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期刊论文 294

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关键词

DX桩 2

催化剂 2

力学性能 2

单边直线感应电机 2

沉降 2

Au/Ti双功能催化剂 1

CO2 加氢 1

COVID-19 1

Chebyshev多项式 1

Cu(In 1

DNA结构 1

Ga)Se2 1

H2有效利用率 1

K 助剂 1

LMS 1

Lagrange方程 1

Mn 助剂 1

PPP项目 1

Pt–Ba–Ce/γ-Al2O3 催化剂,物理化学性质,NOx存储和还原,NOx 排放,H2 还原剂 1

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Promising approach for preparing metallic single-atom catalysts: electrochemical deposition

《能源前沿(英文)》 2022年 第16卷 第4期   页码 537-541 doi: 10.1007/s11708-022-0837-5

Oxygen reduction electrocatalysis: From conventional to single-atomic platinum-based catalysts for proton

《能源前沿(英文)》 doi: 10.1007/s11708-023-0907-3

摘要: Platinum (Pt)-based materials are still the most efficient and practical catalysts to drive the sluggish kinetics of cathodic oxygen reduction reaction (ORR) in proton exchange membrane fuel cells (PEMFCs). However, their catalysis and stability performance still need to be further improved in terms of corrosion of both carbon support and Pt catalyst particles as well as Pt loading reduction. Based on the developed synthetic strategies of alloying/nanostructuring Pt particles and modifying/innovating supports in developing conventional Pt-based catalysts, Pt single-atom catalysts (Pt SACs) as the recently burgeoning hot materials with a potential to achieve the maximum utilization of Pt are comprehensively reviewed in this paper. The design thoughts and synthesis of various isolated, alloyed, and nanoparticle-contained Pt SACs are summarized. The single-atomic Pt coordinating with non-metals and alloying with metals as well as the metal-support interactions of Pt single-atoms with carbon/non-carbon supports are emphasized in terms of the ORR activity and stability of the catalysts. To advance further research and development of Pt SACs for viable implementation in PEMFCs, various technical challenges and several potential research directions are outlined.

关键词: oxygen reduction electrocatalysis     Pt single-atom catalysts     conventional Pt-based catalysts     design thoughts and synthesis     metal-support interactions    

Spin polarization strategy to deploy proton resource over atomic-level metal sites for highly selective CO electrolysis

《化学科学与工程前沿(英文)》 2022年 第16卷 第12期   页码 1772-1781 doi: 10.1007/s11705-022-2197-4

摘要: Unlocking of the extremely inert C=O bond during electrochemical CO2 reduction demands subtle regulation on a key “resource”, protons, necessary for intermediate conversion but also readily trapped in water splitting, which is still challenging for developing efficient single-atom catalysts limited by their structural simplicity usually incompetent to handle this task. Incorporation of extra functional units should be viable. Herein, a proton deployment strategy is demonstrated via “atomic and nanostructured iron (A/N-Fe) pairs”, comprising atomically dispersed iron active centers spin-polarized by nanostructured iron carbide ferromagnets, to boost the critical protonation steps. The as-designed catalyst displays a broad window (300 mV) for CO selectivity > 90% (98% maximum), even outperforming numerous cutting-edge M–N–C systems. The well-placed control of proton dynamics by A/N-Fe can promote *COOH/*CO formation and simultaneously suppress H2 evolution, benefiting from the magnetic-proximity-induced exchange splitting (spin polarization) that properly adjusts energy levels of the Fe sites’ d-shells, and further those of the adsorbed intermediates’ antibonding molecular orbitals.

关键词: CO2 electrolysis     single-atom catalysts     spin polarization     proton dynamics     in situ IR spectroscopy     kinetic isotope effect    

Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation

Xinxiang Cao,Arash Mirjalili,James Wheeler,Wentao Xie,Ben W.-L. Jang

《化学科学与工程前沿(英文)》 2015年 第9卷 第4期   页码 442-449 doi: 10.1007/s11705-015-1547-x

摘要: Galvanic replacement, co-impregnation and sequential impregnation have been employed to prepare Pd-Cu bimetallic catalysts with less than 1 wt-% Cu and ca. 0.03 wt-% Pd for selective hydrogenation of acetylene in excess ethylene. High angle annular dark field-scanning transmission electron microscopy (HAADF-STEM) and H chemisorption results confirmed that Pd-Cu single-atom alloy structures were constructed in all three bimetallic catalysts. Catalytic tests indicated that when the conversion of acetylene was above 99%, the selectivity of ethylene of these three single atom alloy catalysts was still more than 73%. Furthermore, the single atom alloy catalyst prepared by sequential incipient wetness impregnation was found to have the best stability among the three procedures used.

