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催化剂 2

Au/Ti双功能催化剂 1

CO2 加氢 1

H2有效利用率 1

K 助剂 1

Mn 助剂 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

SOFC 1

Si/Al 比值 1

n 型碳纳米管 1

丙烯环氧化 1

乙烷干重整 1

二氧化碳 1

二甲苯 1

产氢活性 1

介观动力学模型 1

催化剂描述符 1

催化还原 1

反应机理 1

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Electrochemical CO reduction to C products over CuZn intermetallic catalysts synthesized by electrodeposition

《能源前沿(英文)》 doi: 10.1007/s11708-023-0898-0

摘要: Electrocatalytic CO2 reduction (ECR) offers an attractive approach to realizing carbon neutrality and producing valuable chemicals and fuels using CO2 as the feedstock. However, the lack of cost-effective electrocatalysts with better performances has seriously hindered its application. Herein, a one-step co-electrodeposition method was used to introduce Zn, a metal with weak *CO binding energy, into Cu to form Cu/Zn intermetallic catalysts (Cu/Zn IMCs). It was shown that, using an H-cell, the high Faradaic efficiency of C2+ hydrocarbons/alcohols (FEC2+) could be achieved in ECR by adjusting the surface metal components and the applied potential. In suitable conditions, FEC2+ and current density could be as high as 75% and 40 mA/cm2, respectively. Compared with the Cu catalyst, the Cu/Zn IMCs have a lower interfacial charge transfer resistance and a larger electrochemically active surface area (ECSA), which accelerate the reaction. Moreover, the *CO formed on Zn sites can move to Cu sites due to its weak binding with *CO, and thus enhance the C–C coupling on the Cu surface to form C2+ products.

关键词: carbon dioxide electroreduction     electrochemistry     co-electrodeposition     intermetallic catalysts     value-added chemicals    

hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated Ni–Sn intermetallic

《化学科学与工程前沿(英文)》 2023年 第17卷 第2期   页码 139-155 doi: 10.1007/s11705-022-2217-4

摘要: Porous carbon-encapsulated Ni and Ni–Sn intermetallic compound catalysts were prepared by the one-pot extended Stöber method followed by carbonization and tested for in-situ hydrothermal deoxygenation of methyl palmitate with methanol as the hydrogen donor. During the catalyst preparation, Sn doping reduces the size of carbon spheres, and the formation of Ni–Sn intermetallic compounds restrain the graphitization, contributing to larger pore volume and pore diameter. Consequently, a more facile mass transfer occurs in carbon-encapsulated Ni–Sn intermetallic compound catalysts than in carbon-encapsulated Ni catalysts. During the in-situ hydrothermal deoxygenation, the synergism between Ni and Sn favors palmitic acid hydrogenation to a highly reactive hexadecanal that easily either decarbonylate to n-pentadecane or is hydrogenated to hexadecanol. At high reaction temperature, hexadecanol undergoes dehydrogenation–decarbonylation, generating n-pentadecane. Also, the C–C bond hydrolysis and methanation are suppressed on Ni–Sn intermetallic compounds, favorable for increasing the carbon yield and reducing the H2 consumption. The n-pentadecane and n-hexadecane yields reached 88.1% and 92.8% on carbon-encapsulated Ni3Sn2 intermetallic compound at 330 °C. After washing and H2 reduction, the carbon-encapsulated Ni3Sn2 intermetallic compound remains stable during three recycling cycles. This is ascribed to the carbon confinement that effectively suppresses the sintering and loss of metal particles under harsh hydrothermal conditions.

关键词: extended Stöber method     carbon encapsulated Ni–Sn intermetallic compounds     confinement     in-situ hydrothermal deoxygenation     hydrogenation     decarbonylation    

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    

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

Current challenge and perspective of PGM-free cathode catalysts for PEM fuel cells

