高通量筛选技术在多相催化研究中的应用

通过对组合催化研究的关键因素－－催化剂高通量筛选技术的评价分析认为：在对已有的催化体系和催化剂优化的同时，如何高校研制开发新筛选检测技术，诸如反应器设计和检测器的选择，是组合催化研究的主导思想，对此的深刻理解和运用将增强实验室的创新能力。     

废弃制冷剂降解方法研究现状及思考

部分人工合成制冷剂由于存在环保问题,目前正按照环保公约进行淘汰。淘汰后的废弃制冷剂需要进行降解销毁,我国是目前国际上主要的制冷剂生产和消费国,因此面临着巨大的废弃制冷剂销毁压力。总结归纳了废弃制冷剂目前主要的降解方法,包括焚烧热解法、等离子法、催化分解法等技术路线的研究进展,并对未来可能的发展方向进行思考与讨论。     

三维金属纳米花的合成和应用研究现状

三维金属纳米花有一系列优越的理化性能,由于结构特异,在催化、传感上应用广泛,还可以用于制作微观尺度的器件,引起了人们极大的兴趣。从选择性刻蚀、模板引导、种子生长法和动力学控制等方面,介绍了近期在三维金属纳米花合成领域取得的进展,并简述了这种纳米粒子在催化以及电催化方面的应用。     

New frontiers in X-ray spectroscopy in heterogeneous catalysis: Using Fe/ZSM-5 as test-system

We have applied a number of novel X-ray spectroscopic tools to Fe/ZSM-5 systems. Fe/ZSM-5 can be considered as an ideal test-system for the characterization techniques in heterogeneous catalysis. The existence of a large range of sites and structures creates a good testing ground to determine which experimental tools are able to resolve such complex system. In situ soft X-ray absorption provides important information on the valence and electronic structure of iron during treatments, with a time scale down to 30 s. Kβ-detected XANES yields unprecedented resolution for pre-edge structures and using hard X-rays can be used under any condition and treatment, including high-pressures. It can be expected that both in situ soft X-ray absorption and Kβ-detected XANES become ‘standard’ tools for catalysis research, similar to traditional XANES and EXAFS today. The X-MCD is also used in this paper but it will probably remain a rather specialized technique in the field of heterogeneous catalysis. Further new developments for catalysis characterization are for all to be expected from X-ray spectro-microscopy, where one will have the possibility to perform the in situ soft X-ray absorption and Kβ-detected XANES experiments with nanometer size spatial resolution.     

Catalysis, the turntable for a clean future

Upgrading the bottom of the barrel for clean fuel production, developing new engines with optimized catalytic posttreatments, implementing clean catalytic combustion technologies, improving the overall CO₂ balance via catalytic processes and, lastly, developing new water purification techniques represent major upheavals in catalysis linked to refining and environmental protection. This paper, thus, will focus on the determining contribution of catalysis to the most recent achievements in these domains. A technico-economic approach will follow, underlining their main incentives and drawbacks within the framework of future environmental constraints.     

甘油催化氧化合成二羟基丙酮研究进展

对甘油选择性催化氧化转化为二羟基丙酮的研究进行综述,介绍了负载型催化剂在不同条件下对产物选择性和反应物转化率的影响,以及催化剂的作用机理。阐述了甘油催化氧化存在的问题以及发展前景。从均相到非均相催化,从单金属到双金属负载催化,从金属到非金属催化,甘油氧化反应的研究不断在完善。研究发现用Bi改性的Pt负载催化剂可以有效地将甘油选择性催化氧化为二羟基丙酮,在最优条件下,可获得较高的甘油转化率和二羟基丙酮选择性,但催化剂稳定性较差,有待进一步提高。杂多酸催化剂以及非金属催化剂也存在稳定性差的问题。指出改善催化剂的稳定性将是未来研究的主要方向。     

酯化用固体超强酸催化剂研究进展

介绍了MxOy/So4^2-型固体超强酸的制备条件对催化剂性能的影响及在酯化反应中的催化作用，分析了催化酯化反应的优点及存在的问题，指出复合型超强酸将是以后研究的重点。     

