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。

In deep learning field, the appropriate selection of constraints directly affects the learning efficiency and learning results of a network. Partial differential equations (PDEs) which are extremely accurate compared to the constraint methods employed in traditional neural networks are natural constraint models in complex physical fields. In this paper, based on this premise we propose a new method to solve complex physical field simulation problems. We approximate the variables in a complex physical field by building a feedforward deep neural network while applying the chain rule of calculus to encode the corresponding PDEs into the loss function to add constraints. It is worth noting that we have only used part of the equations of the physical process rather than all of them. In other words, instead of solving the equations we learn the whole physical process via the partial PDEs constraints and a few data points. We verify the effectiveness of the deep learning method via learning low-temperature plasma model that is composed of complex physical processes. This technique presents a paradigm for the simulation of complex physical field problems. © 2023, Beijing Paike Culture Commu. Co., Ltd.

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。

纳米金属氧化物的粒径对其性能有很大影响,而微波等离子体作为低温等离子体的一种,具有较多高能电子、离子和激发态自由基等高活性物种,以及独特的温度物理特性,有利于降低纳米金属氧化物粒径从而改善其性能,具有较高的研究价值。首先,设计并搭建了一台波导耦合型微波等离子体放电平台,基于发射光谱诊断法对微波等离子体的电气和物理参数进行了分析。研究发现:气体温度、电子温度随微波功率的升高而升高;当微波功率为480 W时,气体温度为1350 K,淬冷速率约为148 K/8),较高的淬冷速率有利于降低纳米金属氧化物的粒径。之后,使用微波等离子体放电平台制备了镍/二氧化铈纳米金属氧化物,探究了不同微波功率,元素不同配比对纳米金属氧化物的影响。结果表明:产物粒径随着微波功率的提高而降低,当微波功率为480 W时,粒径约为8.1 nm,约为浸渍法的三分之一,当镍铈元素物质的量比为1:20时,镍/二氧化铈纳米金属氧化物对甲烷干重整性能最优,并且温度活性测试和反应空速活性测试的性能均优于浸渍法制备镍/二氧化铈纳米金属氧化物（镍铈元素物质的量比为1:20）。最后,探究了不同溶剂对纳米金属氧化物性能的影响。分别以水、2-乙基己酸/乙醇为溶剂制备了不同元素物质的量比铁/二氧化铈纳米金属氧化物。相比于水,以2-乙基己酸/乙醇为溶剂使粒径进一步降低为6.3 nm,同时比表面积增大一倍。以2-乙基己酸/乙醇为溶剂能使纳米金属氧化物的合成路径由以液相途径为主转变为气相和液相两种途径,而气相途径更有利于降低纳米金属氧化物的粒径。另外,通过光谱分析得到,2-乙基己酸/乙醇的引入降低了氧自由基的含量,而在缺氧条件下,有利于四价铈离子向三价铈离子的转变,从而产生更多的氧空位。经过甲烷无氧转化测试发现:在相同元素物质的量比、反应空速的条件下,以2-乙基己酸/乙醇为溶剂制备的铁/二氧化铈纳米金属氧化物的活性高于以水为溶剂制备的铁/二氧化铈纳米金属氧化物。本文设计并搭建的微波等离子体放电平台,能够较为快速、便捷的制备单组份或多组份的纳米金属氧化物,所得产物具有一定的实际应用价值,该工艺为等离子体材料制备领域提供了一种新思路。