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Hydrogenation of ortho-nitrochlorobenzene on activated carbon supported platinum catalysts 被引量:2
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作者 蒋成君 尹红 陈志荣 《Journal of Zhejiang University-Science B(Biomedicine & Biotechnology)》 SCIE EI CAS CSCD 2005年第5期378-381,共4页
Platinum/carbon catalyst is one of the most important catalysts in hydrogenation of ortho-nitrochlorobenzene to 2,2′-dichlorohydrazobenzene. The preparation process and the supports of catalysts are studied in this p... Platinum/carbon catalyst is one of the most important catalysts in hydrogenation of ortho-nitrochlorobenzene to 2,2′-dichlorohydrazobenzene. The preparation process and the supports of catalysts are studied in this paper. Raw materials and preparation procedure of the activated carbon have great influences on the compositions and surface structure of platinum/carbon catalysts. Platinum catalysts supported on activated carbon with high purity, high surface area, large pore volume and appropriate pore structure usually exhibit higher activities for hydrogenation of ortho-nitrochlorobenzene to 2,2′-dichlorohydrazobenzene. The catalyst prepared from H2PtCl6 with pH=3 shows greater catalytic performance than those prepared under other conditions. 展开更多
关键词 platinum/carbon catalyst HYDROGENATION Ortho-nitrochlorobenzene 2 2′-dichlorohydrazobenzene Activated carbon
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Recent advances in morphology control of platinum catalysts toward oxygen reduction reaction
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作者 Shun CHEN Yanru LIU +1 位作者 Xiaogang FU Wanglei WANG 《Frontiers in Energy》 SCIE EI CSCD 2024年第3期330-355,共26页
Exploring advanced platinum (Pt)-based electrocatalysts is vital for the widespread implementation of proton exchange membrane fuel cells (PEMFCs). Morphology control represents an effective strategy to optimize the b... Exploring advanced platinum (Pt)-based electrocatalysts is vital for the widespread implementation of proton exchange membrane fuel cells (PEMFCs). Morphology control represents an effective strategy to optimize the behavior of Pt catalysts. In this work, an attempt is made to comprehensively review the effect of morphology control on the catalytic behavior of catalysts in the oxygen reduction reaction (ORR). First, the fundamental physicochemical changes behind morphology control, including exposing more active sites, generating appropriate lattice strains, and forming different crystalline surfaces, are highlighted. Then, recently developed strategies for tuning the morphologies of electrocatalysts, including core-shell structures, hollow structures, nanocages, nanowires, and nanosheets, are comprehensively summarized. Finally, an outlook on the future development of morphology control of Pt catalysts is presented, including rational design strategies, advanced in situ characterization techniques, novel artificial intelligence, and mechanical learning. This work is intended to provide valuable insights into designing the morphology and technological innovation of efficient redox electrocatalysts in fuel cells. 展开更多
关键词 MORPHOLOGY platinum catalysts ELECTROCATALYSIS ORR PEMFC
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Hydroisomerization performance of platinum supported on ZSM-22/ZSM-23 intergrowth zeolite catalyst 被引量:9
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作者 Chi Kebin Zhao Zhen +8 位作者 Tian Zhijian Hu Sheng Yan Lijun Li Tianshu Wang Bingchun Meng Xiangbin Gao Shanbin Tan Mingwei Liu Yanfeng 《Petroleum Science》 SCIE CAS CSCD 2013年第2期242-250,共9页
