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Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1206-1216 doi: 10.1007/s11705-020-2017-7

摘要： In this work, the detailed oxygen reduction reaction (ORR) catalytic performance of M-N O (M= Fe, Co, and Ni; = 1–4) has been explored via the detailed density functional theory method. The results suggest that the formation energy of M-N O shows a good linear relationship with the number of doped O atoms. The adsorption manner of O on M-N O changed from end-on ( = 1 and 2) to side-on ( = 3 and 4), and the adsorption strength gradually increased. Based on the results for binding strength of ORR intermediates and the Gibbs free energy of ORR steps on the studied catalysts, we screened out two highly active ORR catalysts, namely Co-N O and Ni-N O , which possess very small overpotentials of 0.27 and 0.32 V, respectively. Such activities are higher than the precious Pt catalyst. Electronic structure analysis reveals one of the reasons for the higher activity of Co-N O and Ni-N O is that they have small energy gaps and moderate highest occupied molecular orbital energy levels. Furthermore, the results of the density of states reveal that the O doping can improve the electronic structure of the original catalyst to tune the adsorption of the ORR intermediates.

关键词： M-N-C catalyst     oxygen doping     oxygen reduction reaction     catalytic activity     density functional theory    

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Effect of K and Ca on catalytic activity of Mn-CeO

Boxiong SHEN, Lidan DENG, Jianhong CHEN

《环境科学与工程前沿（英文）》 2013年 第7卷 第4期   页码 512-517 doi: 10.1007/s11783-013-0519-y

摘要： Mn-CeO /Ti-pillared clay (PILC) is an attractive catalyst for selective catalytic reduction of NO at low temperature because of its low cost. The poisoning of K and Ca on the catalyst of Mn-CeO /Ti-PILC is an important problem because K and Ca are always in presence in flue gas. To investigate the effect of K and Ca on the physicochemical characters of the catalysts, the techniques of NH -temperature programmed desorption (TPD), H -temperature programmed reduction (TPR), and X-ray photoelectron spectroscopy (XPS) were used to analyze the fresh and deactivated catalysts of Mn-CeO /Ti-PILC. (Ca)Mn-CeO /Ti-PILC and (K)Mn-CeO /Ti-PILC are denoted for the dopes of the catalyst of Mn-CeO /Ti-PILC with Ca and K, respectively. The activities of Mn-CeO /Ti-PILC, (Ca)Mn-CeO /Ti-PILC and (K)Mn-CeO /Ti-PILC for NH -selective catalytic reduction (SCR) reaction at low temperature were investigated. The results showed that with the dopes of K and Ca on the catalysts, the SCR activities of the catalysts decreased greatly, and K exhibited more poisoning effect than Ca. With the dopes of K and Ca, the acidity, the redox property and chemisorbed oxygen on the surfaces of the catalysts were decreased, which resulted in a decreasing in SCR activity.

关键词： Mn-CeOx/Ti-pillared clay (PILC)     low-temperature selective catalytic reduction (SCR)     K and Ca poisoning effect    

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Catalytic activity of cerium-doped Ru/AlO during ozonation of dimethyl phthalate

ZHOU Yunrui, ZHU Wanpeng, CHEN Xun

《环境科学与工程前沿（英文）》 2008年 第2卷 第3期   页码 354-357 doi: 10.1007/s11783-008-0059-z

摘要： In this paper, factors influencing the mineralization of dimethyl phthalate (DMP) during catalytic ozonation with a cerium-doped Ru/AlO catalyst were studied. The catalytic contribution was calculated through the results of a comparison experiment. It showed that doping cerium significantly enhanced catalytic activity. The total organic carbon (TOC) removal over the doped catalyst at 100 min reached 75.1%, 61.3% using Ru/AlO catalyst and only 14.0% using ozone alone. Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto AlO support. Results of experiments on oxidation by ozone alone, adsorption of the catalyst, Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%, which showed the obvious effect of Ru–Ce/AlO on catalytic activity.

关键词： Ru–Ce/AlO     dimethyl phthalate     mineralization     comparison experiment     catalytic ozonation    

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Effect of TiO 2 loading on the activity of V/TiO 2 -Al 2 O 3 in the catalytic oxidehydrogenation of ethylbenzene

Xiaohong LI, Wenying LI,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 142-146 doi: 10.1007/s11705-009-0233-2

摘要： TiO-AlOmixed oxides with different compositions ranging from 40wt-% to 95wt-% of TiO were prepared by sol-gel method and impregnated with different amounts of VO. Supports and catalysts were characterized by X-ray diffraction (XRD), physisorption, temperature preprogrammed reduction (H-TPR), and ammonia temperature programmed desorption (NH-TPD). TiO content in the support had obvious effect on the crystal structure, texture characteristic, acid property, and catalytic activity in dehydrogenation of ethylbenzene (EB) with carbon dioxide. The highest catalytic activity was acquired when the TiO content was 50 wt-%.

