths 2020年第8期38卷 891-898,I0003页

作者： Shaofei Song Cheng Zhang Yake Lou Yujin Wu Li Wang Yanglong Guo Wangcheng Zhan Yun Guo Key Lab for Advanced Material Laboratory for Research Institute of Industrial CatalysisSchool of Chemistry&Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

The role of water in CO oxidation was investigated on pd/CeO2 with different morphologies(rods(R),cubes(C)and octahedrons(O)).Compared with the absence of water,CO oxidation activity increases 2 times in the presence of water on pd/CeO2-C;but a decrease is found on pd/*** characterization reveals that pd is mainly in the form of solid solution(pdxCe1-xO2-σ)on pd/CeO2-R and a mixture of metal and pdxCe1-xO2-σsolid solution on pd/*** strong interaction between pd and CeO2-R results in the form of stable bidentate carbonates species;while the relatively weak interaction between pd and CeO2-C leads to the produce of unstable monodentate carbonates *** effects of water on CO oxidation activity closely relate with the pd chemical state and the types of carbonates *** restrains CO adsorption on pdxCe1-xO2-σsolid solution,but it has negligent effects on metallic pd *** the presence of water,bidentate carbonates species remains stable but the decrease in the amount of monodentate carbonates species is observed.

关键词： CO oxidation pd catalyst Support morphology Water Rare earths