Hydroisomerization catalysts Pt/ZSM-22, Pt/ZSM-23, and Pt/ZSM-22/ZSM-23 were prepared by supporting Pt on ZSM-22, ZSM-23, and intergrowth zeolite ZSM-22/ZSM-23, respectively. The typical physicochemical properties of ... Hydroisomerization catalysts Pt/ZSM-22, Pt/ZSM-23, and Pt/ZSM-22/ZSM-23 were prepared by supporting Pt on ZSM-22, ZSM-23, and intergrowth zeolite ZSM-22/ZSM-23, respectively. The typical physicochemical properties of these catalysts were characterized by X-Ray Diffraction (XRD), N2 absorption-desorption, Pyridine-Fourier Transform Infrared (Py-FTIR), Transmission Electron Microscopy (TEM), X-Ray Fluorescence (XRF), Scanning Electron Microscopy (SEM) and NH3- Temperature Programmed Desorption (NH3-TPD), and the performance of these catalysts in n-dodecane hydroisomerization was evaluated in a continuous down-flow fixed bed with a stainless steel tubular reactor. The characterization results indicated that the intergrowth zeolite ZSM-22/ZSM-23 possessed the dual structure of ZSM-22 and ZSM-23, and the catalyst Pt/ZSM-22/ZSM-23 had similar pores and weak acidity to Pt/ZSM-22 and Pt/ZSM-23 catalysts. Moreover, Pt/ZSM-22/ZSM-23 catalyst showed a high selectivity in hydroisomerization of long chain n-alkanes to mono-branched isomers. The evaluation results for n-dodecane hydroisomerization indicated that the activity of Pt/ZSM-22/ZSM-23 was the lowest, while the hydroisomerization selectivity was the highest among the three catalysts. The maximum yield of i-dodecane product was 68.3% over Pt/ZSM-22/ZSM-23 at 320 ℃. 展开更多
关键词 ZSM-22/ZSM-23 intergrowth zeolite platinum catalyst N-DODECANE HYDROISOMERIZATION
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LaO_(x)(OH)_(y) supported platinum catalysts for CO oxidation:Deactivation by formation of lanthanum carbonate 被引量:3
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作者 Luozhen Jiang Junxiang Chen Rui Si 《Journal of Rare Earths》 SCIE EI CAS CSCD 2021年第3期297-304,I0003,共9页
Platinum catalyst for CO oxidation has been studied for decades,due to its high activity and good stability.In this work,we prepared three different lantha num oxide or hydroxide supports(LaO_(x)(OH)_(y)),and deposite... Platinum catalyst for CO oxidation has been studied for decades,due to its high activity and good stability.In this work,we prepared three different lantha num oxide or hydroxide supports(LaO_(x)(OH)_(y)),and deposited platinum(Pt) with 0.5 at% via an impregnation approach to synthesize Pt/LaO_(x)(OH)_(y) catalysts.However,we find that these catalysts perform a poor stability for the CO oxidation reaction.The fresh and used samples were comprehensively characterized by multiple techniques including power X-ray diffraction(XRD),X-ray absorption fine structure(XAFS),transmission electron microscopy(TEM),temperature-programmed reduction by carbon monoxide(CO-TPR) and thermogravimetric analysis(TGA),to demonstrate that the oxidized platinum atoms or clusters,without any component of Pt-Pt metallic bond,are highly dispersed on the surface of LaO_(x)(OH)_(y).Furthermore,the as-formed lanthanum carbonate(La_(2)O_(2)CO_(3)) during the exposure to ambient circumstances or in the reaction atmosphere of CO+O_(2),severely impair the reactivity of Pt/LaO_(x)(OH)_(y).On the basis of the obtained experimental results,we have drawn a conclusion that the oxidized P_(t)O_(x) atoms or PtxOy clusters are the active species for CO oxidation,while the formation of lanthanum carbonate is the origin of deactivation on reactivity. 展开更多
关键词 platinum catalyst Lanthanum oxide Lanthanum hydroxide CO oxidation Structure-activity relationship Rare earths
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Ceria supported platinum catalyst for CO oxidation reaction:Importance of metallic active species——Commemorating the 100th anniversary of the birth of Academician Guangxian Xu
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作者 Luozhen Jiang Xin Tao +2 位作者 Li'na Li Wen Xia Rui Si 《Journal of Rare Earths》 SCIE EI CAS CSCD 2021年第5期495-503,共9页
