开发非合成气路线的 CH-CHOH 直接制取高碳液态化学品转化技术可有效规避传统工业中面临的高危反应条件、废水排放、原子经济性低等问题。该文以 CH、CHOH 为原料,采用纳秒脉冲放电等离子体驱动 CH-CHOH 直接合成 C-C液态产品,主要探究

随着全球石油资源重质化程度不断加深，常规石油加氢工艺正面临愈发严重的挑战。低温等离子体技术为缓解加氢工艺中高温、高压、催化剂失活等难题提供了新思路。选择1-甲基萘作为重质油模型化合物，在无催化剂的温和条件下研究脉冲介质阻挡放电等离子体加氢的转化规律和反应机理。结果表明：甲基萘在氢气等离子体中容易发生饱和加氢反应，而在甲烷等离子体中则更易发生不饱和加氢反应；增大脉冲电压与脉冲重复频率有利于等离子体甲基萘加氢，但过高会导致加氢反应向裂解反应转变。获得了等离子体甲基萘加氢反应的发射光谱和Hα谱线演化过程，估算气体温度约为350 K,结合密度泛函计算结果推测等离子体甲基萘加氢是H自由基引发的芳香环逐步加氢反应。研究结果为后续等离子体加氢研究提供了参考。

随着全球石油资源重质化程度不断加深，常规石油加氢工艺正面临愈发严重的挑战。低温等离子体技术为缓解加氢工艺中高温、高压、催化剂失活等难题提供了新思路。选择1-甲基萘作为重质油模型化合物，在无催化剂的温和条件下研究脉冲介质阻挡放电等离子体加氢的转化规律和反应机理。结果表明：甲基萘在氢气等离子体中容易发生饱和加氢反应，而在甲烷等离子体中则更易发生不饱和加氢反应；增大脉冲电压与脉冲重复频率有利于等离子体甲基萘加氢，但过高会导致加氢反应向裂解反应转变。获得了等离子体甲基萘加氢反应的发射光谱和Hα谱线演化过程，估算气体温度约为350 K,结合密度泛函计算结果推测等离子体甲基萘加氢是H自由基引发的芳香环逐步加氢反应。研究结果为后续等离子体加氢研究提供了参考。

Non-thermal plasma is promising for cracking the abundant but low-quality heavy oil into value-add chemicals due to its wide feedstock adaptability and high conversion rate. In this work, heavy oil cracking characteristics by microsecond pulsed spark discharge plasma were investigated in terms of pulse voltage, pulse repetition fre-quency and discharge power. Experiment results indicate pulse voltage and pulse repetition frequency are the main factors to control product yields and distribution. Pulse voltage determines single pulse energy and in-fluences discharge stability and gas temperature. Pulse repetition frequency determines discharge intervals and affects collision reactions and quenching process. The maximum heavy oil conversion rate was 50.4% and the mass yields of H-2 and C2H2 were 3.3% and 19.7% with 10.1 W discharge power, and H-2 and C2H2 production energy consumption were 25.2 kW.h/m(3)H(2) and 55.4 kW.h/m(3)C(2)H(2). Compared with thermal plasma, heavy oil conversion rate of this work increased 12% with above 95% reduction in discharge power, and this work has a significant advantage in H-2 and C2H2 production energy consumption. Carbon nanomaterials composed of carbon nanoflakes and nanoparticles can be obtained while producing H-2 and C2H2. Especially, there were few-layers graphene nanoflakes (GNFs) in the carbon nanomaterials, which realized the full utilization of heavy oil. The possible reaction mechanism of heavy oil cracking was discussed using saturates-nucleating-aromatics-flaking theory. This work provides an effective COx-free method for one-step production of H-2, C2H2 and car -bon nanomaterials, which has wide application prospects for heavy oil utilization.

