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Electrocatalysts Electrocatalysts
Q1 Materials Science Pub Date : 2021-01-01 DOI: 10.1039/9781839163128-00417
C. Feng, H. Su, J. Zeng
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引用次数: 4
Plasmonic photocatalysis 电浆光催化
Q1 Materials Science Pub Date : 2021-01-01 DOI: 10.1142/9781786341259_0010
S. Ramakrishnan, R. T. A. Tirumala, Farshid Mohammadparast, Tong Mou, Tien Le, Bin Wang, M. Andiappan
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引用次数: 1
Catalysis 催化
Q1 Materials Science Pub Date : 2020-08-11 DOI: 10.1002/9783527809080.cataz02996
R. Augustine
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引用次数: 0
Catalysis 催化
Q1 Materials Science Pub Date : 2020-01-01 DOI: 10.1039/9781788019477
D. Yu.
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引用次数: 0
Catalytic Conversion of Biomass-derived Compounds to C4 Chemicals 生物质衍生化合物催化转化为C4化学品
Q1 Materials Science Pub Date : 2019-02-12 DOI: 10.1039/9781788016971-00001
Fan-Xin Zeng, K. Hohn
Increasing interest in converting bio-renewable chemical into liquid fuel, polymers and pharmaceutical products has attract extensive attention both in academic and industrial research to replace petrochemicals with novel platform chemicals derived from bio-based feedstock. Chemistry involving C4 chemicals (molecules with four carbon atoms) has been studied to make a variety of products, including fuel additives and polymer building blocks. This chapter gives an overview of the catalytic synthesis of C4 products from bio-sustainable chemicals, including C4 diols, alkenes, ketones and alcohols, by reviewing the impact of catalyst composition on product selective and the speculated catalytic reaction mechanisms.
将生物可再生化学品转化为液体燃料、聚合物和制药产品的兴趣日益增加,这在学术和工业研究中引起了广泛的关注,用来自生物基原料的新型平台化学品取代石化产品。涉及C4化学物质(具有四个碳原子的分子)的化学已经被研究用于制造各种产品,包括燃料添加剂和聚合物构建块。本章综述了生物可持续化学品(包括C4二醇、烯烃、酮类和醇类)催化合成C4产物的研究进展,综述了催化剂组成对产物选择性的影响以及推测的催化反应机理。
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引用次数: 7
Nanocomposite catalysts for transformation of biofuels into syngas and hydrogen: fundamentals of design and performance, application in structured reactors and catalytic membranes 将生物燃料转化为合成气和氢气的纳米复合催化剂:设计和性能的基础,在结构反应器和催化膜中的应用
Q1 Materials Science Pub Date : 2019-02-12 DOI: 10.1039/9781788016971-00216
V. Sadykov, M. Arapova, E. Smal, S. Pavlova, L. Bobrova, N. Eremeev, N. Mezentseva, M. Simonov
In this review problems related to design and performance of stable and efficient catalysts of biogas/biofuels transformation into syngas and hydrogen based on nanocrystalline oxides with fluorite, perovskite and spinel oxides and their nanocomposites promoted by nanoparticles of Pt group metals and Ni-based alloys are considered. Tailor-made design of these catalysts is based upon elucidation of the relationships between their synthesis procedure, composition, real structure/microstructure, surface properties, oxygen mobility and reactivity determined in a great extent by the metal–support interaction, which requires application of modern sophisticated structural, spectroscopic, kinetic (including in situ FTIRS and isotope transients) methods and mathematical modeling. Thin layers of these optimized catalysts supported on structured heat-conducting substrates, asymmetric supported oxygen or hydrogen separation membranes demonstrated high and stable performance in transformation of biogas and biofuels into syngas and hydrogen.