Ceria supported platinum catalyst has now been widely studied due to its excellent activity for CO oxidatio n.However,the electron state of active metal center is still an open question.In this work,a ce ria nanorod s... Ceria supported platinum catalyst has now been widely studied due to its excellent activity for CO oxidatio n.However,the electron state of active metal center is still an open question.In this work,a ce ria nanorod support was prepared and platinum(Pt)with 0.9 at%was deposited using an impregnation method to obtain Pt/CeO_(2)catalyst.With the help of"light-off"experiment and temperatureprogrammed reduction under CO(CO-TPR)test,the conclusion is proposed that the process of hydrogen reduction can enhance the activity of CO oxidation reaction for the generation of optimal active Pt site.An innovative near-situ X-ray absorption fine structure(XAFS)technique was used to investigate the chemical state of central Pt atom during the reaction process,clearly demonstrating that the high oxidized state of Pt does harm to the activity for CO oxidation while the relatively reductive Pt exhibits high activity,and the different oxidized state and chemical environment of Pt during every process has been identified.Furthermore,the activity of our Pt/CeO_(2)catalyst is superior to that of most of the previous reports about CO catalytic oxidation by Pt based catalyst.Moreover,the optimal active species(Pt-O_(4))have been identified after hydrogen reduction,which could be a possible key strategy to control the oxidation of Pt. 展开更多
关键词 platinum catalyst Ceria support CO oxidation Structure-activity relationship X-ray absorption fine structure Rare earths
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In situ grown nanoscale platinum on carbon powder as catalyst layer in proton exchange membrane fuel cells(PEMFCs) 被引量:2
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作者 Sheng Sui Xiaolong Zhuo +4 位作者 Kaihua Su Xianyong Yao Junliang Zhang Shangfeng Du Kevin Kendall 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2013年第3期477-483,共7页
An extensive study has been conducted on the proton exchange membrane fuel cells (PEMFCs) with reducing Pt loading. This is commonly achieved by developing methods to increase the utilization of the platinum in the ... An extensive study has been conducted on the proton exchange membrane fuel cells (PEMFCs) with reducing Pt loading. This is commonly achieved by developing methods to increase the utilization of the platinum in the catalyst layer of the electrodes. In this paper, a novel process of the catalyst layers was introduced and investigated. A mixture of carbon powder and Nafion solution was sprayed on the glassy carbon electrode (GCE) to form a thin carbon layer. Then Pt particles were deposited on the surface by reducing hexachloroplatinic (IV) acid hexahydrate with methanoic acid. SEM images showed a continuous Pt gradient profile among the thickness direction of the catalytic layer by the novel method. The Pt nanowires grown are in the size of 3 nm (diameter) x l0 nm (length) by high solution TEM image. The novel catalyst layer was characterized by cyclic voltammetry (CV) and scanning electron microscope (SEM) as compared with commercial Pt/C black and Pt catalyst layer obtained from sputtering. The results showed that the platinum nanoparticles deposited on the carbon powder were highly utilized as they directly faced the gas diffusion layer and offered easy access to reactants (oxygen or hydrogen). 展开更多
关键词 platinum catalyst layer carbon powder layer proton exchange membrane fuel cells
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1, 1'—BIS (BENZYLSELENO) FERROCENE PLATINUM COMPLEX AS HYDROSlLYLATION CATALYST FOR OLEFINS 被引量:1
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作者 Jun Zhi YAO Bing Shou TIAN Yuan Yin CHEN Department of Chemistry, Wuhan University, Wuhan, 430072 《Chinese Chemical Letters》 SCIE CAS CSCD 1993年第7期601-602,共2页
1, 1'--Bis(benzylseleno)ferrocene and its platinum complex were synthesized. It was found that the platinum complex was efficient catalyst for the hydrosilylation of olefins with triethoxysilane.