Hydrogenation of aromatic compounds is an important reaction in the petrochemical, pharmaceutical, and organic industries. In this paper, we report a novel catalyst-free hydrogenation process that converted gaseous toluene into methyl-cyclohexane at ambient pressure and room temperature using microsecond pulsed dielectric barrier discharge (DBD). The hydrogenation performance of the toluene was investigated in terms of the pulse repetition frequency, reactor temperature, and toluene concentration. The experiments show that the toluene was easily hydrogenated to methyl-cyclohexane by the H2 DBD plasma, in which higher PRF, lower reactor temperature and higher H2 concentration were favorable for the production of methyl-cyclohexane. The highest molar fraction of the methyl-cyclohexane was 80.1% with energy consumption of 0.12 kW∙h/mmol. Controlled experiments with Ar atmosphere or different feedstocks (d-toluene, methyl-cyclohexadiene and methyl-cyclohexene) indicate that the H radicals from the H2 DBD plasma realize the toluene hydrogenation. The possible reaction mechanism of the plasma-enabled hydrogenation was discussed via the optical emission spectroscopy (OES), density functional theory (DFT) and molecular dynamic simulations, which confirms that the H radicals produced by the electron-impact reactions induce the step-by-step hydrogenation reaction of the toluene. Overall, this work provides not only new insights into the plasma-enabled hydrogenation reaction, but also a potentially effective catalyst-free method for hydrogenation applications. © 2023 Elsevier B.V.

随着原油重质化和劣质化程度的加深以及环保法规的日益严格，加氢脱硫成为获得清洁燃料油的重要手段，催化剂是加氢脱硫技术的核心。针对现有加氢脱硫催化剂制备路线存在的硫化不充分、开工周期长、环境不友好、制备路线繁琐等不足，提出开发兼顾低成本、高活性和环境友好三方面的催化剂制备路线，即以 MoS2直接制备加氢脱硫催化剂。对 MoS2和纳米 MoS2的制备以及 MoS2直接制备加氢脱硫催化剂的研究现状进行了综述，并对该制备路线的研究方向进行了展望。

采用XRD、TEM、XPS以及CO红外吸附等手段，系统研究了Fe、Co和Mo对Ni 2 P电子结构的影响及其对4，6-DMDBT加氢脱硫（HDS）性能的影响。表征结果表明，3种掺杂金属可较好地调整Ni 2 P位点的电子状态，影响含硫有机化合物在Ni 2 P位点上的吸附能。HDS性能评价结果发现，HDS本征活性与Ni 2 P位点的电子结构之间存在火山型关系，使得具有中等电子密度的C O -Ni 2 P/SiO 2 因适中的吸附能呈现出最佳的HDS活性。此外，Ni 2 P的电子缺陷显著促进直接脱硫（DDS）选择性。与Ni 2 P/SiO 2 相比，Mo-Ni 2 P/SiO 2 中Ni 2 P具有更多的电子缺陷，展现出更高的DDS选择性，而Fe-Ni 2 P/SiO 2 和Co-Ni 2 P/SiO 2 中Ni 2 P因具有更高的电子密度，其DDS选择性更低。

Dry reforming of CH4 process can convert greenhouse gases into high-value-added fuels and chemicals with its broad application prospects in environmental protection and renewable energy. Non-thermal plasma is considered an effective alternative method because it can activate CH4 and CO2 under low temperature and atmospheric pressure. This paper is aimed to optimize the plasma-assisted dry reforming of CH4 process in a unipolar microsecond pulsed coaxial dielectric barrier discharge by investigating the effects of reactor structures. The results show that the conversions of reactants and the yields of syngas were significantly affected by the reactor structures. Specifically, a multi-stage or foil external electrode and negative polar discharge could promote CH4 and CO2 conversions, gas product yields, and energy conversion efficiencies. For different electrodes, the maximal conversions of CH4 and CO2 were 20.4% and 14.1%, with an energy conversion efficiency of 4.4% under our experimental conditions. Higher conversions, yields, and energy conversion efficiencies were obtained with lower power input when applying heat insulation measures. CH4 conversion was promoted to 27.9% with a moderate energy conversion efficiency of 3.8%, but the conversion of CO2 was only 12% when packing materials into the reactor. The results can provide specific guidance for designing plasma or plasma-catalytic dry reforming reactor.