提高Mn系低温脱硝催化剂抗硫抗水性能的国内外研究概述

介绍了氮氧化物的来源、SCR脱硝的反应机理和工艺流程、催化剂的硫和水中毒机理,重点介绍了国内外学术和工业界为提高催化剂抗硫和抗水性能所做的研究和尝试,旨在推动低温SCR技术的进展,促进该技术早日实现在工业上的大规模应用。     

Ni、Zn改性Cu/水泥催化剂及其甲醇高温裂解性能

以碱式碳酸镍、碱式碳酸锌、碱式碳酸铜和水泥为原料制备水泥负载的Cu-Ni，Cu-Zn，Cu-Ni-Zn催化剂，考察了合成催化剂的甲醇裂解反应性能。结果表明：在常压、质量空速为3.39 h-1、温度为380~420 ℃的条件下，Cu-Ni/水泥催化剂作用下的甲醇转化率均在96%以上；Cu-Zn/水泥催化剂作用下的甲醇转化率较低，但对H2和CO选择性较高；Cu-Ni-Zn/水泥催化剂经1 600 h运转，甲醇转化率和产物分布变化不大，甲醇转化率基本维持在81%以上，(H2+CO)摩尔分数大于98%，说明Cu-Ni-Zn/水泥催化剂具有良好的高温稳定性。     

Catalytic combustion of methane over a highly active and stable NiO/CeO2 catalyst

In the last decades, many reports dealing with technology for the catalytic combustion of methane (CH₄) have been published. Recently, attention has increasingly focused on the synthesis and catalytic activity of nickel oxides. In this paper, a NiO/CeO₂ catalyst with high catalytic performance in methane combustion was synthesized via a facile impregnation method, and its catalytic activity, stability, and water-resistance during CH₄ combustion were investigated. X-ray diffraction, low-temperature N₂ adsorption, thermogravimetric analysis, Fourier transform infrared spectroscopy, hydrogen temperature programmed reduction, methane temperature programmed surface reaction, Raman spectroscopy, electron paramagnetic resonance, and transmission electron microscope characterization of the catalyst were conducted to determine the origin of its high catalytic activity and stability in detail. The incorporation of NiO was found to enhance the concentration of oxygen vacancies, as well as the activity and amount of surface oxygen. As a result, the mobility of bulk oxygen in CeO₂ was increased. The presence of CeO₂ prevented the aggregation of NiO, enhanced reduction by NiO, and provided more oxygen species for the combustion of CH₄. The results of a kinetics study indicated that the reaction order was about 1.07 for CH₄ and about 0.10 for O₂ over the NiO/CeO₂ catalyst.     

Controllable Fe/HCS catalysts in the Fischer-Tropsch synthesis: Effects of crystallization time

The Fischer–Tropsch synthesis (FTS) continues to be an attractive alternative for producing a broad range of fuels and chemicals through the conversion of syngas (H₂ and CO), which can be derived from various sources, such as coal, natural gas, and biomass. Among iron carbides, Fe₂C, as an active phase, has barely been studied due to its thermodynamic instability. Here, we fabricated a series of Fe₂C embedded in hollow carbon sphere (HCS) catalysts. By varying the crystallization time, the shell thickness of the HCS was manipulated, which significantly influenced the catalytic performance in the FTS. To investigate the relationship between the geometric structure of the HCS and the physic-chemical properties of Fe species, transmission electron microscopy, X-ray diffraction, N₂ physical adsorption, X-ray photoelectron spectroscopy, hydrogen temperature-programmed reduction, Raman spectroscopy, and Mössbauer spectroscopy techniques were employed to characterize the catalysts before and after the reaction. Evidently, a suitable thickness of the carbon layer was beneficial for enhancing the catalytic activity in the FTS due to its high porosity, appropriate electronic environment, and relatively high Fe₂C content.     

中空碳基材料在电解水中的研究进展

氢能所具有的清洁、高能量密度特点，使其成为一种未来的理想能源。相较于石油、天然气等的热解制氢技术，利用可再生清洁能源进行电催化分解水制氢具有高效和清洁无污染的特点，且获得氢气产物纯度高，具备大规模发展的潜力。而在大规模水电解过程中，电催化剂是不可或缺的元素之一。它能有效地加速电解水在阴阳两极反应的动力学过程。传统的贵金属基催化剂具有良好的电催化析氢、析氧活性，但成本高昂、储量稀缺，从而限制了其规模化地推广及应用。开发新型高效廉价的非贵金属基电催化剂已成为时下研究热点。中空碳基纳米材料集成了中空材料和碳基材料的优势，作为电催化剂，在电解水方面有着潜在的应用价值。本文总结了近年来微纳米结构碳基中空材料作为新型电解水催化剂的研究进展，介绍了高效碳基中空析氧/析氢催化剂的设计原则和相应的设计策略，并对开发持久高效的中空碳基电解水催化剂进行了总结和展望。     

Selective Hydrogenation of Biomass-Derived Succinic Acid: Reaction Network and Kinetics

The conversion of bio-based succinic acid (SA) to the value-added chemicals 1,4-butanediol (BDO), γ-butyrolactone (GBL), and tetrahydrofuran (THF) can replace the corresponding petrochemical production routes to achieve a sustainable process. The reaction network for aqueous-phase catalytic hydrogenation of succinic acid over a supported Re-Pd catalyst was identified and the reaction kinetics was determined. With the developed kinetic model, the composition of the product mixture regarding the desired products (BDO, GBL, THF) can be described as a function of educt concentration, temperature, and pressure. The maximum BDO yield was achieved at high pressure and low temperature, while low pressure and high temperature favored GBL and THF production.     

缓冲溶液法制备高效的铁基类芬顿催化剂

负载型金属催化剂在水处理中起着重要的作用，浸渍法是制备负载型催化剂的重要方法。为了克服传统浸渍方法的缺点，本文通过使用甘氨酸/盐酸作为缓冲溶液，严格控制pH，获得高分散的活性组分并以此方法制备了铁基类芬顿催化剂。对苯酚催化降解的实验表明，使用缓冲溶液法制备的催化剂比未使用的样品可以更高效地去除苯酚，1h内对苯酚的降解可达89.3%。此外，通过调节浸渍温度、浸渍时间和缓冲溶液的pH等参数来精确控制活性组分的量和催化活性。更重要的是，此催化剂制备方法可以用于其他负载型金属催化剂的制备，比如过硫酸盐催化剂，并取得了良好的催化效果。     

氧化钨（WO3）薄膜光电催化性能的改善及应用

半导体WO₃具有较小的禁带宽度和良好的稳定性，对可见光具有较强的吸收，在光催化和光电催化领域具有广泛的用途。然而，单一WO₃薄膜仍然存在着光生电子-空穴复合率高、光电催化活性与能量转换效率偏低等问题。本文从WO₃薄膜光电催化性能的改善及应用两个方面对近年来的研究进行了综述。在WO₃薄膜光电催化性能的改善方面，分别从有序纳米结构的构建、离子掺杂与表面修饰进行总结。同时，也归纳总结了WO₃薄膜作为光电极在分解水制氢、光电催化还原CO₂和降解有机污染物等方面的应用，并提出了WO₃薄膜在光电催化过程中存在的问题，指出WO₃有序纳米异质结的构建是提高WO₃薄膜光电催化活性的有效方法。WO₃薄膜光电极的规模制备、廉价助催化剂的使用、光电极的稳定性与耐蚀性是其实际应用过程中需要解决的问题。