关键词: H2 pulse chemisorption     palladium-copper bimetallic catalyst     single atom alloy     acetylene hydrogenation     HAADF-STEM    

The synergic effects of highly selective bimetallic Pt-Pd/SAPO-41 catalysts for the

Guozhi Jia, Chunmu Guo, Wei Wang, Xuefeng Bai, Xiaomeng Wei, Xiaofang Su, Tong Li, Linfei Xiao, Wei Wu

《化学科学与工程前沿(英文)》 2021年 第15卷 第5期   页码 1111-1124 doi: 10.1007/s11705-020-2031-9

摘要: The hydroisomerization of -hexadecane over Pt-Pd bimetallic catalysts is an effective way to produce clean fuel oil. This work reports a useful preparation method of bimetallic bifunctional catalysts by a co-impregnation or sequential impregnation process. Furthermore, monometallic catalysts with loading either Pt or Pd are also prepared for comparison. The effects of the metal species and impregnation order on the characteristics and catalytic performance of the catalysts are investigated. The catalytic test results indicate that the maximum -hexadecane yield over different catalysts increases as follows: Pt/silicoaluminophosphate SAPO-41

关键词: SAPO-41 molecular sieve     Pt-Pd bimetallic site     bifunctional catalysts     n-hexadecane     hydroisomerization    

PM-support interfacial effect and oxygen mobility in Pt, Pd or Rh-loaded (Ce,Zr,La)O catalysts

《环境科学与工程前沿(英文)》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1369-z

摘要:

• Pt/CZL exhibits the optimum catalytic performance for HC and NOx elimination.

关键词: Precious metal-loaded (Ce     Zr     La)O2 catalysts     Oxygen mobility     Catalytic performance    

Investigation of fluorescence characterization and electrochemical behavior on the catalysts of nanosizedPt-Rh/γ-Al

Chang-Mao HUNG, Wen-Liang LAI, Jane-Li LIN

《环境科学与工程前沿(英文)》 2013年 第7卷 第3期   页码 428-434 doi: 10.1007/s11783-013-0517-0

摘要: This work describes the environmentally friendly technology for oxidation of ammonia (NH ) to form nitrogen at temperatures range from 423K to 673K by selective catalytic oxidation (SCO) over a nanosized Pt-Rh/γ-Al O catalyst prepared by the incipient wetness impregnation method of hexachloroplatinic acid (H PtCl ) and rhodium (III) nitrate (Rh(NO ) ) with γ-Al O in a tubular fixed-bed flow quartz reactor (TFBR). The characterization of catalysts were thoroughly measured using transmission electron microscopy (TEM), three-dimensional excitation-emission fluorescent matrix (EEFM) spectroscopy, UV-Vis absorption, dynamic light-scattering (DLS), zeta potential meter, and cyclic voltammetry (CV). The results demonstrated that at a temperature of 673K and an oxygen content of 4%, approximately 99% of the NH was removed by catalytic oxidation over the nanosized Pt-Rh/γ-Al O catalyst. N was the main product in NH -SCO process. Further, it reveals that the oxidation of NH was proceeds by the over-oxidation of NH into NO, which was conversely reacted with the NH to yield N . Therefore, the application of nanosized Pt-Rh/γ-Al O catalyst can significantly enhance the catalytic activity toward NH oxidation. One fluorescent peak for fresh catalyst was different with that of exhausted catalyst. It indicates that EEFM spectroscopy was proven to be an appropriate and effective method to characterize the Pt clusters in intrinsic emission from nanosized Pt-Rh/γ-Al O catalyst. Results obtained from the CV may explain the significant catalytic activity of the catalysts.