本文讨论了以萤石、钙钛矿和尖晶石氧化物为氧化物的纳米晶氧化物及其Pt族金属和ni基合金纳米复合材料为催化剂,设计和性能稳定、高效的沼气/生物燃料合成气和氢气转化催化剂的相关问题。这些催化剂的定制设计是基于阐明它们的合成过程、组成、实际结构/微观结构、表面性质、氧迁移率和反应性之间的关系,这在很大程度上取决于金属-载体相互作用,这需要应用现代复杂的结构、光谱、动力学(包括原位FTIRS和同位素瞬态)方法和数学建模。这些优化后的催化剂薄层负载在结构化导热衬底、不对称负载的氧或氢分离膜上,在将沼气和生物燃料转化为合成气和氢气方面表现出高而稳定的性能。
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引用次数: 8
Opportunities for controlling catalysis by designing molecular environments around active sites: cations supported on amorphous versus crystalline zeolitic silicate supports 通过设计活性位点周围的分子环境来控制催化的机会:无定形和结晶沸石硅酸盐支撑的阳离子
Q1 Materials Science Pub Date : 2019-02-12 DOI: 10.1039/9781788016971-00072
Nicolás A. Grosso‐Giordano, S. Zones, Alexander Katz
Opportunities for synthetically controlling the molecular architecture of catalytic active sites supported on amorphous silica versus zeolitic silicates are critically examined, and the role that support crystallinity could play on catalytic properties is assessed. We first summarize structural features of active sites on silicate supports and contrast the inherent disorder of amorphous silica surfaces to the order of crystalline zeotypes. We then analyze, within the context of selected catalytic systems currently employed in industrial practice, how these structures affect inner- and outer-sphere environments of isolated active sites, and how these environments could impact catalytic activity and the development of next generation catalysts.
对非晶二氧化硅和沸石硅酸盐支撑的催化活性位点的分子结构进行综合控制的机会进行了严格的研究,并评估了支撑结晶度对催化性能的影响。我们首先总结了硅酸盐载体上活性位点的结构特征,并将非晶态二氧化硅表面固有的无序性与结晶型的有序性进行了对比。然后,我们在工业实践中所选用的催化系统的背景下,分析这些结构如何影响分离活性位点的内外球环境,以及这些环境如何影响催化活性和下一代催化剂的发展。
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引用次数: 3
Understanding catalysis for processing glycerol and glycerol-based derivatives for the production of value added chemicals 了解加工甘油和甘油衍生物用于生产增值化学品的催化作用
Q1 Materials Science Pub Date : 2019-02-12 DOI: 10.1039/9781788016971-00267
Matthew Drewery, G. Sánchez, M. Li, E. Kennedy, M. Stockenhuber
An increase in biodiesel production has seen a dramatic increase in the production of glycerol, the main by-product. To maintain biodiesel production as economically viable, processes for valorising the 10 wt% glycerol waste stream need to be developed. The content of this chapter discusses recent work which examines potential catalytic processes for producing value added chemicals using glycerol as a platform chemical. Significant research has focussed on catalytic reactions tailored to selectively convert oxygenates from biological resources to produce valuable chemicals. While homogenous and biological catalytic processes are important, heterogeneously catalysed reactions are considered to be more desirable and potentially more economically viable due to advantages in feedstock processing. The current transesterification process associated with biodiesel production results in a number of contaminants in the glycerol stream, such as free fatty acids and residual catalyst salts, which affects downstream processing. Special emphasis is given to understand how contaminants of various by-products interact with surfaces and identify robust catalysts while examining alternative catalytic processes for producing biodiesel with purer product streams.
随着生物柴油产量的增加,主要副产品甘油的产量也大幅增加。为了保持生物柴油生产在经济上的可行性,需要开发对10%甘油废物流进行增值的工艺。本章的内容讨论了最近的工作,研究了使用甘油作为平台化学品生产增值化学品的潜在催化过程。重要的研究集中在选择性地将生物资源中的氧合物转化为有价值的化学物质的催化反应上。虽然均相和生物催化过程很重要,但由于在原料处理方面的优势,多相催化反应被认为是更可取的,并且可能在经济上更可行。目前与生物柴油生产相关的酯交换过程导致甘油流中存在许多污染物,如游离脂肪酸和残留的催化剂盐,这些污染物会影响下游加工。特别强调的是,了解各种副产品的污染物如何与表面相互作用,并确定强大的催化剂,同时检查替代催化过程,以生产更纯净的产品流的生物柴油。
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引用次数: 0
Methane activation and conversion on well-defined metal-oxide Surfaces: in situ studies with synchrotron-based techniques 甲烷在明确定义的金属氧化物表面上的活化和转化:同步加速器技术的原位研究
Q1 Materials Science Pub Date : 2019-02-12 DOI: 10.1039/9781788016971-00198
J. Rodríguez, Feng Zhang, Z. Liu, S. Senanayake
Research focussed on in situ studies for the activation and conversion of methane on well-defined metal-oxide surfaces is reviewed. In recent years, experiments with single-crystal surfaces and well-ordered films have increased our understanding of the interaction of methane with solid surfaces. Late transition metals interact weakly with methane and elevated temperatures (>400 K) are necessary to enable a significant dissociation on the hydrocarbon. In contrast, an IrO2(110) surface dissociates methane at temperatures below 200 K. Cooperative interactions between O and Ir are responsible for the binding of methane and the breaking of a C–H bond. This type of cooperative interactions involving O and a metal cation have also been seen on Ni/CeO2(111) and Co/CeO2(111) surfaces which dissociate methane at room temperature. Experiments of AP-XPS and in situ TR-XRD have shown that the active phase of metal/oxide catalysts used for the dry-reforming of methane frequently is a dynamic entity which evolves when the reaction conditions change. The addition of water to a mixture of CH4/O2 shifts the selectivity towards methanol production on CeO2/CuOx/Cu(111) and Ni/CeO2(111) surfaces. Metal-support interactions and water site-blocking play a crucial role in the conversion of methane to methanol on these catalysts.