Gang WU

《能源前沿(英文)》 2017年 第11卷 第3期   页码 286-298 doi: 10.1007/s11708-017-0477-3

摘要: To significantly reduce the cost of proton exchange membrane fuel cells, platinum-group metal (PGM)-free cathode catalysts are highly desirable. Current M-N-C (M: Fe, Co or Mn) catalysts are considered the most promising due to their encouraging performance. The challenge thus has been their stability under acidic conditions, which has hindered their use for any practical applications. In this review, based on the author’s research experience in the field for more than 10 years, current challenges and possible solutions to overcome these problems were discussed. The current Edisonian approach (i.e., trial and error) to developing PGM-free catalysts has been ineffective in achieving revolutionary breakthroughs. Novel synthesis techniques based on a more methodological approach will enable atomic control and allow us to achieve optimal electronic and geometric structures for active sites uniformly dispersed within the 3D architectures. Structural and chemical controlled precursors such as metal-organic frameworks are highly desirable for making catalysts with an increased density of active sites and strengthening local bonding structures among N, C and metals. Advanced electrochemical and physical characterization, such as electron microscopy and X-ray absorption spectroscopy should be combined with first principle density functional theory (DFT) calculations to fully elucidate the active site structures.

关键词: oxygen reduction     fuel cells     cathode     nonprecious metal catalysts     carbon nanocomposites    

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    

Catalytic combustion of volatile organic compounds using perovskite oxides catalysts—a review

《化学科学与工程前沿(英文)》 2023年 第17卷 第11期   页码 1649-1676 doi: 10.1007/s11705-023-2324-x

摘要: With the rapid development of industry, volatile organic compounds (VOCs) are gaining attention as a class of pollutants that need to be eliminated due to their adverse effects on the environment and human health. Catalytic combustion is the most popular technology used for the removal of VOCs as it can be adapted to different organic emissions under mild conditions. This review first introduces the hazards of VOCs, their treatment technologies, and summarizes the treatment mechanism issues. Next, the characteristics and catalytic performance of perovskite oxides as catalysts for VOC removal are expounded, with a special focus on lattice distortions and surface defects caused by metal doping and surface modifications, and on the treatment of different VOCs. The challenges and the prospects regarding the design of perovskite oxides catalysts for the catalytic combustion of VOCs are also discussed. This review provides a reference base for improving the performance of perovskite catalysts to treat VOCs.

关键词: perovskite oxides     volatile organic compounds     catalytic combustion     reaction mechanism    

Enhanced activity of bimetallic Fe-Cu catalysts supported on ceria toward water gas shift reaction: synergistic

《化学科学与工程前沿(英文)》 2023年 第17卷 第12期   页码 1962-1972 doi: 10.1007/s11705-023-2359-z

摘要: Within the “hydrogen chain”, the high-temperature water gas shift reaction represents a key step to improve the H2 yield and adjust the H2/COx ratio to fit the constraints of downstream processes. Despite the commercial application of the high-temperature water gas shift, novel catalysts characterized by higher intrinsic activity (especially at low temperatures), good thermal stability, and no chromium content are needed. In this work, we propose bimetallic iron-copper catalysts supported on ceria, characterized by low active phase content (iron oxide + copper oxide < 5 wt %). Fresh and used samples were characterized by inductively coupled plasma mass spectrometry, X-ray diffraction, nitrogen physisorption, scanning electron microscopy coupled with energy-dispersive X-ray spectroscopy, and temperature programmed reduction in hydrogen to relate physicochemical features and catalytic activity. The sample with iron/copper ≈ 1 and 4 wt % active phase content showed the best catalytic properties in terms of turnover frequency, no methane formation, and stability. Its unique properties were due to both strong iron-copper interaction and strong metal-support interaction, leading to outstanding redox behavior.

关键词: water gas shift     iron     copper     bimetallic catalysts     ceria     hydrogen    

NiBO (B = Mn or Co) catalysts for NH-SCR of NO at low-temperature in microwave field

《环境科学与工程前沿(英文)》 2023年 第17卷 第8期 doi: 10.1007/s11783-023-1696-y

摘要:

● Microwave-assisted catalytic NH3-SCR reaction over spinel oxides is carried out.

关键词: Microwave field     Spinel oxides     NOx     Selective catalytic reduction    

Application of electrode materials and catalysts in electrocatalytic treatment of dye wastewater

《化学科学与工程前沿(英文)》 2021年 第15卷 第6期   页码 1427-1443 doi: 10.1007/s11705-021-2108-0

摘要: The dye industry produces a large amount of hazardous wastewater every day worldwide, which brings potential threaten to the global environment. As an excellent method for removal of water chroma and chemical oxygen demand, electrocatalytic methods are currently widely used in the treatment of dye wastewater. The selection and preparation of electrode materials and electrocatalysts play an important role on the electrocatalytic treatment. The aim of this paper is to introduce the most excellent high-efficiency electrode materials and electrocatalysts in the field of dye wastewater treatment. Many electrode materials such as metal electrode materials, boron-doped diamond anode materials and three-dimensional electrode are introduced in detail. Besides, the mechanism of electrocatalytic oxidation is summarized. The composite treatment of active electrode and electrocatalyst are extensively examined. Finally, the progress of photo-assisted electrocatalytic methods of dye wastewater and the catalysts are described.