关键词: ammonia (NH3)     nanosized Pt-Rh/γ-Al2O3 catalyst     excitation-emission fluorescent matrix (EEFM)     selective catalytic oxidation (SCO)     tubular fixed-bed reactor (TFBR)    

Study on the growth of platinum nanowires as cathode catalysts in proton exchange membrane fuel cells

Ruiqing Wang, Xiaolan Cao, Sheng Sui, Bing Li, Qingfeng Li

《化学科学与工程前沿(英文)》 2022年 第16卷 第3期   页码 364-375 doi: 10.1007/s11705-021-2052-z

摘要: The platinum nanowires have been verified to be a promising catalyst to promote the performance of proton exchange membrane fuel cells. In this paper, accurately controlled growth of nanowires in a carbon matrix is achieved for reducing Pt loading. The effects of formic acid concentration and reaction temperature on the morphology and size of the Pt nanowires, as well as their electrochemical performances in a single cell, are investigated. The results showed that the increase in the formic acid concentration results in a volcano trend with the length of Pt nanowires. With increasing reduction temperature, the diameter of Pt nanowires increases while Pt particles evolve from one-dimensional to zero-dimensional up to 40 °C. A mechanism of the Pt nanowires growth is proposed. The optimized Pt nanowires electrode exhibits a power density (based on electrochemical active surface area) 79% higher than conventional Pt/C one. The control strategy obtained contributes to the design and control of novel nanostructures in nano-synthesis and catalyst applications.

关键词: Pt nanowires     morphology     structure control     in situ growth mechanism     proton exchange membrane fuel cells    

H2Pt-Ba-Ce /γ-Al2O3 催化剂NOx 存储和还原机理的影响研究 Article

王攀, 裔静, 孙川, 罗鹏, 雷利利

《工程(英文)》 2019年 第5卷 第3期   页码 568-575 doi: 10.1016/j.eng.2019.02.005

摘要:

本研究采用浸渍法制备了Pt-Ba-Ce/γ-Al2O3催化剂,利用实验评价了H2 对NSR(NOx storage and reduction)催化剂存储和还原机理的影响,并采用综合表征技术研究了Pt-Ba-Ce /γ-Al2O3

关键词: Pt–Ba–Ce/γ-Al2O3 催化剂,物理化学性质,NOx存储和还原,NOx 排放    

Real atom economy and its application for evaluation the green degree of a process

Weihan WANG, Jing Lü, Li ZHANG, Zhenhua LI

《化学科学与工程前沿(英文)》 2011年 第5卷 第3期   页码 349-354 doi: 10.1007/s11705-010-1030-7

摘要: Green chemistry has attracted more attention in the past century. Among the 12 principles of green chemistry, only atom economy and E factor can be expressed quantitatively to depict the impact of a chemical process to environment. Atom economy was thought better than the traditional yield for evaluating the atom efficiency of raw materials. But it is not enough to reflect the conversion degree of raw material. In this paper, we proposed the concept of real atom economy (RAE) as a metric. RAE could combine the above two factors together to better express the green degree of a process. We further suggested an equation to correlate E factor with RAE. The concept of RAE is proved to be helpful for estimating an environmentally benign process.

关键词: green chemistry     real atom economy     E factor     atom economy     yield    

Pt/C催化剂电子结构调控产氢介观动力学研究 Article

陈文尧, 傅文钊, 段学志, 陈炳旭, 钱刚, 司锐, 周兴贵, 袁渭康, 陈德

《工程(英文)》 2022年 第14卷 第7期   页码 124-133 doi: 10.1016/j.eng.2020.11.014

摘要:

通过调控金属-载体界面间的电子传递提高催化性能已被证明是一种有效且具有挑战性的催化研究策略。本文提出了一种调变铂/碳纳米复合物催化剂中碳载体表面化学性质(载体表面吸电子/给电子含氧官能团),用以精细调控负载金属铂电子性质及其催化性能的方法。本文以氨硼烷水解制氢作为模型反应,结合密度泛函理论(DFT)计算、先进表征技术、动力学及同位素研究,定量关联了载体表面化学性质、铂电荷数与电子结合能、活化熵与活化焓,以及催化活性之间的关系。通过解耦碳载体表面复杂的影响因素,提出铂电荷数可作为实验易测量的催化活性描述符,其中通过铂电荷数的调变可使催化性能提升15倍。在此基础上,首次建立了包含催化剂活性描述符与活性位数量的介观动力学模型,可分别定量催化剂电子与几何效应,并预测催化性能的变化。本文提出的介观动力学模型可进一步用于设计与构筑高效的金属/碳催化剂。