关键词： desorption     different     TiO-AlOmixed     physisorption     ethylbenzene    

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Electro-catalytic activity of CeO modified graphite felt for carbamazepine degradation via E-peroxone

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1410-x

摘要：

•CeOx/GF-EP process had the better degradation efficiency than GF-EP process.

关键词： E-peroxone     CeOx     Graphite felt     Carbamazepine     Mineralization    

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Catalytic activity of noble metal nanoparticles toward hydrodechlorination: influence of catalyst electronic

Man ZHANG,Feng HE,Dongye ZHAO

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 888-896 doi: 10.1007/s11783-015-0774-1

摘要： In this study, stabilized Pd, Pt and Au nanoparticles were successfully prepared in aqueous phase using sodium carboxymethyl cellulose (CMC) as a capping agent. These metal nanoparticles were then tested for catalytic hydrodechlorination toward two classes of organochlorinated compounds (vinyl polychlorides including trichloroethylene (TCE), tetrachloroethylene (PCE), and alkyl polychlorides including 1,1,1-trichloroethane (1,1,1-TCA), and 1,1,1,2-tetrachloroethane (1,1,1,2-TeCA)) to determine the rate-limiting steps and to explore the reaction mechanisms. The surface area normalized reaction rate constant, , showed a systematic dependence on the electronic structure (the density of states at the Fermi level) of the metals, suggesting that adsorption of organochlorinated reactants on the metal catalyst surfaces is the rate-limiting step for catalytic hydrodechlorination. Hydrodechlorination rates of 1,1,1-TCA and 1,1,1,2-TeCA agreed with the bond strength of the first (weakest) dissociated C-Cl bond, suggesting that C-Cl bond cleavage, which is the first step for dissociative adsorption of the alkyl polychlorides, controlled the catalytic hydrodechlorination rate. However, hydrodechlorination rates of TCE and PCE correlated with the adsorption energies of their molecular (non-dissociative) adsorption on the noble metals rather than with the first C-Cl bond strength, suggesting that molecular adsorption governs the reaction rate for hydrodechlorination of the vinyl polychlorides.

关键词： catalytic hydrodechlorination     electronic structure     metal nanoparticles     reaction mechanisms    

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The formation and catalytic activity of silver nanoparticles in aqueous polyacrylate solutions

Jie Wang, Jianjia Liu, Xuhong Guo, Liang Yan, Stephen F. Lincoln

《化学科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 432-439 doi: 10.1007/s11705-016-1584-0

摘要： Silver nanoparticles (AgNPs) have been synthesized in the presence of polyacrylate through the reduction of silver nitrate by sodium borohydride in aqueous solution. The AgNO and polyacrylate carboxylate group concentrations were kept constant at 2.0 × 10 and 1.0 × 10 mol?L , respectively, while the ratio of [NaBH ]/[AgNO ] was varied from 1 to 100. The ultra-violet-visible plasmon resonance spectra of these solutions were found to vary with time prior to stabilizing after 27 d, consistent with changes of AgNP size and distribution within the polyacrylate ensemble occurring. These observations, together with transmission electron microscopic results, show this rearrangement to be greatest among the samples at the lower ratios of [NaBH ]/[AgNO ] used in the preparation, whereas those at the higher ratios showed a more even distribution of smaller AgNP. All ten of the AgNP samples, upon a one thousand-fold dilution, catalyze the reduction of 4-nitrophenol to 4-aminophenol in the temperature range 283.2–303.2 K with a substantial induction time being observed at the lower temperatures.

关键词： silver nanoparticles     polyacrylates     catalysis     mechanism     sodium borohydride    

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Catalytic activity of manganese oxide supported on alumina in the synthesis of quinoxalines

Rekha M., H. Kathyayini, N. Nagaraju

《化学科学与工程前沿（英文）》 2013年 第7卷 第4期   页码 415-421 doi: 10.1007/s11705-013-1360-3

摘要： Two catalysts, alumina and manganese oxide supported on alumina, have been prepared by calcination and precipitation-impregnation methods, respectively. The catalysts are characterised by the following techniques: Brunner-Emmett-Teller-N adsorption-desorption for surface area, temperature programmed desorption of NH and -butyl amine back titration methods for surface acidity, powder X-ray diffraction for textural properties, and Fourier transform infrared spectroscopy for the anionic radicals. The catalytic activity has been determined under heterogeneous conditions in the condensation reaction between -phenylenediamine and benzil. The product purity is checked by thin-layer chromatography and melting point. The products are also analysed by LC-MS and H-NMR techniques. The yields of the products have been found to be good and catalysts exhibited excellent recyclability. The effect of changing the reaction parameters such as temperature, reaction time, amount of the catalyst, nature of solvent and molar ratio of reactants on the yield of the product has been studied. The surface acidity of the catalysts plays an important role in activating the reaction.