关键词 BIS BENZYLSELENO FERROCENE platinum COMPLEX AS HYDROSlLYLATION catalyst FOR OLEFINS AS
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Nanostructured ultrathin catalyst layer with ordered platinum nanotube arrays for polymer electrolyte membrane fuel cells 被引量:10
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作者 Ruoyi Deng Zhangxun Xia +2 位作者 Ruili Sun Suli Wang Gongquan Sun 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第4期33-39,共7页
Fabrication of novel electrode architectures with nanostructured ultrathin catalyst layers is an effective strategy to improve catalyst utilization and enhance mass transport for polymer electrolyte membrane fuel cell... Fabrication of novel electrode architectures with nanostructured ultrathin catalyst layers is an effective strategy to improve catalyst utilization and enhance mass transport for polymer electrolyte membrane fuel cells (PEMFCs).Herein,we report the design and construction of a nanostructured ultrathin catalyst layer with ordered Pt nanotube arrays,which were obtained by a hard-template strategy based on ZnO,via hydrothermal synthesis and magnetron sputtering for PEMFC application.Because of the crystallographically preferential growth of Pt (111) facets,which was attributed to the structural effects of ZnO nanoarrays on the Pt nanotubes,the catalyst layers exhibit obviously higher electrochemical activity with remarkable enhancement of specific activity and mass transport compared with the state-of-the-art randomly distributed Pt/C catalyst layer.The PEMFC fabricated with the as-prepared catalyst layer composed of optimized Pt nanotubes with an average diameter of 90(±10) nm shows excellent performance with a peak power density of 6.0W/mgPt at 1 A/cm^2,which is 11.6%greater than that of the conventional Pt/C electrode. 展开更多
关键词 catalyst layer Membrane electrode assembly platinum NANOTUBE arrays Fuel cells
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CROWN FUNCTIONALIZED LINEAR POLYSILOXANE PLATINUM COMPLEX AS HYDROSILYLATION CATALYST
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作者 陈远荫 卢雪然 +1 位作者 龚淑玲 张宝莲 《Chinese Journal of Polymer Science》 SCIE CAS CSCD 1994年第4期352-357,共6页
A modified method of preparing crown functionalized linear polysiloxane has been described.4'-allylbenzo-15-crown-5 was subjected to hydrosilylation with methyldichlorosilane,followed bypolycondensation with silan... A modified method of preparing crown functionalized linear polysiloxane has been described.4'-allylbenzo-15-crown-5 was subjected to hydrosilylation with methyldichlorosilane,followed bypolycondensation with silanol-terminated polydimethylsiloxane to give the title crownfunctionalized linear polysiloxane. It was found that the polysiloxane could be coordinated withplatinum salt to form platinum complex, which could catalyze the hydrosilylation of olefins withtriethoxysilane efficiently. 展开更多
关键词 Functionalized polysiloxane Crown ether platinum complex Hydrosilylation catalyst Polymeric crown ether
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SILICA-BOUND CROWN ETHERS PLATINUM COMPLEX AS HYDROSILYLATION CATALYST
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作者 陈远荫 孟令芝 +2 位作者 李立平 罗介奇 胡缙昌 《Chinese Journal of Polymer Science》 SCIE CAS CSCD 1993年第1期22-25,共4页
Silica-bound 15-Crown-5, 18-Crown-6 with a spacer of propyloxymethyl and their platinum complexes have been synthesized. It was found that they were efficient catalysts for the hydrosilylation of olefms with triethoxy... Silica-bound 15-Crown-5, 18-Crown-6 with a spacer of propyloxymethyl and their platinum complexes have been synthesized. It was found that they were efficient catalysts for the hydrosilylation of olefms with triethoxysilane in the temperature range of 60 to 130 ℃. 展开更多
关键词 Crown ether Supported crown ether platinum complex Hydrosilylation catalyst Supported catalyst.
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4-Selena-7-thiaoctyl Polystyrene-supported Platinum Complex as Hydrosilylation Catalyst
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作者 MENG Ling zhi KE Ai qing and CHEN Yuan yin (Department Chemistry, Wuhan University, Wuhan, 430072) 《Chemical Research in Chinese Universities》 SCIE CAS CSCD 1998年第4期56-59,共4页
IntroductionSelenoetherplatinumcomplexesasanewkindofhydrosilylationcatalysthavebeendrawnmuchatentionrecently... IntroductionSelenoetherplatinumcomplexesasanewkindofhydrosilylationcatalysthavebeendrawnmuchatentionrecently.Aseriesofselenoe... 展开更多
关键词 Polystyrene bound catalyst platinum complex HYDROSILYLATION β methylthioethyl β hydroxyethyl selenoether
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The Effect of Platinum on Stability of the B_2O_3/TiO_2-ZrO_2 Catalyst for Beckmann Rearrangement of Cyclohexanone Oxime
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作者 Dong Sen MAO Guan Zhong LU 《Chinese Chemical Letters》 SCIE CAS CSCD 2006年第8期1025-1028,共4页
The addition of platinum over the B2O3/TiO2-ZrO2 remarkably enhanced its catalytic stability in the vapor phase Beckmann rearrangement of cyclohexanone oxime under the carder gas of H2. The content of coke deposited ... The addition of platinum over the B2O3/TiO2-ZrO2 remarkably enhanced its catalytic stability in the vapor phase Beckmann rearrangement of cyclohexanone oxime under the carder gas of H2. The content of coke deposited on catalyst surface was decreased from 1.92% over the B2O3/TiO2-ZrO2 to 1.14% over the platinum promoted B2O3/TiO2-ZrO2 after reaction of six hours. This result indicates that the platinum added on the B2O3/TiO2-ZrO2 catalyst plays an important role in reducing the coke formation on the catalyst surface. 展开更多
关键词 Cyclohexanone oxime vapor-phase Beckmann rearrangement Ε-CAPROLACTAM B2O3/TiO2-ZrO2 catalyst platinum.