关键词: 介观动力学模型     催化剂描述符     铂电荷数     碳表面化学     产氢活性    

The cooperation effect of Ni and Pt in the hydrogenation of acetic acid

《化学科学与工程前沿(英文)》 2022年 第16卷 第3期   页码 397-407 doi: 10.1007/s11705-021-2076-4

摘要: The catalytic hydrogenation of carboxylic acid to alcohols is one of the important strategies for the conversion of biomass. Herein, a series of Ni-doped PtSn catalysts were prepared, characterized and studied in the hydrogenation of acetic acid. The Ni dopant has a strong interaction with Pt, which promotes the hydrogen adsorption, providing an activated hydrogen-rich environment for the hydrogenation. Meanwhile, the presence of Ni also improves the Pt dispersion, giving more accessible active sites for hydrogen activation. The cooperation of Pt and Ni significantly promotes the catalytic activity of the hydrogenation of acetic acid to ethanol. As a result, the catalyst with 0.1% Ni exhibits the best reaction activity, and its space time yield is twice as that of the PtSn/SiO2 catalyst. It provides a meaningful instruction on the catalyst design for the carboxylic acid hydrogenation.

关键词: acetic acid     ethanol     hydrogenation     Pt     Ni     cooperation effect    

Pt–C interactions in carbon-supported Pt-based electrocatalysts

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1677-1697 doi: 10.1007/s11705-023-2300-5

摘要: Carbon-supported Pt-based materials are highly promising electrocatalysts. The carbon support plays an important role in the Pt-based catalysts by remarkably influencing the growth, particle size, morphology, dispersion, electronic structure, physiochemical property and function of Pt. This review summarizes recent progress made in the development of carbon-supported Pt-based catalysts, with special emphasis being given to how activity and stability enhancements are related to Pt–C interactions in various carbon supports, including porous carbon, heteroatom doped carbon, carbon-based binary support, and their corresponding electrocatalytic applications. Finally, the current challenges and future prospects in the development of carbon-supported Pt-based catalysts are discussed.

关键词: Pt–C interactions     Pt-based materials     carbon support     electrocatalysis    

Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performance

《化学科学与工程前沿(英文)》 2023年 第17卷 第12期   页码 1949-1961 doi: 10.1007/s11705-023-2360-6

摘要: This study aimed to prepare and apply a novel Pt/CdMoO4 composite photocatalyst for photocatalytic N2 fixation and tetracycline degradation. The Pt/CdMoO4 composite was subjected to comprehensive investigation on the morphology, structure, optical properties, and photoelectric chemical properties. The results demonstrate the dispersion of Pt nanoparticles on the CdMoO4 surface. Close contact between CdMoO4 and Pt was observed, resulting in the formation of a heterojunction structure at their contact region. Density functional theory calculation and Mott-Schottky analysis revealed that Pt possesses a higher work function value than CdMoO4, resulting in electron drift from CdMoO4 to Pt and the formation of a Schottky barrier. The presence of this barrier increases the separation efficiency of electron-hole pairs, thereby improving the performance of the Pt/CdMoO4 composite in photocatalysis. When exposed to simulated sunlight, the optimal Pt/CdMoO4 catalyst displayed a photocatalytic nitrogen fixation rate of 443.7 μmol·L‒1·g‒1·h‒1, which is 3.2 times higher than that of pure CdMoO4. In addition, the composite also exhibited excellent performance in tetracycline degradation, with hole and superoxide species identified as the primary reactive species. These findings offer practical insights into designing and synthesizing efficient photocatalysts for photocatalytic nitrogen fixation and antibiotics removal.