关键词： alumina     manganese oxide deposited on alumina     quinoxaline synthesis    

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Preparation of Ni/SiO catalyst in ionic liquids for hydrogenation

FAN Qingming, LIU Yingxin, ZHENG Yifan, YAN Wei

《化学科学与工程前沿（英文）》 2008年 第2卷 第1期   页码 63-68 doi: 10.1007/s11705-008-0013-4

摘要： A series of silica supported nickel catalysts were prepared from nickel nitrate and tetraethyl orthosilicate by the sol-gel method with the imidazolium type ionic liquids as solvents. The catalysts were characterized by means of X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS). Their catalytic performances for the selective hydrogenation of cinnamaldehyde to hydrocinnamaldehyde were investigated. The results show that the Ni/SiO catalyst prepared with 1-(2-hydroxyethyl)-3-methyl-imidazole tetrafluoroborate ionic liquid as solvent exhibits the highest catalytic activity for the reaction. Under the optimal conditions of catalyst dosage (based on the mass of cinnamaldehyde used) 10%, reaction pressure 2 MPa, temperature 373 K and reaction time 2 h, the conversion of cinnamaldehyde and the selectivity to hydrocinnamaldehyde can reach 97.6% and 98.8%, respectively.

关键词： dispersive     conversion     catalytic     2-hydroxyethyl     catalytic activity    

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Preparation and catalytic performance of La0.8Sr0.2CoO3 supported on the mullite fiber ceramic

ZENG Lingke, LIU Yanchun, LIU Ping′an, WANG Hui, SHUI Anze, DUAN Bilin

《化学科学与工程前沿（英文）》 2007年 第1卷 第4期   页码 372-376 doi: 10.1007/s11705-007-0067-8

摘要： The perovskite-type LaSrCoO supported on the mullite fiber porous ceramics was prepared by means of the impregnating method, and was then characterized by scanning electron microscopy (SEM) and X-ray diffraction (XRD); thus we can come to the conclusion that the perovskite-type composite oxidant can disperse on the surface of mullite fiber ceramics. The catalytic activity of the LaSrCoO for NO and CO was evaluated. The effect of the doped 0.1 wt-% PdCl on the catalytic activity of the perovskite-type LaSrCoO was also discussed. The results show that the conversion rates of NO and CO respectively reaches 74.5% and 99% at 601°C without doped Pd, and both reach 100% at 350°C with a little doped Pd.

关键词： porous     conversion     catalytic activity     electron microscopy     perovskite-type LaSrCoO    

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Characterization and catalytic activity of soft-templated NiO-CeO

Luciano Atzori, Maria Giorgia Cutrufello, Daniela Meloni, Barbara Onida, Delia Gazzoli, Andrea Ardu, Roberto Monaci, Maria Franca Sini, Elisabetta Rombi

《化学科学与工程前沿（英文）》 2021年 第15卷 第2期   页码 251-268 doi: 10.1007/s11705-020-1951-8

摘要： Nanosized NiO, CeO and NiO-CeO mixed oxides with different Ni/Ce molar ratios were prepared by the soft template method. All the samples were characterized by different techniques as to their chemical composition, structure, morphology and texture. On the catalysts submitted to the same reduction pretreatment adopted for the activity tests the surface basic properties and specific metal surface area were also determined. NiO and CeO nanocrystals of about 4 nm in size were obtained, regardless of the Ni/Ce molar ratio. The Raman and X-ray photoelectron spectroscopy results proved the formation of defective sites at the NiO-CeO interface, where Ni species are in strong interaction with the support. The microcalorimetric and Fourier transform infrared analyses of the reduced samples highlighted that, unlike metallic nickel, CeO is able to effectively adsorb CO , forming carbonates and hydrogen carbonates. After reduction in H at 400 °C for 1 h, the catalytic performance was studied in the CO and CO co-methanation reaction. Catalytic tests were performed at atmospheric pressure and 300 °C, using CO/CO /H molar compositions of 1/1/7 or 1/1/5, and space velocities equal to 72000 or 450000 cm ∙h ∙g . Whereas CO was almost completely hydrogenated in any investigated experimental conditions, CO conversion was strongly affected by both the CO/CO /H ratio and the space velocity. The faster and definitely preferred CO hydrogenation was explained in the light of the different mechanisms of CO and CO methanation. On a selected sample, the influence of the reaction temperature and of a higher number of space velocity values, as well as the stability, were also studied. Provided that the Ni content is optimized, the NiCe system investigated was very promising, being highly active for the CO co-methanation reaction in a wide range of operating conditions and stable (up to 50 h) also when submitted to thermal stress.