开发石油化工催化新技术的一些科研领域

催化发明创造的历史经验告诉我们:新催化材料的开拓是创造发明新催化剂的源泉,这种新催化剂的发现往往是开发新催化工艺的基础。膜分离是正在大力开发的新技术。膜分离与催化相结合形成了膜反应器催化的新研究领域,这为发明新催化过程开辟了新机会。近年来均相催化的进展拓宽了工艺化学的地平线,这看来是将来会取得最大进展的领域。因此,为了发明创造石油炼制和石油化工新催化剂和新催化工艺,必须大力加强新催化材料、膜反应器催化和均相催化三个领域的开拓性探索和导向性基础研究。     

低毒金属配合物催化丙交酯开环聚合研究进展

可生物降解材料聚丙交酯主要通过丙交酯开环聚合反应制备,金属配合物催化剂由于具有结构易调变、催化活性高和立体选择性等优点,成为丙交酯开环聚合反应中应用最多的催化剂。近年来,低毒金属配合物催化剂引起了人们的极大关注。本文详细评述了低毒锂、钠、钾、钙、镁和锌配合物催化剂的最新研究进展,重点阐述了配体类型、配体上不同取代基的结构、电子效应对催化剂催化性能的影响,分析了溶剂对配合物在溶液中的状态以及对单体的配位、插入和聚合反应的影响。本文还对该领域发展趋势进行了展望,随着对低毒金属配合物催化丙交酯开环聚合机理研究的深入,未来将从配体结构设计出发,开发催化活性更高、性能更好的配合物催化剂,进而制得高质量的聚丙交酯。     

双季戊四醇合成工艺研究进展

介绍了双季戊四醇(双季)合成工艺的研究现状。阐述了由单季戊四醇(单季)生产中副产双季,以单季为原料在酸催化下分子间脱水、或基于与尿素／碳酰胺反应、或经过单季偏酯、或采用3,3-二羟甲基氧杂环丁烷和赤藓(糖)醇为起始原料制取双季的工艺过程及新技术,指出在生产单季中副产双季是双季的主要获取途径,提高副产双季的收率及单、双季分离条件是今后的主要研究方向。     

铑催化高碳烯烃氢甲酰化合成高碳醇进展

介绍了近年来铑／膦催化高碳烯烃氢甲酰化的研究和开发进展。特别是以ＴＰＰＯ／Ｒｈ为催化剂的Ｍｉｔｓｕｂｉｓｈｉ Ｋａｓｅｉ工艺和水／有机两相为主的各种两相催化技术。近年的进展表明,通过创新膦配体以及采用两相催化体系,有望使更有效,更经济的铑催化工艺在高碳烯烃氢甲酰化的应用中取得突破。     

Systematic Investigations of Vibrational and Fluid-Mechanical Stability of Coated Monolithic Catalysts

Heterogeneous catalysts usually consist of porous, inorganic materials. Especially in the mobile application, e.g., in exhaust gas catalysis as a part of the gas line of an engine, there are loads due to vibrations and high gas velocities. It can be assumed that physical stress will lead to a loss of the catalytically active coating. The present contribution describes experimental setups and methods for a systematic and reproducible investigation of the main influences to the mass loss due to vibrational and fluid-mechanical stress caused by particle-free gas flows.     

Synthesis and Catalysis in China

In 2000 China ranked 5^th in the world (7.9%) in the publication of SCI papers on organic synthesis and catalysis; by 2008 China had become 1^st (21.6%), followed by the USA, Germany and Japan. Major contributions made by Chinese research groups in the last decade in the areas of total synthesis of complex natural products, cross‐coupling, asymmetric catalysis, and heterogeneous catalysis are highlighted. The output and quality of the research on synthesis and catalysis from China continue to increase, so that with the rapid development of China’s economy, Chinese chemists will make greater contributions to organic synthesis and catalysis in the future.     

