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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    

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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    

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A review of Pt-based electrocatalysts for oxygen reduction reaction

Changlin ZHANG, Xiaochen SHEN, Yanbo PAN, Zhenmeng PENG

《能源前沿（英文）》 2017年 第11卷 第3期   页码 268-285 doi: 10.1007/s11708-017-0466-6

摘要： Development of active and durable electrocatalyst for oxygen reduction reaction (ORR) remains one challenge for the polymer electrolyte membrane fuel cell (PEMFC) technology. Pt-based nanomaterials show the greatest promise as electrocatalyst for this reaction among all current catalytic structures. This review focuses on Pt-based ORR catalyst material development and covers the past achievements, current research status and perspectives in this research field. In particular, several important categories of Pt-based catalytic structures and the research advances are summarized. Key factors affecting the catalyst activity and durability are discussed. An outlook of future research direction of ORR catalyst research is provided.

关键词： oxygen reduction reaction (ORR)     electrocatalysis     platinum catalyst     activity     durability    

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Design of efficient Pt-based electrocatalysts through characterization by X-ray absorption spectroscopy

Nebojsa S. MARINKOVIC, Kotaro SASAKI, Radoslav R. ADZIC

《能源前沿（英文）》 2017年 第11卷 第3期   页码 236-244 doi: 10.1007/s11708-017-0487-1

摘要： A method is described to determine the internal structure of electrocatalyst nanoparticles by X-ray absorption spectroscopy (XAS). The nondestructive spectroscopic technique typically utilizing synchrotron radiation as the source measures changes in the X-ray absorption coefficient as a function of energy. The bulk technique has found its use for materials characterization in all scientific areas, including nanomaterials. The analysis of the internal structure of nanoparticles reveals interatomic distances and coordination numbers for each element, and their values and mutual relations indicate whether the elements form a homogeneous or heterogeneous mixture. The core-shell heterogeneous structure in which certain elements are predominantly located in the core, and others form the encapsulating shell is of particular importance in catalysis and electrocatalysis because it may reduce the amount of precious metals in nanoparticles by replacing the atoms in the core of nanoparticles with more abundant and cheaper alternatives. The examples of nanoparticle structures designed in the laboratory and the approach to model efficient catalysts through systematic analysis of XAS data in electrochemical systems consisting of two and three metals are also demonstrated.

关键词： X-ray absorption spectroscopy     EXAFS     XANES     nanocatalysts     core shell    

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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    

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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    

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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)    

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Effect of Fe content on FeMn catalysts for light alkenes synthesis

ZHOU Jun, CHU Wei, ZHANG Hui, XU Huiyuan, ZHANG Tao

《化学科学与工程前沿（英文）》 2008年 第2卷 第3期   页码 315-318 doi: 10.1007/s11705-008-0050-z

摘要： The effect of Fe content on FeMn/MgO catalysts for light alkenes synthesis through CO hydrogenation was investigated. Catalysts were prepared by a conventional co-impregnation method, characterized using BET, X-ray powder diffraction (XRD) and Temperature-programmed reduction (H-TPR) techniques. High activity was obtained over the catalyst with 9 wt-% Fe content, over which CO conversion and the selectivity of C–C reached 91.36% and 58.48%, respectively. With the increase of Fe content, both the conversion and the selectivity were improved within a certain range and then decreased. The results show that the surface area of the catalyst played an important role in the catalytic reaction. With the increase of Fe loading, the interaction action between Fe and Mn was enhanced and FeMn solid solution was formed.

关键词： conventional co-impregnation     increase     conversion     loading     H-TPR    

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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    

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H2 对Pt-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    

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Selective preparation for biofuels and high value chemicals based on biochar catalysts

《能源前沿（英文）》 2023年 第17卷 第5期   页码 635-653 doi: 10.1007/s11708-023-0878-4

摘要： The reuse of biomass wastes is crucial toward today’s energy and environmental crisis, among which, biomass-based biochar as catalysts for biofuel and high value chemical production is one of the most clean and economical solutions. In this paper, the recent advances in biofuels and high chemicals for selective production based on biochar catalysts from different biomass wastes are critically summarized. The topics mainly include the modification of biochar catalysts, the preparation of energy products, and the mechanisms of other high-value products. Suitable biochar catalysts can enhance the yield of biofuels and higher-value chemicals. Especially, the feedstock and reaction conditions of biochar catalyst, which affect the efficiency of energy products, have been the focus of recent attentions. Mechanism studies based on biochar catalysts will be helpful to the controlled products. Therefore, the design and advancement of the biochar catalyst based on mechanism research will be beneficial to increase biofuels and the conversion efficiency of chemicals into biomass. The advanced design of biochar catalysts and optimization of operational conditions based on the biomass properties are vital for the selective production of high-value chemicals and biofuels. This paper identifies the latest preparation for energy products and other high-value chemicals based on biochar catalysts progresses and offers insights into improving the yield of high selectivity for products as well as the high recyclability and low toxicity to the environment in future applications.

关键词： biomass     biochar catalysts     biofuels     high chemicals    

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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    

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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    

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Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

《化学科学与工程前沿（英文）》 2015年 第9卷 第3期   页码 280-294 doi: 10.1007/s11705-015-1524-4

摘要： Developing metal-free, carbon-based catalysts to replace platinum-based catalysts for oxygen reduction reactions (ORRs) is an emerging area of research. In recent years, different carbon structures including carbon doped with IIIA-VIIA heteroatoms (C−M site-based, where M represents the doped heteroatom) and polynitrogen (PN) compounds encapsulated in carbon nanotubes (CNTs) (N−N site-based) have been synthesized. Compared to metallic catalysts, these materials are highly active, stable, inexpensive, and environmentally friendly. This review discusses the development of these materials, their ORR performances and the mechanisms for how the incorporation of heteroatoms enhances the ORR activity. Strategies for tailoring the structures of the carbon substrates to improve ORR performance are also discussed. Future studies in this area will need to include optimizing synthetic strategies to control the type, amount and distribution of the incorporated heteroatoms, as well as better understanding the ORR mechanisms in these catalysts.

关键词： oxygen reduction reaction     electrocatalysis     metal-free     carbon-based     polynitrogen    

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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    

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标题 作者 时间 类型 操作

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

期刊论文

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

期刊论文

A review of Pt-based electrocatalysts for oxygen reduction reaction

Changlin ZHANG, Xiaochen SHEN, Yanbo PAN, Zhenmeng PENG

期刊论文

Design of efficient Pt-based electrocatalysts through characterization by X-ray absorption spectroscopy

Nebojsa S. MARINKOVIC, Kotaro SASAKI, Radoslav R. ADZIC

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

Effect of Fe content on FeMn catalysts for light alkenes synthesis

ZHOU Jun, CHU Wei, ZHANG Hui, XU Huiyuan, ZHANG Tao

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

H2 对Pt-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

Selective preparation for biofuels and high value chemicals based on biochar catalysts

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

Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

期刊论文

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

期刊论文