关键词： soft template method     NiO-CeO2 catalysts     CO and CO2 co-methanation     synthetic natural gas production    

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Noncovalent immobilization of MnP from on carbon nanotubes

Jiaxi LI , Xianghua WEN ,

《环境科学与工程前沿（英文）》 2009年 第3卷 第3期   页码 294-299 doi: 10.1007/s11783-009-0041-4

摘要： Manganese peroxidases (MnP) from were adsorbed onto multi-walled carbon nanotubes (MWNT). Four different loadings of MnP on MWNTs were investigated, and the maximum enzyme loading of 47.5 µg/mg of MWNTs was obtained in 12 h. The adsorbed MnP showed a catalytic activity of up to 0.1 U/mg of the weight of the system of MnP/MWNTs, with 23% of its original activity retained. The AFM image of the adsorbed enzymes indicated that a layer of MnP covered the surface of the MWNTs and retained its original three-dimensional shape. Amino-based nonspecific interactions may play the dominant role in the adsorption of MnP on MWNTs.

关键词： manganese peroxidases (MnP)     Phanerochaete chrysosporium     carbon nanotubes     immobilization     catalytic activity    

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Isolation of microbe for asymmetric reduction of prochiral aromatic ketone and its reaction characters

YANG Zhonghua, WANG Yu, WANG Guanghui, ZENG Rong, YAO Shanjing

《化学科学与工程前沿（英文）》 2007年 第1卷 第4期   页码 416-420 doi: 10.1007/s11705-007-0076-7

摘要： The favorable microbes for the asymmetric reduction of prochiral aromatic ketones was isolated from soil using acetophenone as the sole carbon source, when the asymmetric reduction of acetophenone (ACP) to chiral ?-phenethyl alcohol (PEA) was chosen as the model reaction. Two microbe strains with excellent catalytic activity were obtained. They were and identified by bacteria identification. The product of the asymmetric reduction of ACP catalyzed by was mainly R-PEA and that by was mainly S-PEA. The yield and enantiomeric excesses (e.e.) could respectively reach 75% and 90% for , and 80% and 70% for , much higher than those catalyzed by baker s yeast.

关键词： excellent catalytic     prochiral aromatic     enantiomeric     -phenethyl     catalytic activity    

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Fabrication of three-dimensional porous La-doped SrTiO3 microspheres with enhanced visible light catalyticactivity for Cr(VI) reduction

Dong Yang, Xiaoyan Zou, Yuanyuan Sun, Zhenwei Tong, Zhongyi Jiang

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 440-449 doi: 10.1007/s11705-018-1700-4

摘要：

In recent years, much effort has been focused on the development of the photocatalysts with high performance under visible light irradiation. In this paper, three-dimensional porous La-doped SrTiO3 (LST) microspheres were prepared by a modified sol–gel method, in which the agarose gel/SrCO3 microsphere and La2O3 were employed as the template and the La resource, respectively. The as-prepared LST microspheres exhibit a porous structure with a diameter of about 10 µm and a surface pore size of about 100 nm. The La element was doped into the crystal lattice of SrTiO3 by the substitution of La3+ for Sr2+. Therefore, the absorption edge of LST samples shifts toward the visible light region, and their photocatalytic activity for the Cr(VI) reduction is enhanced under visible light. Among all LST samples, LST-0.5 (the La3+ doping content is 0.5 wt-%) exhibited the highest visible-light photocatalytic activity, which can reduce 84% Cr(VI) within 100 min. This LST materials may become a promising photocatalyst for the facile treatment of wastewater containing poisonous heavy metal ions.

