天然气在能源结构中占据着不可或缺的地位，高含硫天然气田的安全稳定开采对我国“川气东送”工程具有重大意义。而高含硫天然气中硫化氢具有强腐蚀性，易引发天然气集输管道腐蚀，从而造成大范围硫化氢泄漏中毒事故的发生。高含硫天然气是一种典型的混合气体，其泄漏影响范围受到环境与自身浓度配比等多种条件的共同作用，导致泄漏影响范围难以快速划分，进而影响气体泄漏后的应急救援工作开展，且现有点式监测与阈值安全预警方法难以对高含硫气田进行全域、全过程泄漏的动态监测预警。因此，本文开展了高含硫天然气中甲烷与硫化氢混合气体的中红外激光器同步监测技术研究，以高含硫天然气泄漏监测为入手，通过模拟高含硫天然气泄漏射流与扩散实验、高含硫天然气分子间与大尺度数值模拟仿真，揭示了高含硫天然气的泄漏扩散机理，进而开展高含硫天然气泄漏危险区域动态预警方法研究。论文主要研究成果如下：

（1）高含硫天然气中甲烷与硫化氢混合气体的中红外激光同步监测技术。基于硫化氢的谱线展宽与吸收线型，确定了高含硫天然气集输管道泄漏场景下气体的一般谱线展宽形式，结合硫化氢气体在中红外波段的基频振动跃迁带分布特征，选定8.309μm为中红外激光器的中心波段，搭建了中红外遥测式激光监测系统的光学与电学结构，实现了光路上特征气体浓度变化的动态感知。针对中红外激光系统测量特征气体浓度时二次谐波存在的整流效应、纹波以及噪声信号等干扰，提出了EMD-SG信号滤波方法，能够去除二次谐波中存在的干扰噪声。针对系统监测时硫化氢与甲烷气体的特征曲线相互干扰问题，提出了混叠谐波曲线的信号解耦方法，并建立了混合气体浓度反演模型，形成了中红外激光遥测系统，可对光路上的甲烷与硫化氢气体浓度进行实时遥测。

（2）通过纹影与自研高含硫天然气泄漏实验台分析泄漏气体在射流与扩散阶段的运移规律。基于对高含硫天然气集输管道泄漏事故的统计，明确了高含硫天然气集输管道泄漏扩散的主要因素。基于泄漏射流的纹影实验表明，泄漏气体受到流速的影响，会呈现出典型的涡流现象；且在泄漏过程中随着气体的射流动能逐渐降低，重力与自身气体成分逐渐成为驱动泄漏气体运移的主要因素，从而导致泄漏气体出现过渡动能平衡与羽流扩散现象；泄漏气体射流距离与气体中硫化氢浓度、流速呈正相关，与泄漏孔径呈负相关。基于泄漏扩散的热成像与中红外激光实验表明，泄漏气体在扩散过程中会呈现出浓度配比不变、浓度逐渐降低的整体运动与稀释现象；且泄漏气体在环境风速的影响下，自身硫化氢含量、环境风速与泄漏气体截距呈线性相关，而与泄漏孔径与流量呈波动相关，实验结果揭示了高含硫天然气的泄漏射流-扩散规律。

（3）通过MS分子仿真与FLACS大尺度高含硫天然气泄漏仿真实验，共同揭示高含硫天然气泄漏扩散机理。基于硫化氢与甲烷分子仿真实验表明，甲烷与硫化氢混合气体由于范德华力与分压的影响，相比单个气体具有更快的扩散速率；且甲烷与硫化氢受范德华力影响，在分子间距4Å位置处存在一个RDF特征峰；混合气体的扩散系数与温度呈正比，与压力呈反比关系，与硫化氢浓度则呈现出具有两个分压与范德华力动态平衡点的波动关系。基于大尺度高含硫天然气泄漏仿真实验表明，硫化氢浓度在泄漏射流与垂直方向影响范围呈负相关、在横向截距上呈现出与分子仿真相同的波动变化；环境风速对泄漏垂直与横向截距方向影响范围呈负相关、而在射流方向呈正相关；结合模拟实验结果，泄漏孔径与管内压力对泄漏影响范围呈波动上升的关系；环境温度对泄漏扩散范围呈正相关，结合实验模拟结果，有效揭示了高含硫天然气泄漏扩散机理。