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Pt/Co_3O_4/3DOM Al_2O_3:Highly effective catalysts for toluene combustion 被引量:9
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作者 杨黄根 邓积光 +3 位作者 刘雨溪 谢少华 徐鹏 戴洪兴 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第6期934-946,共13页
Three-dimensionally ordered macro-/mesoporous alumina(3DOM Al2O3)-supported cobalt oxide and platinum nanocatalysts(xPt/yCo3O4/3DOM Al2O3,Pt mass fraction(x%)= 0-1.4%,Co3O4 mass fraction(y%) = 0-9.2%) were pre... Three-dimensionally ordered macro-/mesoporous alumina(3DOM Al2O3)-supported cobalt oxide and platinum nanocatalysts(xPt/yCo3O4/3DOM Al2O3,Pt mass fraction(x%)= 0-1.4%,Co3O4 mass fraction(y%) = 0-9.2%) were prepared using poly(methyl methacrylate) templating,incipient wetness impregnation and polyvinyl alcohol-protected reduction.The resulting xPt/yCo3O4/3DOM Al2O3 samples displayed a high-quality 3DOM architecture with macropores(180-200 nm in diameter) and mesopores(4-6 nm in diameter) together with surface areas in the range of 94 to 102m^2/g.Using these techniques,Co3O4 nanoparticles(NPs,18.3 nm) were loaded on the 3DOM Al2O3 surface,after which Pt NPs(2.3-2.5 nm) were uniformly dispersed on theyCo3O4/3DOM Al2O3.The1.3Pt/8.9Co3O4/3DOM Al2O3 exhibited the best performance for toluene oxidation,with a T(90%) value(the temperature required to achieve 90%toluene conversion) of 160 ℃ at a space velocity of20000 mL g^(-1) h^(-1).It is concluded that the excellent catalytic performance of the 1.3Pt/8.9Co3O4/3DOM Al2O3 is owing to well-dispersed Pt NPs,the high concentration of adsorbed oxygen species,good low-temperature reducibility,and strong interaction between the Pt and Co3O4 NPs,as well as the unique bimodal porous structure of the support. 展开更多
关键词 Three-dimensionally ordered macropore Alumina-supported cobalt oxide catalyst Supported platinum catalyst Toluene combustion
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Pd(111)与Pt(111)上NO氧化的第一性原理研究
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作者 李志军 曹飞 +3 位作者 王学豹 李世龙 张时杰 李振国 《天津大学学报(自然科学与工程技术版)》 EI CAS CSCD 北大核心 2024年第6期588-594,共7页