关键词： SrTiO3     La3+ doping     porous microsphere     visible-light photocatalysis     Cr(VI) reduction    

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Magnetic-porous microspheres with synergistic catalytic activity of small-sized gold nanoparticles and

Kadriye Özlem Hamaloğlu, Ebru Sağ, Çiğdem Kip, Erhan Şenlik, Berna Saraçoğlu Kaya, Ali Tuncel

《化学科学与工程前沿（英文）》 2019年 第13卷 第3期   页码 574-585 doi: 10.1007/s11705-019-1799-y

摘要： Fe O nanoparticles immobilized on porous titania in micron-size range were decorated with small-sized gold nanoparticles and used as a plasmonic catalyst for the reduction of 4-nitrophenol. Monodisperse-porous magnetic titania microspheres were synthesized with bimodal pore-size distribution by the sol-gel templating method. Small-sized gold nanoparticles obtained by the Martin method were attached onto the aminated form of the magnetic titania microspheres. A significant enhancement in the catalytic activity was observed using the gold nanoparticle-decorated magnetic titania microspheres compared to gold nanoparticle-decorated magnetic silica microspheres because of the synergistic effect between small-sized gold nanoparticles and titania. The synergistic effect for gold nanoparticle-attached magnetic titania microspheres could be explained by surface plasmon resonance-induced transfer of hot electrons from gold nanoparticles to the conduction band of titania. Using the proposed catalyst, 4-nitrophenol could be converted to 4-aminophenol in an aqueous solution within 0.5 min. The 4-nitrophenol reduction rates were 2.5–79.3 times higher than those obtained with similar plasmonic catalysts. The selection of micron-size, magnetic, and porous titania microspheres as a support material for the immobilization of small-sized gold nanoparticles provided a recoverable plasmonic catalyst with high reduction ability.

关键词： small-sized gold nanoparticles     magnetic titania microspheres     sol-gel template synthesis     plasmonic catalysis     4-nitrophenol    

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标题 作者 时间 类型 操作

Probing the catalytic activity of M-N

Fan Ge, Qingan Qiao, Xin Chen, You Wu

期刊论文

Effect of K and Ca on catalytic activity of Mn-CeO

Boxiong SHEN, Lidan DENG, Jianhong CHEN

期刊论文

Catalytic activity of cerium-doped Ru/AlO during ozonation of dimethyl phthalate

ZHOU Yunrui, ZHU Wanpeng, CHEN Xun

期刊论文

Effect of TiO 2 loading on the activity of V/TiO 2 -Al 2 O 3 in the catalytic oxidehydrogenation of ethylbenzene

Xiaohong LI, Wenying LI,

期刊论文

Electro-catalytic activity of CeO modified graphite felt for carbamazepine degradation via E-peroxone

期刊论文

Catalytic activity of noble metal nanoparticles toward hydrodechlorination: influence of catalyst electronic

Man ZHANG,Feng HE,Dongye ZHAO

期刊论文

The formation and catalytic activity of silver nanoparticles in aqueous polyacrylate solutions

Jie Wang, Jianjia Liu, Xuhong Guo, Liang Yan, Stephen F. Lincoln

期刊论文

Catalytic activity of manganese oxide supported on alumina in the synthesis of quinoxalines

Rekha M., H. Kathyayini, N. Nagaraju

期刊论文

Preparation of Ni/SiO catalyst in ionic liquids for hydrogenation

FAN Qingming, LIU Yingxin, ZHENG Yifan, YAN Wei

期刊论文

Preparation and catalytic performance of La0.8Sr0.2CoO3 supported on the mullite fiber ceramic

ZENG Lingke, LIU Yanchun, LIU Ping′an, WANG Hui, SHUI Anze, DUAN Bilin

期刊论文

Characterization and catalytic activity of soft-templated NiO-CeO

Luciano Atzori, Maria Giorgia Cutrufello, Daniela Meloni, Barbara Onida, Delia Gazzoli, Andrea Ardu, Roberto Monaci, Maria Franca Sini, Elisabetta Rombi

期刊论文

Noncovalent immobilization of MnP from on carbon nanotubes

Jiaxi LI , Xianghua WEN ,

期刊论文

Isolation of microbe for asymmetric reduction of prochiral aromatic ketone and its reaction characters

YANG Zhonghua, WANG Yu, WANG Guanghui, ZENG Rong, YAO Shanjing

期刊论文

Fabrication of three-dimensional porous La-doped SrTiO3 microspheres with enhanced visible light catalyticactivity for Cr(VI) reduction

Dong Yang, Xiaoyan Zou, Yuanyuan Sun, Zhenwei Tong, Zhongyi Jiang

期刊论文

Magnetic-porous microspheres with synergistic catalytic activity of small-sized gold nanoparticles and

Kadriye Özlem Hamaloğlu, Ebru Sağ, Çiğdem Kip, Erhan Şenlik, Berna Saraçoğlu Kaya, Ali Tuncel

期刊论文