关键词: electrocatalytic oxidation     electrode     electrocatalysis     dye wastewater    

Advances and perspectives in catalysts for liquid-phase oxidation of cyclohexane

Hui LI, Yuanbin SHE, Tao WANG

《化学科学与工程前沿(英文)》 2012年 第6卷 第3期   页码 356-368 doi: 10.1007/s11705-012-0903-3

摘要: The latest progress and developments in catalysts for the oxidation of cyclohexane are reviewed. Catalytic systems for the oxidation of cyclohexane including metal supported, metal oxides, molecular sieves, metal substituted polyoxometalates, photocatalysts, organocatalysts, Gif systems, metal-organic catalysts and metalloporphyrins are discussed with a particular emphasis on metalloporphyrin catalytic systems. The advantages and disadvantages of these methods are summarized and analyzed. Finally, the development trends in the oxidation technology of cyclohexane are examined.

关键词: cyclohexane     liquid-phase oxidation     catalysis    

Computational design of heterogeneous catalysts and gas separation materials for advanced chemical processing

Huaiwei Shi, Teng Zhou

《化学科学与工程前沿(英文)》 2021年 第15卷 第1期   页码 49-59 doi: 10.1007/s11705-020-1959-0

摘要: Functional materials are widely used in chemical industry in order to reduce the process cost while simultaneously increase the product quality. Considering their significant effects, systematic methods for the optimal selection and design of materials are essential. The conventional synthesis-and-test method for materials development is inefficient and costly. Additionally, the performance of the resulting materials is usually limited by the designer’s expertise. During the past few decades, computational methods have been significantly developed and they now become a very important tool for the optimal design of functional materials for various chemical processes. This article selectively focuses on two important process functional materials, namely heterogeneous catalyst and gas separation agent. Theoretical methods and representative works for computational screening and design of these materials are reviewed.

关键词: heterogeneous catalyst     gas separation     solvent     porous adsorbent     material screening and design    

Preparation and influence of performance of anodic catalysts for direct methanol fuel cell

WANG Zhenbo, YIN Geping, SHI Pengfei

《化学科学与工程前沿(英文)》 2007年 第1卷 第1期   页码 20-25 doi: 10.1007/s11705-007-0005-9

摘要: This research aims at increasing the utilization of platinum-ruthenium alloy (Pt-Ru) catalysts and thus lowering the catalyst loading in anodes for methanol electrooxidation. The direct methanol fuel cell s (DMFC) anodic catalysts, Pt-Ru/C, were prepared by chemical reduction with a reducing agent added in two kinds of solutions under different circumstances. The reducing agent was added in hot solution with the protection of inert gases or just air, and in cold solution with inert gases. The catalysts were treated at different temperatures. Their performance was tested by cyclic voltammetry and potentiostatic polarization by utilizing their inherent powder microelectrode in 0.5 mol/L CHOH and 0.5 mol/L HSO solution. The structures and micro-surface images of the catalysts were determined and observed by X-ray diffraction and transmission electron microscopy, respectively. The catalyst prepared in inert gases showed a better catalytic performance for methanol electrooxidation than that prepared in air. It resulted in a more homogeneous distribution of the Pt-Ru alloy in carbon. Its size is small, only about 4.5 nm. The catalytic performance is affected by the order of the reducing agent added. The performance of the catalyst prepared by adding the reductant at constant temperature of the solution is better than that prepared by adding it in the solution at 0?C and then heating it up to the reducing temperature. The structure of the catalyst was modified, and there was an increase in the conversion of ruthenium into the alloyed state and an increase in particle size with the ascension of heat treatment temperature. In addition, the stability of the catalyst was improved after heat treatment.