Development of Time-Resolved XAFS Instrumentation for Quick EXAFS and Energy-Dispersive EXAFS Measurements on Catalyst Systems

From its very earliest days, at which time measuring a spectrum took at least 1 h, XAFS has been used for catalysis studies. In more recent times technological advances have improved the time resolution to minutes and seconds with quick EXAFS, and subsecond to millisecond with energy-dispersive EXAFS. This paper describes the instrumentation necessary and elucidates with specific examples where this has been used. In particular the Daresbury QEXAFS monochromator will be shown and several examples of combined XAFS and diffraction, a powerful technique for in situ studies. The development of energy dispersive EXAFS at Daresbury will be described. Recent results on in situ Rh catalysis combining EDE and mass spec measurements at the ESRF are highlighted, and finally the details of the latest microstrip detector that will enable continuous measurements at 10 s time intervals is presented.     

When NHC Ligands Make a Difference in Gold Catalysis

Thanks to their unique electronic and steric properties, carbene ligands offer highly valuable features for catalysis, including homogenous gold catalysis. The use of carbene-gold complexes has improved existing reactions, either by modifying reactivity modes or by leading to highly asymmetric processes. These topics will be discussed on the basis of selected examples.     

焦炉气制甲醇方案的比较与选择

对催化纯氧转化和无催化纯氧转化2种以焦炉气转化制甲醇合成气的方法从工艺流程、过程特点、关键技术和主要设备等方面进行了阐述和比较,结果表明,目前应先选用催化纯氧转化法,待烧嘴问题解决后,则应优先选用无催化纯氧转化制甲醇合成气。     

New Paradigms and Future Critical Directions in Heterogeneous Catalysis and Multifunctional Reactors

Heterogeneous catalysis is a key pillar of the global industrial chemical and petrochemical sector, and 85% of all chemical products are produced with at least one catalytic step. Indeed, catalysis and catalytic reactors are a critical underpinning science for energy, environmental, and economic security. This paper reviews some future critical directions for research in catalysis science, toward a greener and more sustainable future. We believe that even a relatively mature field as heterogeneous catalysis and nanomaterials can be vitalized and spurred by major discoveries, but an outside-the-box thinking and a focused effort in a large plurality of disciplines is necessary. Thus, critical research needs in several areas, including heterogeneous and homogeneous catalysis, biocatalysis, photocatalysis, electrochemical conversions, and computational catalysis, are reviewed. The research needs of the future lie at the intersection of synthesis of novel nanostructured materials with tunable pore size distribution, controlled porosity, and high surface area; development of new catalytic applications for such materials; and the science of advanced characterization including in situ spatiotemporal analysis. In the area of computational catalysis, we believe that the future lies in the development of hybrid methods (parallel and serial) which can model the typical multiscale phenomena that are typically encountered in protein translocation and signal transduction, charge transport, enzymatic catalysis, surface chemistry, and self-assembly in complex fluids. As we promulgate the new directions to the catalysis fraternity, some prior research areas will unfortunately need to be relegated to obsolescence, to maintain a healthy balance on the research forefront.     

Surface Science Studies on the Zirconia-Based Model Catalysts

Zirconia possesses ideal chemical and mechanical stability properties. It has been widely used in many technical applications such as gas sensors, protective coatings and heterogeneous catalysis. In particular, in heterogeneous catalysis, zirconia has been used in many catalytic reactions not only as the metal catalysts’ support but also as the pure catalyst; it can be also used as an additive to improve the catalytic performances of the catalysts. To gain fundamental understanding of the roles that zirconia plays in catalysis, significant surface science studies based on zirconia model catalysts have been performed. In this paper, we will present a short review of recent surface science studies on the zirconia-based model catalysts. These model catalysts include single crystalline yttria-stabilized zirconia surfaces, zirconia thin films which were grown on metal single crystal surfaces and zirconia-supported metal catalysts. Besides the focuses on the surface chemistry of model zirconia surfaces, the surface structures and adsorption/reaction properties of the zirconia-supported metal catalysts will be also addressed.