（4）高含硫天然气集输管道气体泄漏危险区域动态预警方法研究。根据国家相关行业标准，按高含硫天然气中硫化氢预警浓度将泄漏气体范围划分为四个等级，建立了高含硫天然气集输管道气体泄漏安全评价体系。结合上述泄漏模拟与仿真实验结果，针对高含硫天然气泄漏数据量少的问题，提出了改进GAN网络结构，用于高含硫天然气泄漏数据扩充，并建立泄漏数据集。提出GWO-双层GRNN-ANN网路结构，建立硫化氢预警浓度与高含硫天然气最远泄漏扩散距离之间的非线性映射关系，得到高含硫天然气集输管道泄漏距离的耦合模型，利用不同泄漏时刻关键硫化氢浓度下耦合模型输出的最远距离值优化高斯扩散模型，得到高含硫天然气集输管道泄漏危险区域的动态三维预警模型。最终在以西南某气田为假定泄漏场景，可视化展示了该动态预警模型的安全预警范围与系统运行结果。

本研究研制了适用于大范围混合气体监测的中红外遥测式激光器，阐明了高含硫天然气泄漏射流-扩散规律，揭示了高含硫天然气集输管道气体泄漏机理，并提出泄漏危险区域动态三维预警模型，结果具有良好的可视化监测预警效果。对高含硫天然气集输管道泄漏动态监测预警效率的提升，具有重要的意义与作用。

Natural gas occupies an indispensable position in the energy structure, and the safe and stable exploitation of high-sulfur natural gas fields is of great significance for China's "Natural Gas Transmission from Sichuan to East China" project. However, the presence of hydrogen sulfide (H2S) in high-sulfur natural gas exhibits strong corrosive properties, which can easily lead to the corrosion of natural gas gathering and transmission pipelines, resulting in large-scale hydrogen sulfide leakage and poisoning accidents. High-sulfur natural gas is a typical mixed gas, and the influence range of its leakage is affected by various conditions, including environmental factors and its own concentration ratios. Additionally, existing point monitoring and threshold safety warning methods struggle to perform dynamic monitoring and early warning for leakage risks in high-sulfur gas fields across the entire domain and throughout the process. Consequently, this study focuses on the development of a mid-infrared laser synchronous monitoring device and methodology for methane and hydrogen sulfide mixed gas in high-sulfur natural gas. By simulating leakage jets and diffusion experiments, along with large-scale numerical simulations of high-sulfur natural gas molecules, the leakage diffusion mechanism of high-sulfur natural gas is elucidated, further leading to research on dynamic warning methods for hazardous leakage zones of high-sulfur natural gas. The main research outcomes are as follows:

(1) Synchronous monitoring device and method for mixed gases based on mid-infrared laser technology. Through the analysis of the spectral broadening and absorption line profiles of hydrogen sulfide, the typical spectral broadening pattern for gases in leakage scenarios of high-sulfur natural gas pipelines was established. By combining the distribution characteristics of the fundamental vibrational transition bands of hydrogen sulfide in the mid-infrared range, a central wavelength of 8.309 μm was selected for the mid-infrared laser. An optical and electrical structure of a mid-infrared remote sensing laser system was constructed to achieve dynamic sensing of characteristic gas concentration changes along the optical path. To address interferences such as rectifying effects, ripples, and noise signals during measurements of characteristic gas concentrations, an EMD-SG signal filtering approach was proposed to effectively eliminate unwanted noise in the second harmonic. A signal decoupling method was developed to overcome the interference problem stemming from overlapping characteristic curves of hydrogen sulfide and methane during system monitoring, resulting in the establishment of a mixed gas concentration inversion model. Formation of a mid-infrared laser telemetry system for real-time monitoring of methane and hydrogen sulphide.

