NSERC-DFG SUSTAIN: Plasma-electrification of chemical produce – towards a green circular industry with net-zero carbon output and sustainable processing (PLANET)

PLANET确定了一种基于非热等离子体的分子解离的新方法，作为减少温室气体排放和大气中二氧化碳含量的一种手段。目的是为气候危机找到创新的解决方案。通过操纵振动激发，我们将CO2分解为氧气（O2）和一氧化碳（CO），其可以进一步用于例如，生产燃料以达到净零碳排放。振动激发到分子解离点-称为振动爬梯-是有效的等离子体解离CO2的关键。振动爬梯通过与低能电子的碰撞而最大化。我们使用一种新的基于时间的电子能量控制来产生这些电子。由于所需的电场太低，无法在大气压下维持等离子体，PLANET的方法是使用电压波形剪裁（VWT）和高压ns脉冲的组合。脉冲实现击穿和VWT允许我们控制非热能量转移到电子在时域和维持放电的电场足够低，以选择性地激发振动分布。使用互补的混合模拟和新的实验超快诊断方法，观察非绝热时间尺度上的激发和去激发，我们将获得必要的洞察基本等离子体化学。基于等离子体的CO2重整在PLANET中解决的三个主要研究挑战是：i）超越最先进的电场剪裁，ii）通过开发新的混合方法来模拟复杂的等离子体化学，iii）通过使用中红外超快光谱解决振动能态的非绝热动力学来分析CO2解离途径。

PLANET identifies a novel approach for non-thermal plasma-based dissociation of molecules as a means to reduce greenhouse gas emissions as well as CO2 content in the atmosphere. The aim is to find innovative solutions for the climate crisis. Via steered vibrational excitation we will split CO2 into oxygen (O2) and carbon monoxide (CO), which can be further used to e.g., produce fuels to reach net-zero carbon output. Vibrational excitation up to the point of molecule dissociation - known as vibrational ladder climbing - is key to efficient plasma-based dissociation of CO2. Vibrational ladder climbing is maximized by collisions with low-energy electrons. We use a novel time-based control of the electron energy to generate these electrons. Since the required electric fields are too low to sustain a plasma at atmospheric pressure, PLANET’s approach is to use a combination of voltage waveform tailoring (VWT) and high voltage ns-pulses. The pulses achieve breakdown and VWT allows us to control the non-thermal energy-transfer to the electrons in the time domain and to sustain the discharge with an electric field low enough to selectively excite the vibrational distribution. Using complementary hybrid simulation and novel experimental ultrafast diagnostic methods that observe the excitation and de-excitation on a non-adiabatic timescale, we will gain the necessary insight into the fundamental plasma chemistry. The three major research challenges of plasma-based CO2 reforming addressed in PLANET are i) to move beyond state-of-the-art in electric field tailoring, ii) to model the complex plasma chemistry by developing new hybrid approaches, and iii) to analyze the CO2 dissociation pathways, by resolving the non-adiabatic dynamics of the population of the vibrational energy states with mid-IR ultrafast spectroscopy.