综述了甲烷在明确的金属氧化物表面上的活化和转化的原位研究。近年来,单晶表面和有序薄膜的实验增加了我们对甲烷与固体表面相互作用的认识。晚期过渡金属与甲烷的相互作用弱,需要升高温度(约400 K)才能使碳氢化合物发生明显的离解。相反,IrO2(110)表面在低于200 K的温度下解离甲烷。O和Ir之间的协同相互作用负责甲烷的结合和碳氢键的断裂。在室温下解离甲烷的Ni/CeO2(111)和Co/CeO2(111)表面也发现了O和金属阳离子的这种类型的协同相互作用。AP-XPS和原位TR-XRD实验表明,用于甲烷干重整的金属/氧化物催化剂的活性相往往是一个随反应条件变化而演化的动态实体。在CH4/O2混合物中加水使CeO2/CuOx/Cu(111)和Ni/CeO2(111)表面上的甲醇选择性发生变化。金属支撑相互作用和水的位置阻塞在这些催化剂上甲烷转化为甲醇的过程中起着至关重要的作用。
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引用次数: 1
Direct non-oxidative methane conversion in membrane reactor 膜反应器中直接非氧化甲烷转化
Q1 Materials Science Pub Date : 2019-02-12 DOI: 10.1039/9781788016971-00127
Su Cheun Oh, Mann Sakbodin, Dongxia Liu
Methane is an abundant fossil resource and the main constituent of natural gas and oil-associated gases. Innovation in methane conversion chemistry and technology is essential to provide value-added chemicals and fuels, which could be an alternative to petroleum. Direct non-oxidative methane conversion (DNMC) has been studied to produce C2 (e.g., acetylene, ethylene, ethane) and aromatics (e.g., benzene and naphthalene), when combined are referred to as C2+ hydrocarbons. However, thermodynamic constraint in DNMC leads to low methane conversion, low C2+ yield, and rapid catalyst deactivation by coke. Membrane reactors comprised of active DNMC catalysts and hydrogen-permeable membranes have the potential to alleviate the thermodynamic barriers and increase methane conversion. This chapter summarizes the past research and ongoing development on DNMC reaction in membrane reactors. The catalysts, membrane materials, reactor configurations and performance for DNMC in membrane reactors are discussed. The challenges, strategies to mitigate reactor deterioration during DNMC, as well as future research and development directions to advance this technology for one-step conversion of methane to C2+ hydrocarbon fuels and chemicals are presented.
甲烷是一种丰富的化石资源,是天然气和石油伴生气的主要成分。甲烷转化化学和技术的创新对于提供可替代石油的增值化学品和燃料至关重要。直接非氧化甲烷转化(DNMC)已被研究用于生产C2(如乙炔、乙烯、乙烷)和芳烃(如苯和萘),当结合时称为C2+碳氢化合物。然而,DNMC的热力学约束导致甲烷转化率低、C2+产率低、催化剂被焦炭失活快。由活性DNMC催化剂和透氢膜组成的膜反应器具有缓解热力学障碍和提高甲烷转化率的潜力。本章总结了膜反应器中DNMC反应的研究现状和发展趋势。讨论了膜反应器中DNMC的催化剂、膜材料、反应器结构和性能。提出了DNMC过程中面临的挑战、缓解反应器恶化的策略,以及推进该技术一步转化为C2+碳氢燃料和化学品的未来研究和发展方向。
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Catalysis Structure & Reactivity
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