(2) Analysis of gas leakage behavior during the jetting and diffusion phases using a self-developed high-sulfur natural gas leakage experimental platform. Based on statistical analysis of high-sulfur natural gas pipeline leakage incidents, the primary factors influencing the diffusion of high-sulfur natural gas leaks were identified. Schlieren apparatus experiments on leakage jets demonstrated that the leakage gas is influenced by flow velocity, exhibiting typical vortex phenomena. As the kinetic energy of the gas jet decreases during the leakage process, gravity and the gas's own composition become the main factors influencing the movement of the leaking gas, leading to a transition energy balance and plume diffusion phenomena. The distance of the leakage gas jet correlates positively with hydrogen sulfide concentration and flow velocity, while it correlates negatively with the leakage aperture. Thermal imaging and mid-infrared laser experiments indicate that the leaking gas shows a phenomenon of unchanged concentration ratio yet gradually decreasing overall concentration during diffusion. The relationship among hydrogen sulfide content, environmental wind speed, and leakage gas intercept is linear, while fluctuations are observed with respect to the leakage aperture and flow rate, revealing the diffusion behavior of high-sulfur natural gas leakage.

(3) Identification of the leakage diffusion mechanism through molecular simulation and large-scale FLACS simulations for high-sulfur natural gas leaks. Molecular simulations of hydrogen sulfide and methane indicate that the mixed gas exhibits a faster diffusion rate compared to individual gases. An RDF characteristic peak exists at a molecular distance of 4 Å due to the influence of van der Waals forces acting on CH₄ and H₂S. The diffusion coefficient of the mixed gas shows a positive correlation with temperature and a negative correlation with pressure, while the relationship with hydrogen sulfide concentration exhibits fluctuations that correspond to two dynamic equilibrium points of partial pressure and van der Waals forces. Large-scale simulations of high-sulfur natural gas leakage show that the concentration of hydrogen sulfide negatively correlates with the influence range in the vertical direction of the leakage jet, while exhibiting fluctuation patterns similar to those in molecular simulations in the lateral intercept. Environmental wind speed negatively affects the influence ranges in the vertical and lateral directions, but positively correlates with the jet direction. Additionally, the leakage aperture and internal pressure present a fluctuating increase in influence range; environmental temperature positively correlates with the leakage diffusion range, effectively unveiling the mechanisms underlying high-sulfur natural gas leakage and diffusion.

(4) Research on dynamic warning methods for hazardous leakage zones in high-sulphur natural gas gathering and transmission pipelines. Based on national industry standards and hydrogen sulphide warning concentrations in high-sulphur natural gas, the leakage gas range is categorised into four levels, establishing a safety evaluation system for leakage in high-sulphur natural gas pipelines. To alleviate the problem of limited leakage data, an improved GAN network structure was proposed for data augmentation, resulting in the creation of a leakage data set. A GWO two-layer GRNN-ANN network structure was developed to establish a non-linear mapping relationship between the hydrogen sulphide warning concentration and the maximum leak dispersion distance of high sulphur natural gas. The Gaussian dispersion model was then optimised using the maximum distance values from the coupling model under key hydrogen sulphide concentrations at different leakage times, resulting in a dynamic 3D early warning model for hazardous leakage zones of high-sulphur natural gas pipelines. Finally, a hypothetical leakage scenario from a natural gas field in southwest China was used to visualise the safety warning range and system operation results of the dynamic early warning model.

The research outcomes resulted in a mid-infrared remote sensing laser device designed for large-scale mixed gas monitoring, clarified the leakage jet-diffusion behavior of high-sulfur natural gas, revealed the leakage mechanisms of high-sulfur natural gas pipelines, and proposed a dynamic three-dimensional warning model for hazardous leakage zones, which has excellent visualization capabilities for monitoring and early warning. This holds significant importance and utility for enhancing the efficiency of dynamic monitoring and early warning of high-sulfur natural gas pipeline leaks.

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