随着排放法规的日益严格,发动机的氮氧化物(NO_(x))后处理已成为当今研究的重点问题.针对目前可有效降低稀燃汽油机NO_(x)的稀燃氮氧化物捕集器中铂(Pt)和钯(Pd)两种贵金属之间的替换问题,进行了密度泛函理论(density functional theory... 随着排放法规的日益严格,发动机的氮氧化物(NO_(x))后处理已成为当今研究的重点问题.针对目前可有效降低稀燃汽油机NO_(x)的稀燃氮氧化物捕集器中铂(Pt)和钯(Pd)两种贵金属之间的替换问题,进行了密度泛函理论(density functional theory,DFT)计算研究.首先,对一氧化氮(NO)、氧气(O_(2))、二氧化氮(NO_(2))在两种催化剂(111)表面的吸附进行了研究,之后,在两催化剂表面对比研究了氧化过程中涉及的O_(2)解离与NO氧化两反应过程,揭示了NO在Pd与Pt催化剂上的氧化机理.结果显示:3种物质在催化剂表面的吸附强度为NO>O_(2)>NO_(2).氧覆盖度将会改变氮氧化物的最佳吸附构型,随着表面氧原子的增加NO会由三重空位式吸附转变为顶点吸附,NO_(2)会由μ-N,O-亚硝基吸附转变为硝基吸附.在O_(2)解离过程中Pt的催化能力优于Pd,但是两者对NO氧化的催化能力接近.在Pd和Pt表面反应限速步骤都是O_(2)的解离,Pd对O_(2)较弱的解离能力导致了其NO的转化效率低于Pt.氧覆盖度对氧化过程存在影响,通过电子结构分析发现,氧覆盖度的提升使催化剂与吸附物质之间的吸附能下降,这导致了反应由吸热变为放热,使催化可以自发进行.反应生成的NO_(2)需要1.00 eV以上的能量完成脱附,这在原子层面解释了NO_(2)对NO氧化反应的抑制作用. 展开更多
关键词 稀燃氮氧化物捕集器 第一性原理 铂族催化剂 一氧化氮氧化
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铁捕集法从失效铝基催化剂中富集铂的研究
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作者 童伟锋 赵家春 +5 位作者 周廷熙 吴跃东 张纯熙 王亚雄 范云鹏 杨一滨 《贵金属》 CAS 北大核心 2024年第S01期116-119,共4页
进行了从失效铝基丙烷脱氢催化剂中回收铂的研究,采用火法熔炼铁捕集法实现铂的高效富集。重点研究了在熔炼温度为1400℃的条件下,熔炼时间、捕集剂(磁铁矿)用量、造渣剂(CaO、SiO_(2))用量、助熔剂(Na_(2)CO_(3)、硼砂)用量对铂回收率... 进行了从失效铝基丙烷脱氢催化剂中回收铂的研究,采用火法熔炼铁捕集法实现铂的高效富集。重点研究了在熔炼温度为1400℃的条件下,熔炼时间、捕集剂(磁铁矿)用量、造渣剂(CaO、SiO_(2))用量、助熔剂(Na_(2)CO_(3)、硼砂)用量对铂回收率的影响。结果表明,在熔炼温度1400℃,熔炼时间4 h,加入质量为失效催化剂60%的磁铁矿、50%的CaO、35%的SiO_(2)、30%的Na_(2)CO_(3)、60%硼砂的条件下,铂平均回收率为99.31%。 展开更多
关键词 有色金属冶金 丙烷脱氢催化剂 富集 铁捕集法
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High activity of a Pt decorated Ni/C nanocatalyst for hydrogen oxidation 被引量:3
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作者 高孝麟 王昱飞 +2 位作者 谢和平 刘涛 储伟 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第2期396-403,共8页
The Pt decorated Ni/C nanocatalysts were prepared for hydrogen oxidation reaction(HOR) in fuel cell.By regulating the contents of Pt and Ni in the catalyst,both the composition and the structure affected the electro... The Pt decorated Ni/C nanocatalysts were prepared for hydrogen oxidation reaction(HOR) in fuel cell.By regulating the contents of Pt and Ni in the catalyst,both the composition