关键词: photocatalytic N2 fixation     Pt/CdMoO4     tetracycline degradation     Schottky barrier    

A facile synthesis of high activity cube-like Pt/carbon composites for fuel cell application

Reza B. MOGHADDAM, Samaneh SHAHGALDI, Xianguo LI

《能源前沿(英文)》 2017年 第11卷 第3期   页码 245-253 doi: 10.1007/s11708-017-0492-4

摘要: High activity catalyst with simple low-cost synthesis is essential for fuel cell commercialization. In this study, a facile procedure for the synthesis of cube-like Pt nanoparticle (Pt ) composites with high surface area carbon supports is developed by mixing precursor of Pt with carbon supports in organic batches, hence, one pot synthesis. The Pt grow with Vulcan XC-72 or Ketjen black, respectively, and then treated for 5.5 h at 185ºC (i.e., Pt /V and Pt /K). The resulting particle sizes and shapes are similar; however, Pt /K has a larger electrochemical active surface area (EASA) and a remarkably better formic acid (FA) oxidation performance. Optimization of the Pt /K composites leads to Pt /K that has been treated for 10 h at 185ºC. With a larger EASA, Pt /K is also more active in FA oxidation than the other Pt /K composites. Impedance spectroscopy analysis of the temperature treated and as-prepared (i.e., untreated) Pt /K composites indicates that Pt /K is less resistive, and has the highest limiting capacitance among the Pt /K electrodes. Consistently, the voltammetric EASA is the largest for Pt /K. Furthermore, Pt /K is compared with two commercial Pt/C catalysts, Tanaka Kikinzoku Kogyo (TKK), and Johnson Matthey (JM)Pt/C catalysts. The TKK Pt/C has a higher EASA than Pt /K, as expected from their relative particles sizes (3–4 nm vs. 6–7 nm for Pt /K), however, Pt /K has a significantly better FA oxidation activity.

关键词: synthesis     cube-like Pt     Pt/C composite     catalyst     impedance    

标题 作者 时间 类型 操作

Promising approach for preparing metallic single-atom catalysts: electrochemical deposition

期刊论文

Oxygen reduction electrocatalysis: From conventional to single-atomic platinum-based catalysts for proton

期刊论文

Spin polarization strategy to deploy proton resource over atomic-level metal sites for highly selective CO electrolysis

期刊论文

Investigation of the preparation methodologies of Pd-Cu single atom alloy catalysts for selective hydrogenation

Xinxiang Cao,Arash Mirjalili,James Wheeler,Wentao Xie,Ben W.-L. Jang

期刊论文

The synergic effects of highly selective bimetallic Pt-Pd/SAPO-41 catalysts for the

Guozhi Jia, Chunmu Guo, Wei Wang, Xuefeng Bai, Xiaomeng Wei, Xiaofang Su, Tong Li, Linfei Xiao, Wei Wu

期刊论文

PM-support interfacial effect and oxygen mobility in Pt, Pd or Rh-loaded (Ce,Zr,La)O catalysts

期刊论文

Investigation of fluorescence characterization and electrochemical behavior on the catalysts of nanosizedPt-Rh/γ-Al

Chang-Mao HUNG, Wen-Liang LAI, Jane-Li LIN

期刊论文

Study on the growth of platinum nanowires as cathode catalysts in proton exchange membrane fuel cells

Ruiqing Wang, Xiaolan Cao, Sheng Sui, Bing Li, Qingfeng Li

期刊论文

H2Pt-Ba-Ce /γ-Al2O3 催化剂NOx 存储和还原机理的影响研究

王攀, 裔静, 孙川, 罗鹏, 雷利利

期刊论文

Real atom economy and its application for evaluation the green degree of a process

Weihan WANG, Jing Lü, Li ZHANG, Zhenhua LI

期刊论文

Pt/C催化剂电子结构调控产氢介观动力学研究

陈文尧, 傅文钊, 段学志, 陈炳旭, 钱刚, 司锐, 周兴贵, 袁渭康, 陈德

期刊论文

The cooperation effect of Ni and Pt in the hydrogenation of acetic acid

期刊论文

Pt–C interactions in carbon-supported Pt-based electrocatalysts

期刊论文

Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performance

期刊论文

A facile synthesis of high activity cube-like Pt/carbon composites for fuel cell application

Reza B. MOGHADDAM, Samaneh SHAHGALDI, Xianguo LI

期刊论文