关键词: catalyst prepared     stability     ascension     potentiostatic polarization     platinum-ruthenium    

Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

Xinxiang Cao, Tengteng Lyu, Wentao Xie, Arash Mirjalili, Adelaide Bradicich, Ricky Huitema, Ben W.-L. Jang, Jong K. Keum, Karren More, Changjun Liu, Xiaoliang Yan

《化学科学与工程前沿(英文)》 2020年 第14卷 第4期   页码 522-533 doi: 10.1007/s11705-019-1822-3

摘要: A series of PdCu bimetallic catalysts with low Cu and Pd loadings and different Cu: Pd atomic ratios were prepared by conventionally sequential impregnation (CSI) and modified sequential impregnation (MSI) of Cu and Pd for selective hydrogenation of acetylene. Characterization indicates that the supported copper (II) nitrate in the PdCu bimetallic catalysts prepared by MSI can be directly reduced to Cu metal particles due to the hydrogen spillover from Pd to Cu(NO ) crystals. In addition, for the catalysts prepared by MSI, Pd atoms can form PdCu alloy on the surface of metal particles, however, for the catalysts prepared by CSI, Pd tends to migrate and exist below the surface layer of Cu. Reaction results indicate that compared with CSI, the MSI method enables samples to possess preferable stability as well as comparable reaction activity. This should be due to the MSI method in favor of the formation of PdCu alloy on the surface of metal particles. Moreover, even Pd loading is super low,<0.045 wt-% in this study, by through adjusting Cu loading to an appropriate value, attractive reactivity and selectivity still can be achieved.

关键词: copper     palladium     catalysts     acetylene     selective hydrogenation    

High-entropy catalysts for electrochemical water-electrolysis of hydrogen evolution and oxygen evolution

《能源前沿(英文)》 doi: 10.1007/s11708-023-0892-6

摘要: High entropy materials (HEMs) have developed rapidly in the field of electrocatalytic water-electrolysis for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) due to their unique properties. In particular, HEM catalysts are composed of many elements. Therefore, they have rich active sites and enhanced entropy stability relative to single atoms. In this paper, the preparation strategies and applications of HEM catalysts in electrochemical water-electrolysis are reviewed to explore the stabilization of HEMs and their catalytic mechanisms as well as their application in support green hydrogen production. First, the concept and four characteristics of HEMs are introduced based on entropy and composition. Then, synthetic strategies of HEM catalysts are systematically reviewed in terms of the categories of bottom-up and top-down. The application of HEMs as catalysts for electrochemical water-electrolysis in recent years is emphatically discussed, and the mechanisms of improving the performance of electrocatalysis is expounded by combining theoretical calculation technology and ex-situ/in situ characterization experiments. Finally, the application prospect of HEMs is proposed to conquer the challenges in HEM catalyst fabrications and applications.

关键词: high-entropy     electrocatalysis     synthetic methods     water-electrolysis     hydrogen and oxygen evolutions    

标题 作者 时间 类型 操作

Electrochemical CO reduction to C products over CuZn intermetallic catalysts synthesized by electrodeposition

期刊论文

hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated Ni–Sn intermetallic

期刊论文

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

期刊论文

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

期刊论文

Current challenge and perspective of PGM-free cathode catalysts for PEM fuel cells

Gang WU

期刊论文

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

期刊论文

Catalytic combustion of volatile organic compounds using perovskite oxides catalysts—a review

期刊论文

Enhanced activity of bimetallic Fe-Cu catalysts supported on ceria toward water gas shift reaction: synergistic

期刊论文

NiBO (B = Mn or Co) catalysts for NH-SCR of NO at low-temperature in microwave field

期刊论文

Application of electrode materials and catalysts in electrocatalytic treatment of dye wastewater

期刊论文

Advances and perspectives in catalysts for liquid-phase oxidation of cyclohexane

Hui LI, Yuanbin SHE, Tao WANG

期刊论文

Computational design of heterogeneous catalysts and gas separation materials for advanced chemical processing

Huaiwei Shi, Teng Zhou

期刊论文

Preparation and influence of performance of anodic catalysts for direct methanol fuel cell

WANG Zhenbo, YIN Geping, SHI Pengfei

期刊论文

Preparation and investigation of Pd doped Cu catalysts for selective hydrogenation of acetylene

Xinxiang Cao, Tengteng Lyu, Wentao Xie, Arash Mirjalili, Adelaide Bradicich, Ricky Huitema, Ben W.-L. Jang, Jong K. Keum, Karren More, Changjun Liu, Xiaoliang Yan

期刊论文

High-entropy catalysts for electrochemical water-electrolysis of hydrogen evolution and oxygen evolution

期刊论文