and the structure affected the electrochemical catalytic characteristics of the Pt-Ni/C catalysts.When the Pt mass content was 3.1% percent and that of Ni was 13.9% percent,the Pt-Ni/C-3 catalyst exhibited a larger electrochemically active surface area and a higher exchange current density toward HOR than those of pure supported platinum sample.Our study demonstrates a feasible approach for designing the more efficient catalysts with lower content of noble metal for HOR in fuel cell. 展开更多
关键词 platinum catalyst Galvanic displacement Nickel supported on carbon Hydrogen oxidation reaction Electrochemically active surface
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三维碳纤维基复合材料及其在海水溶解氧电池中的应用性能 被引量:1
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作者 王金涛 段体岗 +3 位作者 郭建章 马力 余聚鑫 张海兵 《材料导报》 EI CAS CSCD 北大核心 2024年第4期214-219,共6页
以三维碳纤维刷为基体通过一步水热还原法制备了石墨烯/铂复合电极(Pt-G/CFB),分析结果表明碳纤维丝束上均匀生长和包覆了大量Pt纳米微粒和石墨烯,Pt晶粒尺寸约3.1 nm;复合电极具有较大比表面积和丰富的介孔结构。Pt-G催化剂在氧还原反... 以三维碳纤维刷为基体通过一步水热还原法制备了石墨烯/铂复合电极(Pt-G/CFB),分析结果表明碳纤维丝束上均匀生长和包覆了大量Pt纳米微粒和石墨烯,Pt晶粒尺寸约3.1 nm;复合电极具有较大比表面积和丰富的介孔结构。Pt-G催化剂在氧还原反应(ORR)中表现出良好的催化性能和稳定性。将复合电极与Al合金阳极组成海水溶解氧电池进行放电测试,电池在低温、贫氧及小电流密度条件下放电性能良好,最大功率密度达到197 mW/L。 展开更多
关键词 海水溶解氧电池 改性碳纤维 石墨烯-铂复合催化剂 氧还原反应 恒电流放电
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硅氢加成反应用均相铂催化剂研究进展
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作者 张柯 陈祝安 +3 位作者 黄光英 晏彩先 常桥稳 左川 《贵金属》 CAS 北大核心 2024年第3期93-101,共9页
有机硅化合物和以其为基础的有机硅材料兼备了无机材料和有机材料的独特结构和性能,在国防军工、工农业生产、高新技术、医药卫生和日常生活中均有着重要的应用。硅氢加成反应是有机硅化学反应中最重要的反应类型之一。本文综述了硅氢... 有机硅化合物和以其为基础的有机硅材料兼备了无机材料和有机材料的独特结构和性能,在国防军工、工农业生产、高新技术、医药卫生和日常生活中均有着重要的应用。硅氢加成反应是有机硅化学反应中最重要的反应类型之一。本文综述了硅氢加成反应用铂(Pt)催化剂的Chalk-Harrod机理及其修正机理的研究动向及发展现状,进一步对铂(Pt)催化剂,如Speier催化剂、Karstedt催化剂、其他铂(Pt)配合物催化剂等均相催化剂的研究进展及优缺点进行了评述,展望了硅氢加成反应中均相铂催化剂的发展方向。 展开更多
关键词 硅氢加成 催化机理 铂催化剂 有机硅 进展
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SnCl_(2)促进的Pt1/PS-PPh_(2)催化剂高选择性催化高碳烯烃氢甲酰化反应
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作者 虞周楠 张磊磊 +7 位作者 谈源龙 井日峥 曹宏晨 楼才溢 格日乐 王军虎 王爱琴 张涛 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第5期316-326,共11页
氢甲酰化作为工业上制备醛、醇等含氧化合物的重要反应,广泛应用于制备洗涤剂、增塑剂、表面活性剂和香料等.目前,氢甲酰化反应主要使用HCo(CO)_(4),HCo(CO)_(3)(PR_(3))和HRh(CO)(PPh_(3))_(2)等配合物作为催化剂.尽管Co基催化剂可以... 氢甲酰化作为工业上制备醛、醇等含氧化合物的重要反应,广泛应用于制备洗涤剂、增塑剂、表面活性剂和香料等.目前,氢甲酰化反应主要使用HCo(CO)_(4),HCo(CO)_(3)(PR_(3))和HRh(CO)(PPh_(3))_(2)等配合物作为催化剂.尽管Co基催化剂可以将高碳烯烃、内烯烃以及支链烯烃高选择性地转化为直链醛,但其反应条件(5-30 MPa,140-200℃)较苛刻,且容易发生烯烃加氢等副反应.相比之下,Rh催化剂的活性比Co基催化剂高1-2个数量级,且反应条件较为温和.但Rh储量稀少,价格昂贵,而且对于高碳烯烃氢甲酰化反应,Rh催化剂难以分离和循环使用.因此,研究者开展了其他金属催化剂的研究,其中Pt-Sn催化剂因其出色的区域选择性而备受关注.但目前Pt-Sn催化剂多局限于均相催化体系,而且Sn助剂的作用尚不明确.本文采用商业化三苯基膦嫁接的聚苯乙烯小球为载体,通过浸渍法制备了SnCl_(2)-Pt_(1)/PS-PPh_(2)单原子催化剂,考察了其在长链-烯烃氢甲酰化反应中的催化性能,并研究了Sn的促进作用.首先,以1-己烯氢甲酰化为探针反应,对催化剂的组成以及反应条件进行了优化.当Pt/P/Sn=1/2/5时,催化剂表现出最高的催化活性,在90-120℃和4-6 MPa合成气条件下,催化剂转化频率(TOF)为40 h^(-1),产物醛的正异比>42.随后,考察了催化剂的底物适用性.结果表明,C6-C12的高碳烯烃均可被高选择性地转化为相应的醛(正异比>20).然而,在循环使用实验中,由于SnCl_(2)不能稳定锚定在载体上,第二次循环时催化活性降低.但通过补加SnCl_(2),催化活性可以完全恢复.高压热过滤实验及元素检测结果表明,反应过程中Pt没有流失.X射线吸收光谱(XAFS)表征结果表明,反应后Pt仍以单原子形式存在,说明Pt1/PS-PPh_(2)具有良好的稳定性.通过准原位X-射线吸收谱、Mössbauer谱和红外光谱表征对反应过程中Pt和Sn的电子性质和配位结构进行了研究.结果表明,SnCl_(2)在反应过程中逐渐转化为Sn(dioxane)Cl3-物种(1,4-二氧六环为反应溶剂),并与Pt原子形成Pt-Sn键.当反应体系中没有Sn时,Pt(II)会被合成气过度还原并发生团聚.当没有膦配体时,Pt原子也会发生聚集,而且SnCl_(2)会在Pt(II)的催化作用下发生水解生成SnO.因此Sn(dioxane)Cl3-与膦配体共同抑制了Pt(I)在反应过程中的还原与聚集.最后,通过XAFS表征深入研究了反应机理.分析结果表明,CO在催化剂上具有较强的吸附作用,而H_(2)则可能以异裂的方式在催化剂上被活化.据此提出可能的反应机理:首先,H_(2)在催化剂上活化先形成Pt-H物种;随后,烯烃插入Pt-H,形成Pt-烷基物种;接着,CO迁移并插入,生成Pt-酰基物种;最后,经过还原消除步骤,得到最终的产物醛.综上,本文制备了一种对高碳烯烃氢甲酰化反应具有良好催化性能的SnCl_(2)-Pt1/PS-PPh_(2)单原子催化剂,为低成本非Rh基催化剂的开发提供借鉴.同时,揭示了催化体系中Sn的促进作用,为通过Lewis酸来调控催化剂的性能提供了参考. 展开更多
关键词 氢甲酰化反应 铂-锡催化剂 高碳烯烃 区域选择性 单原子催化剂
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汽车尾气治理用三效催化剂中铂钯替代的研究进展
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作者 张馨元 王成雄 +3 位作者 郑婷婷 杨冬霞 夏文正 赵云昆 《贵金属》 CAS 北大核心 2024年第S01期142-147,共6页
铂族金属的最大工业用途是汽车尾气净化催化剂,排放法规的日趋严格、汽车产销量的快速增长等因素,导致应用于尾气净化催化剂的钯、铑供需矛盾日益突出。本文从单Pt催化剂、Pt-Rh催化剂和Pt-Pd-Rh催化剂等方面综述了含铂三效催化剂技术... 铂族金属的最大工业用途是汽车尾气净化催化剂,排放法规的日趋严格、汽车产销量的快速增长等因素,导致应用于尾气净化催化剂的钯、铑供需矛盾日益突出。本文从单Pt催化剂、Pt-Rh催化剂和Pt-Pd-Rh催化剂等方面综述了含铂三效催化剂技术的最新研究进展,总结了铂、钯替代或共用的理论和技术可行性,同时分析了存在的不足,并展望未来重点研究方向。 展开更多
关键词 汽车尾气 排放 三效催化剂
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